Femtosecond Laser

Micromachining of glass integrated

devices for XUV filtering in High-
order Harmonic Generation
MASTER OF SCIENCE IN ENGINEERING PHYSICS - NANOOPTICS AND
PHOTONICS

Author: Alessandro Paletti

Student ID: 944263

Advisor: Prof. Roberto Osellame
Co-advisor: Dr. Rebeca Martínez Vázquez
Academic Year: 2020-2021
Il lavoro di tesi

Il lavoro di tesi porta in copertina il nome di chi l’ha scritta, del relato e del
correlatore, ma dovrebbero esserci molte più scritte. Certo il contributo di quei nomi
è essenziale e il loro contributo è più tangibile, però attorno e spesso dentro altri
hanno “scritto”. Il primo ringraziamento, quindi, va al Prof. Osellame che ha reso
possibile questo lavoro e che riesce a coordinare un fantastico. Il gruppo si, in ogni
suo componete: chi ti ha soltanto salutato o chi ti ha consigliato. Alcuni mi hanno
dato un grandissimo aiuto nell’ambito sperimentale, altri dal punto di vista
relazionare e altri ancora in entrambi gli ambiti. Spesso mi hanno tirato su o
scherzato e spesso salvato, visto tutti i “danni” combinati!!!!
Proprio di questi disastri voglio scusarmi con la persona più importante per la
realizzazione di questa tesi: Rebeca. Grazie per tutti gli insegnamenti, i consigli e le
sgridate, ne meritavo anche di più. Ha saputo indirizzarmi senza costringermi e
consigliarmi senza influenzarmi. Poche persone mi hanno insegnato qualcosa
veramente, perché l’insegnamento non è cosa da tutti, Lei è tra queste: sia dal punto
professionale che umano. Avrà sempre la mia stima e riconoscenza!!!

Volevo poi ringraziare il reparto tecnico e il gruppo UDYNI per aver anch’essi
contribuito.

Ci sono, ovviamente, persone al di fuori del Dipartiremo.

Primi tra tutti i “profeti di sciagura”, quelli che sono sempre lì a svilirti o a
demoralizzarti. Non c’è né bisogno, ci penso io da solo…
Un grazie ancora più sentito va ai falsi “amici”, quelli che non ti tarpano le ali, ma
anzi te le spiegano. Non sperano, in realtà, che tu cada per deriderti, ma per poter
illuderti di sacrificarsi porgendoti una mano per rialzarti: falsi, ipocriti e moralisti.
Mutano i loro bisogni in attenzioni e distorcono la realtà per alienarti: hanno sempre
maschere affascinati. Arrivano, però, i giorni delle prove di sforzo e lì si sbriciolano,
come zolle dopo mesi di siccità. Urlate quanto volete, io non mi sposto.

Per fortuna ci sono persone sincere, non le cito perché il mio grazie lo custodisco in
me e ho la presunzione di trasformarlo in atti e parole che lo dimostrino. Tutto va
dimostrato, costruito e applicato, altrimenti svanisce e nulla muove.

i
Abstract
This thesis work is focused on the fabrication of fused silica chips used as integrated
filters for High-order Harmonic Generation (HHG): a highly non-linear effect that
generates coherent radiation in the form of high-order harmonics of the driving laser
frequency. In particular, pulse trains in the attosecond time scale of extreme
ultraviolet radiation (EUV) and soft X-rays (SXR) are generated.

The generation chips, on which the filters will be integrated, exploit the interaction of
some noble gases with IR radiation (800 nm) to generate XUV radiation, but the
process is highly inefficient and the radiation at the output of the HHG stage has a
residual component of the driving field that co-propagates with that generated. The
various applications that use high-order harmonics require pure XUV radiation
beams, so filters are used to remove the IR radiation.
The purpose of the devices manufactured is to replace traditional (mainly metallic)
filters with the same performance, but reducing the operating space and replacement
time, increasing the filtered bandwidth and storing the IR radiation for re-use. To do
so we will exploit the hollow waveguide principle, to modify the IR driving field
beam a spatially separate it from the generated XUV.
The filters are manufactured using the FLICE technique (Femtosecond Laser
Irradiation followed by Chemical Etching) which, by combining irradiation with
femtosecond pulses and acid etching of the glass sample, makes it possible to
construct very complex hollow micrometric architectures. The generation chips also
use the same technique. Our chip will consist of two hollow channels, one to guide
IR radiation and the other to allow the transmission of XUV radiation.
During this thesis project we studied this specific design by varying the size of
the UV channels in order to experimentally find the best configuration. The filters
were then optically characterized in order to assess their guideing characteristics, and
therefore their ability of filtering, the IR radiation.

These chips are presented as one of the first examples of integrable glass filters,
whose operating principle, architecture and manufacturing method will pave the
way for a future XUV spectroscopy lab on a chip.

Keywords: FLM, HHG, filter, FLICE, XUV, IR, fused silica, hollow wave guide

iii
Abstract in lingua italiana
Questo lavoro di tesi si è focalizzato sulla fabbricazione di chip in silice fusa utilizzati
come filtri integrati per la generazione armonica di alto ordine (HHG): un effetto
altamente non lineare che genera radiazione coerente sotto forma di armoniche di
alto ordine della frequenza del laser di guida. In particolare, vengono generati treni
di impulsi nella scala temporale degli attosecondi della radiazione ultravioletta
estrema (EUV) e dei raggi X morbidi (SXR).

I chip di generazione, su cui verranno integrati i filtri, sfruttano l'interazione di alcuni

gas nobili con la radiazione IR (800 nm) per generare radiazione XUV, ma il processo
è altamente inefficiente e la radiazione all'uscita dello stadio HHG ha una
componente residua del campo guida che co-propaga con quella generata. Le varie
applicazioni che utilizzano armoniche di alto ordine richiedono fasci di radiazioni
XUV pure, di conseguenza vengono utilizzati filtri per rimuovere la radiazione IR.
Lo scopo dei dispositivi realizzati è quello di sostituire i filtri tradizionali
(principalmente metallici) con le stesse prestazioni, ma riducendo lo spazio operativo
e il tempo di sostituzione, aumentando la larghezza di banda filtrata e conservando
la radiazione IR per riutilizzarla. Per fare questo sfrutteremo il principio della guida
d'onda cava, per modificare il fascio di campo guida IR e separarlo spazialmente dal
XUV generato.
I filtri sono realizzati con la tecnica FLICE (Femtosecond Laser Irradiation followed
by Chemical Etching) che, combinando l'irradiazione con impulsi a femtosecondi e
l'incisione con acido del campione di vetro, permette di costruire architetture
micrometriche cave molto complesse. Anche i chip di generazione utilizzano la stessa
tecnica. Il nostro chip sarà composto da due canali cavi, uno per guidare la
radiazione IR e l'altro per permettere la trasmissione della radiazione XUV.
Durante questo progetto di tesi abbiamo studiato questo specifico design variando la
dimensione dei canali UV al fine di trovare sperimentalmente la migliore
configurazione. I filtri sono stati poi caratterizzati otticamente per valutare le loro
caratteristiche di guida, e quindi la loro capacità di filtrare, la radiazione IR.

Questi chip sono presentati come uno dei primi esempi di filtri di vetro integrabili, il
cui principio di funzionamento, l'architettura e il metodo di fabbricazione apriranno
la strada per un futuro laboratorio di spettroscopia XUV su un chip.

Parole chiave: FLM, HHG, filtri, FLICE, XUV, IR, silice fusa, guide d’onda cave

iv
Introduction
The development of technologies based on integrated optics is one of the active and
studied fields of photonics. Its wide ranging applications in various research and
industrial sectors make it one of the most innovative technologies of recent years.
The devices designed aim to reduce the size of existing technologies and increase
their performance, but also to discover and manipulate new physical phenomena
and their applications.

The devices we have fabricated are designed to be used as integrated filters on chips
designed for high-order harmonic generation. The HHG enables the generation of
radiation in the extreme ultraviolet (EUV) and soft X-rays (SXR) and such pulses
make it possible to explore ultrafast phenomena occurring in matter whose dynamics
could be captured in their fundamental time scales (∼ fs) and lengths (∼ nm) by
attosecond pulses, if they are actually generated by chips.

The generation of this radiation is based of bulky instrumentation and occupy very
large spaces, moreover this phenomena have very low efficiencies; as a consequence
a lor of effort is dedicated on overcoming these limitations. The integrated filters here
presented are thought to be a key element in reducing the operating space of
traditionally used filters and in the filtering efficiency.
The operating principle of the generation chips is based on highly non-linear optical
phenomena triggered in the hollow structures between certain noble gases and IR
radiation, the result of which is the production of XUV radiation. The intensity of the
generated radiation is ∼ 10-4 - 10-5 the intensity of the driving field, so after the HHG
phenomena it is necessary to remove the more intense part of the radiation (residual
driving field). Filters are placed after the generation source in order to filter
out this residual radiation from the driving field, which is essential to use the XUV
component.
The first part of the thesis is focused on the manufacture of the integrated filters
using the FLICE technique. This technique is based on the combination of
Femtosecond Laser Micromachining (FLM) followed by chemical etching, which
allows the creation of hollow structures with very complex geometries and small
dimensions inside glass substrates. The design is based on the profile of the co-
propagating radiation after the source, so it was essential to fabricate several samples
to optimize the geometry of the filter and obtain different sizes of hollow channels.
The second part of the thesis is focused on the analysis of the geometrical aspects and
the preliminary optical characterization of the filters. The impact of the geometry on
the IR radiation losses was evaluated in order to find the parameters that allow a
better efficiency.
Measurements were planned with the filter integrated in the generation chip to
collect XUV spectra and quantify the attenuation of IR radiation under real working
v
conditions, but due to unexpected experimental problems in the HHG laboratory,
only one measurement could be made on an initial prototype.
In this thesis, the theoretical and practical aspects of understanding the phenomena
studied and the work carried out are explained.
The thesis is organized as follows:
• in Chapter 1 we will introduce the Femtosecond Laser Micromachining
technique (FLM), describing the physical phenomena involved in this process
and the working parameters for obtaining different geometries and
dimensions. The analysis will focus on the fabrication of microchannels with
the FLICE technique (Femtosecond Laser Irradiation followed by Chemical
Etching), in fused silica.
• In Chapter 2, the physical basis for High-order Harmonic Generation (HHG)
will be introduced with the semi-classical three-phase model and a quantum
interpretation. The theory for radiation guiding in hollow waveguides will be
presented along with the conditions necessary to optimize the process. The
generation of HHG in gas-filled hollow waveguides will be explained, in
particular illustrating quasi-phase-matching (QPM) techniques. The operating
principles and performance of conventional filters are then illustrated.
• In Chapter 3 we introduce the experimental apparatus used for the
microfabrication of the device, the characterization of the filter and the
generation set-up.
• In Chapter 4 a generation chip based on gas-filled hollow waveguides is
illustrated with results. We will explain the working principle of the filter. We
will show the step-by-step microfabrication process and the characteristics of
the microchip, with particular attention to the parameters for optimizing the
geometry. We will illustrate a possible development of the filter design with
the fabrication of a prototype.
• In Chapter 5, we will present the results obtained from the characterization
and illustrate the parameters involving the IR radiation guiding efficiency. We
will then present the only measurement made of the filter integrated in the
chip, with its setup improvements.

vi
Contents
Sommario

Il lavoro di tesi............................................................................................................................................ i
Abstract...................................................................................................................................................... iii
Abstract in lingua italiana ........................................................................................................................ iv
Introduction................................................................................................................................................ v
List of Figures ............................................................................................................................................. x
List of Tables ........................................................................................................................................... xiii
Chapter one ............................................................................................................................................... 1
Femtosecond laser micromachining and FLICE..................................................................................... 1
1.1 Introduction ............................................................................................................................... 1
1.2 Radiation-matter interaction..................................................................................................... 2
1.3 Exposure parameters ................................................................................................................. 5
1.4 Femtosecond Laser micromachining followed by chemical etching (FLICE)....................... 9
1.4.1 Irradiation- physical phenomena (nanogratings) ...........................................................10
Chapter two..............................................................................................................................................16
High-order Harmonic Generation ..........................................................................................................16
2.1 Introduction ..............................................................................................................................16
2.2 Physical interpretation: semiclassical model ..........................................................................16
2.2.1 Ionization ...........................................................................................................................18
2.2.2 Motion in the Electric Field ..............................................................................................19
2.2.3 Recombination ..................................................................................................................21
2.3 HHG in hollow waveguide......................................................................................................22
2.4 HHG in gases media.................................................................................................................24
2.4.1 Phase matching in hollow waveguides ...........................................................................26
2.4.2 Quasi-Phase matching in hollow waveguides................................................................30
2.4.3 Quasi-Phase matching in modulated gas density ..........................................................32
2.4.4 Advantages of HHG in hollow waveguides ...................................................................35
2.5 Filtering in HHG experiments .................................................................................................35
Chapter three............................................................................................................................................39
Experimental Apparatus .........................................................................................................................39
3.1 Fabrication set-up .....................................................................................................................39
3.1.1 Laser source .............................................................................................................................40
vii
 3.1.2 Beam steering ...........................................................................................................................40
3.1.3 Translational stage...................................................................................................................41
3.1.4 Wet chemical etching ..............................................................................................................41
3.2 Hollow Waveguide characterization set-up ...........................................................................42
3.3 High order harmonic generation.............................................................................................43
3.3.1 Laser source .............................................................................................................................44
3.3.2 Vacuum chamber .....................................................................................................................44
Chapter four .............................................................................................................................................47
Lab on a chip for HHG ............................................................................................................................47
4.1 Introduction ..............................................................................................................................47
4.2 HHG in glass chip ....................................................................................................................47
4.3 Integrated X-UV filter idea ......................................................................................................51
4.4 Filtering chip fabrication ..........................................................................................................54
4.4.1 IR waveguide parameters ................................................................................................55
4.4.2 UV channel optimization of radius and profile ..............................................................58
4.4.3 IR filtering optimization: double IR waveguide. ............................................................63
Chapter five ..............................................................................................................................................66
Towards lab on a chip for HHG and XUV filtering ..............................................................................66
5.1 Introduction ....................................................................................................................................66
5.2 Optical characterization of the integrated filters .........................................................................66
5.3 Experimental apparatus for HHG and XUV filtering in chip .....................................................71
5.4 Preliminary results of XUV filtering .............................................................................................72
Conclusions ..............................................................................................................................................75
Bibliography .............................................................................................................................................77

viii
List of Figures
1.1 FLM writing principle schematic representation of the focus point moving in the
material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Schematic representation of non-linear absorption in a bulky material . . . . . . . . . 3
1.3 Timescale of the physical phenomena associated with the interaction of a
femtosecond laser pulse with transparent materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.4 Schematic representation of the two translating configurations. . . . . . . . . . . . . . . . 8
1.5 Illustration of the FLM main steps. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
1.6 Different morphological modifications induced in fused silica by FLM. . . . . . . . . 9
1.7 Schematic representation of Transient Nanoplasmonic Model . . . . . . . . . . . . . . . 11
1.8 Scanning electron images of nanogratings formed with writing direction. . . . . . 12
1.9 Schematic representation of the FLICE technique. . . . . . . . . . . . . . . . . . . . . . . . . . . 12
1.10 Conical etching. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
1.11 Schematic representation of a conical spiral and schematic representation of an
uncompensated microchannel. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
1.12 Optical images of inner surfaces before and after thermal annealing. . . . . . . . . . 14

2.1 Schematic representation of three-steps model for High-order Harmonic

Generation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.2 Schematic representation of a HHG spectrum. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.3 Atomic Coulomb potential when distorted by an intense laser field, in the
tunneling regime . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
2.4 Trajectories of the free electron as a function of laser phase, for different values of
the ionization time. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
2.5 Dependance of cut-off energy for several gases. . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
2.6 Transmission of the EH1m modes for a 70 m capillary radius as a function of fiber
length . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . 24
2.7 Representation of an extreme nonlinear upconversion of a femtosecond laser. . 25
2.8 Harmonic intensity as a function of propagation distance for phase matching. . 26
2.9 Harmonic intensity as a function of the phase mismatch . . . . . . . . . . . . . . . . . . . . 27
2.10 On axis photon flux as a function of the medium length. . . . . . . . . . . . . . . . . . . . 28
2.11 Measured and calculated pressure dependence of the harmonic yield for several
gases. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
2.12 Dependance of energy cut-off as function of driving wavelength in Xe gas . . . 29
2.13 Differences in harmonic emission in a gas-filled straight and modulated hollow
waveguide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31

x
2.14 Dependence of harmonic emission in a gas-filled modulated and straight
waveguide, as a function of propagation distance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
2.15 Differences in harmonic emission in a He gas-filled modulated fiber, at different
modulation periods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
2.16 Harmonic spectra obtained with the use of multiple gas jets technique at
different distances . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33
2.17 Schematic of the experimental setup that use multiple and successive gas jets for
HHG. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
2.18 Enhancement factors of HHG. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
2.19 Schematic representation of HHG with gas cell. . . . . . . . . . . . . . . . . . . . . . . . . . . . 35
2.20 Measured spectra of the generated XUV light. . . . . . . . . . . . . . . . . . . . . . . . . . . . . .36
2.21 Harmonic spectra recorded by FFS after spectral selection by metallic foils. . . . 36
2.22 Setup with a mirror pair as filter. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .37

3.1 Schematic experimental apparatus for femtosecond laser writing. . . . . . . . . . . . . .39

3.2 Schematic experimental apparatus for hollow waveguide characterization. . . . . 42
3.3 Drawing and photo of the filter holder used in the characterization. . . . . . . . . . . .43
3.4 High-order harmonic generation and acquisition schematic setup . . . . . . . . . . . . 43

4.1 Design of the micro-chip. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .48

4.2 Numerical simulation of helium-gas fluidics inside the micromachined device. .49
4. 3 HHG spectra generated by 500 µJ in helium at different backing pressures. . . . .50
4.4 Log-scale HHG spectra (not normalized) at the cutoff plotted to the photon
energy. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
4.5 Design of the filter. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .52
4.6 Path of the copropagating beams in the integrated filter with generation chip. . .53
4.7 Filtering idea. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
4.8 XUV radiation intensity profile simulation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
4.9 Attenuation as a function of radius of curvature. . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
4.10 Dimensions of device. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .55
4.11 Steps for radiating the cylindrical surface. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56
4.12 IR channel subdivision. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57
4.13 Distance between the channels and their size . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .57
4.14 Irradiated glass with 5 parallel lines with a gap of 3 µm. . . . . . . . . . . . . . . . . . . . .58
4.15 Filter after process of irradiation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 59
4.16 Sample of reference. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 60
4.17 Sample’s edge of reference. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .60
4.18 XUV channels for different filters. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
4.19 Filter with the reference channels. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 63
4.20 'Bifurcated' filter. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .64

xi
5.1 Mode profiles 𝐸𝐻11 , 𝑇𝑀01 𝑎𝑛𝑑 𝑇𝐸01 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .67
5.2 Mode profile for IR channels with different angles of bending. . . . . . . . . . . . . . . . 68
5.3 Mode profiles for filters A, B and C.. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 70
5.4 Mode profiles for filters D and E. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 70
5.5 Mode profiles for filter “Bifurcated”. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
5.6 Filter on the holder integrated with the generation chip in the vacuum chamber. .
. . . .72
5.7 Filter used for preliminary measurement. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .72
5.8 Spectra of generated radiation collected with and without filter installation. . . . 73

xii
List of Tables
2.1 Summarizes the various IR radiation filtering techniques. . . . . . . . . . . . . . . . . . . . 35

4.1 Summarizes the data obtained from a sample to assess the relationship between
powers, number of lines and dimensions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .59
4.2 Shows the measurements of filters with different diameters of the XUV channel. .
. . . 61

5.1 Show results of samples without the channel XUV. . . . . . . . . . . . . . . . . . . . . . . . . . 68

5.2 Show results of filter con different radios of guide IR and the channel XUV. . . . .69

xiii
xiv
Chapter one
Femtosecond laser micromachining and
FLICE

1.1 Introduction

In 1996, K. M. Davis et al introduced a new technique to induce permanent changes

in glass by focusing a femtosecond laser beam: Femtosecond Laser Micromachining
(FLM) [1]. They suggested that the interaction of the laser with the glass gives rise to
an increase in the refractive index, so it is possible to inscribe waveguides or excavate
channels for different applications, all in a small portion of volume with control over
spatial parameters on the order of micrometers (Fig 1.1).

Fig. 1.1: FLM writing principle schematic representation of the focus

point moving in the material.

In a paper of 2001 by Marcinkevicious et al. [2] is demonstrated that a 5% of aqueous

solution of HF acid was able to etch a 3D pattern written by a focused femtosecond
laser, this permits the fabrication of micrometric hollow channels with a circular
cross section inside a fused silica substrate. From this, Optofluidics exploits the
possibility of manufacturing complex devices that allow the integration of fluidics
and optics [3, 4]. These devices make Optofluidics applicable in many fields of
research and industry.
FLM is 3D technique that allow the fabrication of complex structures that would be
otherwise impossible to obtain with techniques previously known such as silica-on-
1
silicon, ion exchange or lithographic methods: to possible obtain only, in general,
planar structures [5].
Ultrashort laser pulses with durations in the femtosecond range allow the structuring
of all materials, such as crystals [6], glasses [2, 7] or polymers [6], with high precision
and minimal thermal and mechanical influence.
FLM consists in irradiating a transparent material with focused femtosecond laser
pulses, the non-linear absorption by the sample, due to the high peak intensities,
causing localized material modification in a confined volume, determined by the
focused spot, even at moderate pulse energies [4]. The desired geometry of the
structure is obtained through the relative motion between the sample and the laser
focus.
FLM typically operates with the range of frequencies from UV to IR that correspond
the transparency window of fused silica [8, 9]. Furthermore being a widely used
optical material with a well-known structure (excellent chemical and mechanical
stability) and high commercial availability, studies have focused on this material.

1.2 Radiation-matter interaction

The interaction between a focused femtosecond laser pulse with a high peak intensity
(of the order of 1013 Wcm−2 [10]) induces a material modification in the focus region.
Indeed near-IR photons (𝜆 = 800-1000 nm) are non-linearly absorbed by the glass, as
the photon energy is lower than the bandgap energy between valence band and
conduction band in the electronic structure of the glass hence not take a place
phenome to excite electronic transition (the relation 𝐸𝑔 > ℎ𝜈 always holds in FLM).
The focal volume of the laser beam is the only finite region of space where changes
are induced. In this area, in fact, the peak of the pulses can have an intensity such as
to reach the non-linear absorption threshold of the material: around TW/cm2. The
consequence is the excitation of electrons from the valence to conduction band, the
following formation of an electron plasma which will transfer its energy to the
surrounding material [11].
Plasma generation is triggered by two possible physical mechanisms: multiphoton
ionization and tunnel ionization. Multiphoton ionization is the main phenomenon and
causes the direct ionization of matter by incoming radiation. This mechanism is
possible even if the energy of a photon, at the considered frequencies, is not sufficient
to excite a electron in the conduction band, but if possible that m multiple photons
have energy to be absorbed by a valence band electron and to be promoted in
conduction band (𝑚ℎ𝜈 > 𝐸𝑔 ).

2
Tunnelling ionization is a further mechanism that is included in higher laser
intensities. This phenomenon take place because the strong time-varying
electromagnetic field distort the band structure with consequence reduction of band
gap, hence band-to-band electron transitions can be accomplished by quantum
tunnelling. These processes are schematic in Fig 1.2:

Fig. 1.2: Schematic representation of the phenomena occurring in a bulky material by

femtosecond laser micromachining: (a) multiphoton ionization, (b) tunnel ionization, (c)
avalanche ionization [13].

Keldysh demonstrated that the frequency and the intensity of laser are two variables
that permit to understand what of two physical mechanism is dominant [12]. hence
to introduce the Keldysh parameter:

𝜔 𝑚𝑒 𝑐𝑛𝜀0 𝐸𝑔
𝛾= √ (1.1)
𝑒 𝐼

being 𝜔 the laser frequency, 𝐼 the laser intensity at the focus, 𝑚𝑒 the effective electron
mass, 𝑒 the electron charge, 𝑐 the speed of light, 𝑛 the linear refractive index and 𝜀0
the permittivity of the free space.
This parameter allows to discriminate three qualitatively different cases:
3
 ▪ If 𝛾 » 1: low laser intensities and high hence frequencies multiphoton
ionization dominates (but still below that needed for linear photon
absorption).
▪ If 𝛾 « 1: high laser intensities and low frequencies hence tunnel ionization
dominates
▪ If 𝛾 ≈ 1, nonlinear photoionization can be understood as a combination of the
two.

The last mechanism that can take a place is avalanche photoionization. This is a main
phenomenon for the creation of plasma but start only after the precedent process. In
fact, is necessary that multiple free electrons are excited at the bottom of the
conduction band (so-called hot electrons [10]), they can linearly absorb photons,
increasing their kinetic energy until 𝐸𝑘 > 𝐸𝑔 , such that a further valence electrons
excitation is possible by impact ionization with conduction electrons. The “hot
electrons” and the electrons generated for ionization can in turn acquire energy from
the laser pulse, become “hot” and excite other electrons, hence, to generate avalanche
effect, with duration as long as the laser fields interacts with the material, and a
consequent exponentially increase of free carriers density in the focal region [13].
Until the density of plasma is minor of value of density so-called critical (≈ 1021 cm−3),
the laser pulse cannot propagate through it, being partially reflected and partially
absorbed at the surface. When this densities they are equal, the plasma frequency
equals the laser frequency and most of the energy is transferred to the electronic
plasma due to resonant effect: the resulting plasma relaxation returns energy to the
lattice, causing the material modification [14] in timescales (≈ 10 ps) longer than
femtosecond pulse duration [15]. It is usually assumed that when the carrier reaches
this critical value the optical breakdown occurs. In glass, the corresponding laser
intensity is of the order of 1013 W cm−2.
Depending on the pulse duration we can distinguish two situations:
1) In the regime of ”longer” laser pulses (pico-nanosecond regime), avalanche
ionization depends only on the seed electrons of the process provided by
thermal excitation of defect states or of impurities [10]. The number of
impurities and dislocation within the focal volume is subject to large
fluctuation, so the process of free carrier formation would be stochastic,
hence caused in a less uniform machining.
2) In the regime of ”shorter” laser pulses (sub-picosecond regime), the
ionization processes contribute to the promotion of electrons to the
conduction band in the focal region. The plasma relaxation takes place in a
shorter timescale than energy transfer time to the lattice and so minimizing
heat diffusion coming out from the focal volume [14]. This leading to a
confined material modification, even smaller than the focal volume due to
nonlinear phenomena, with consequence that the electron plasma is
4
 generated in a deterministic and uniform energy absorption. The result is
that in this regime the micromachining technique is more sensitive and
precise than in the longer pulse regime (Fig 1.3).
To ionized matter is typically associated a characteristic frequency, called plasma
frequency [15]:
4𝜋𝑒 2 𝑛𝑒
𝜔𝑝 2 = (1.2)
𝑚𝑒∗
where 𝑚𝑒∗ is the effective mass of the electron.

Fig. 1.3: Timescale of the most important phenomena occurring in the interaction of a femtosecond laser with a
transparent material. Thermal and structural events take place long after carrier excitation [11].

1.3 Exposure parameters

Fused silica was used in the manufacture of our devices, due to the advantages
described in the previous section. We will focus on the parameters that determine the
FLM results, which are: the focusing conditions, the laser source parameters, the
writing configuration and the intensity regime.

• Laser source parameters

In FLM, to avoid linear absorption processes it is necessary that the wavelength of

the femtosecond laser belongs to the transparency window of the material.
Initially it was used a 𝜆 = 800 nm, but Shah et al. [16] demonstrated that an
5
enhancement of the writing quality is obtained if at high repetition rate a doubled
frequency laser beam is used. Hence using a 1045 nm fundamental frequency and
doubling with a second harmonic generation stage using a BBO crystal (a writing
laser wavelength of 522 nm in the green), it was possible to obtain an increased
efficiency of ionization process.
It is necessary to introduce a new parameter: the repetition rate frep; its importance
will be clear when we explain the formation of nanogratings (section 1.3.1).
Defining the characteristic thermal diffusion time tth (typical value of 1/tth in fused
silica is around 1 MHz), is possible to discriminate three different f rep regimes:
1) Low repetition rate regime: frep (1 − 200 kHz) >> 1/tth. The interval between the
pulses is such as to allow thermic relaxation (cooling), that is the return to the
initial temperature: consequently, the changes to the material are caused by
the contribution of a single pulse. In this situation, the energy pulse is big
enough to allow a weaker focus, but a lower translational speed is required (≈
10 µs) for a sufficient energy transfer to the sample [8].
2) High repetition rate regime: frep (4 − 25 MHz) << 1/tth. The thermal energy does
not have sufficient time to be dissipated, so there is an increase in temperature
with consequent melting of the material beyond the focused zone [14, 17]. The
changes in the regions are therefore not directly related to the laser source and
the setup, but to the isotropic diffusion of heat. An advantage of this mode is
the possibility of low peak intensities (high intensities require high NA and
therefore less flexibility) and faster writing.
3) Intermediate repetition rate: frep (200 − 4 MHz) ≈ 1/tth. In this regime, we have
discrete translation speed and a mild focus, obtaining the characteristics of the
high repetition rate regime [18].

The polarization will be further discussed in Section 1.3, as it is tied up the

orientation of the nanogratings formation.

• Focusing conditions

The focusing of the laser pulse, through an optical system, to form a micrometric
focal spot on the material is essential to allow the threshold intensity necessary to
activate non-linear absorption processes to be exceeded. In the description we
will neglect the spherical and chromatic aberrations that the optical system
introduces and model the generated optical intensity profile as a linear Gaussian
beam. We thus introduce the well-known equations that define the beamwaist 𝜔0
and the Rayleigh range 𝑧0 (propagating along z axis):
𝜆𝑀2
𝜔0 = (1.3)
𝑁𝐴𝜋

6
 𝑛𝜆𝑀2
𝑍0 = (1.4)
𝑁𝐴2 𝜋

with 𝑛 is the refractive index of the material, 𝑀2 is the beam propagation factor,
𝑁𝐴 is the numerical aperture of the focusing objective and 𝜆 is the free space
wavelength. We thus determine the focal volume and note that this volume will
be circular in the x-y plane and elongated along z. The high optical aperture of the
lens allows for better precision, which is especially important for very deep
structures. Defining a specific NA for a specific depth is essential to take
advantage of specific optics and compensation techniques [19]. These must be
used to avoid further spherical aberration introduced by the refractive index
variation caused by the air-glass interface, which causes relative beam distortion.
A possible solution is the use of oil immersion lenses, which however limit the
depth of writing.

• Writing configuration

The relative motion and velocity between the sample and the beam determines
the energy deposited on the material; these direct and indirect factors are what
then determine the final structure of the chip. The relative motion can be parallel
or perpendicular.
▪ Transverse writing (Fig 1.4a): the sample is translated orthogonally to the laser
beam, so the length is not limited by the working distance and this allows
writing to depths of even millimeters, which is essential for creating 3D
optical circuits. The enormous disadvantage of this writing mode is the
formation of channels with high cross-sectional asymmetry, which is caused
by the relationship between depth of focus and spot size. This asymmetry has
an impact on the number and properties of modes supported by straight
waveguides. To overcome this problem, we find several possible solutions in
the literature: beam shaping techniques (use of a cylindrical telescope or
multiscan writing techniques [20, 21, 22]), use of a slit before the focusing lens
[23], stacking several laser zones side by side [24], shaping of the focal volume
by means of an appropriate focusing geometry [25] use of a deformable mirror
[26].
▪ Longitudinal writing (Fig 1.4b): the sample is moved parallel to the laser beam
forming a cylindrical symmetry to the modified volume. The main
disadvantages are the working distance of the lens and the obligatory bottom-
up writing to avoid volumes already modified in the path of the laser: in
general, it is always important to avoid overwriting.
The translation speed must be such that enough energy is deposited to reach
the necessary threshold for the FLM process.
7
 Let us consider 𝑣 the relative velocity, 𝐹 the fluence impacting the material
and the effective number of pulses in the reflector, the net fluence is:
2𝜔0 𝑓𝑟𝑒𝑝
𝑁𝐹 = 𝐹 (1.5)
𝑣

Fig. 1.4: Schematic representation of the two translating configurations: (a) transverse writing
and (b) longitudinal writing. Arrow represents the translation direction of the sample.

• Intensity regimes

The intensity of the pulse is the main parameter that discriminates the
morphological evolution of the irradiated material after the physical phenomena
described in the previous paragraphs have been triggered. The result of the
fabrication, hence the permanent changes, has been shown to be of three types
(Fig 1.5):

Fig. 1.5: Illustration of the FLM main steps: (a) the laser is focused insight the
material, (b) energy is absorbed via a nonlinear mechanism, (c) laser transfers its
energy to the surrounding material resulting in a permanent modification (d) [11].

8
 1. For peak intensities of about 1011 W/cm2 ("low") one is above the threshold of
the non-linear absorption. The result is the homogeneous variation of the
refractive index in the focal volume: this allows the fabrication of optical
waveguides [27, 28, 29] (Fig 1.6 a);
2. For peak intensities around 1012 W/cm2 ("intermediate") there is the formation
of nanogratings at lower wavelengths, resulting in a change in the birefringent
refractive index. This regime, together with an acid solution, is exploited for
the fabrication of hollow channels: the FLICE technique [30, 31, 32] (Fig 1.6 b);
3. For peak intensities above 1014 W/cm2 ("high") in the focal volume, pressures
above Young's modulus are generated, causing micro-explosions and shock
waves. These phenomena lead to the formation of a less dense or hollow
("empty") core surrounded by a region with a higher refractive index [33]. This
regime is not exploitable for micromaching techniques, but for other
applications [34, 35] (Fig 1.6 c).

Fig. 1.6: Different morphological modifications induced in fused silica by FLM: a) smooth modification regime [29], b)
sub-wavelength nano-gratings regime and c) disruptive modification regime [33].

1.4 Femtosecond Laser micromachining followed by

chemical etching (FLICE)

To fabricate hollow structures in fused silica, advantage is taken of the faster etching
of acid solutions into the fused silica for irradiated areas compared to unmodified
areas. The first step is to irradiate specific areas of the sample to create a specific 3D
structure with permanent modifications. The second step is immersion in an acid
solution that will selectively etch this structure by emptying it [36].

9
1.4.1 Irradiation- physical phenomena (nanogratings)

From the above introduction, it is clear that for the manufacture of micro-channels it
is necessary to apply an intensity regime that increases the selectivity of the etching
rate. From section 1.2 it is understood that the "intermediate" regime with the
formation of nanogratis is the one to be achieved. To explain the results generated,
we introduce the Transient nanoplasmonic model, proposed by Hnatovsky et al. [37, 38]
(Fig 1.7). These structures have a periodicity dependent on the laser wavelength and
polarization, the physical mechanism of which can be broken down into several
steps:

1. the presence of defects and colour centres in the material and non-linear
absorption lead to the formation of hot-spots in the focal volume.
2. the first ionization causes a reduction in the energy bandgap, thus increasing the
probability of absorption in these areas: memory effect [39]. The consequence of
this effect is the evolution of the hot-spots into spherical nanoplasms with the
arrival of the pulse train at the same spot. It is evident that this process depends
on the intensity and speed of translation, but also on the density of the plasma
generated in the dielectric.
3. The electric field affecting the nanoplasms preferably increases in the direction
perpendicular to the laser polarization. The deformation of nanoplasms into
nanoellipsoids is directly proportional to the attainment of the plasma frequency
[40]. Near this frequency, the elongation is so extreme that the nanoellipsoids
mutate into nanoplanes.
4. During the evolutionary process, the nanoplasms are arranged stochastically, but
when the critical density is exceeded they become metallic and affect the
propagation of light in such a way that they are arranged in parallel nanoplanes
spaced 𝜆/2𝑛, where 𝜆 is the wavelength of the laser and n is the refractive index
of the fused silica [40, 41] (Fig 1.7 e).

10
 Fig. 1.7: Schematic representation of Transient Nanoplasmonic Model [37]: a) local, ionized hot-spots
generation, b) nanoplasmas formation, c) nanoplanes formation and d) parallel self-alignment of
nanoplanes e) Different results when varying the laser wavelength in fused silica [40, 41].

1.4.2 Chemical etching

The traditionally used acid is HF, which partially dissolves in water and releases F-
and H+. The fluorine ion reacts with the silicon atoms, whereas the hydrogen ion
(proton) reacts with the oxygen atoms [42]. This reaction is summarized below [43]:

SiO2 + 4HF → SiF4 + 2H2O (1.6)

It is important to note that although fused silica is an amorphous material, a basic

structure of Si - O - Si covalent bonds can be identified. This reaction takes place both
on irradiated material, at "low" and "intermediate" pulse intensity, and on intact
material: what varies is the time at which the reaction takes place. The different
reaction speeds are probably due firstly to the phenomenon of ionization, which
modifies the bond with the silicon by making the oxygen atom more exposed,
making it more prone to protonation [42]. The second reason is the presence of the
nanogratings, which increase the fluidity of the acid in the channels, which explains
the greater efficiency of the "intermediate" regime compared with the "low" regime
where they are not formed. A possible proof of this thesis is to be found in the
different reaction if one varies the polarization of the laser and therefore the
arrangement of the nanogratings, in fact defining ⃗⃗⃗ 𝐸 the field polarization and ⃗⃗⃗𝑆 the
direction of translation:

• 𝐸 ǁ ⃗⃗⃗⃗𝑆 , the nanocracks are perpendicular to the writing axis: the diffusion of the
⃗⃗⃗
acid is limited by the aligned nanocracks and drastically reduced (Fig 1.8 a);
• ⃗⃗ , the nanoplanes are parallel to the writing axis and elongated: the etching
⃗⃗⃗ ⊥ 𝑆
𝐸
rate of the solution is increased the etching rate of the solution (Fig 1.8 b);
• ⃗⃗⃗ ʘ 𝑆
𝐸 ⃗⃗⃗ (circular polarization), no preferred direction for the nanoplanes: an
intermediate situation between the previous conditions, which can be used for the
fabrication of structures with no preferred direction.
11
 Figure 1.8: Scanning electron images of nanogratings formed with writing direction (a)
parallel and (b) perpendicular to the electromagnetic field [13].

From reaction (1.6) it can be seen that fresh acid solutions must be used to remove
the accumulation of the product in the channels as there is a rapid saturation of the
HF solutions, this requirement presents a difficulty for the renewal of the solution in
the deep microchannels. To facilitate this renewal and increase the homogeneity of
the result, the incision process is usually carried out in an ultrasound bath. The
concentration of the solution is chosen according to the desired characteristics (length
and shape) of the micro-channels, and the temperature of the solution can be
optimized to accelerate the speed of chemical etching (Fig. 1.9). Increasing the
selectivity of chemical etching would allow the fabrication of micro-channels buried
in fused silica. A possible change in the HF chemical etching process could be KOH,
which provides constant high e selectivity, followed by a reduced etch rate, allowing
the fabrication of structures with a higher aspect ratio [44]. The use of KOH is limited
by its very low action on unaltered SiO2, which makes it very slow to start etching.

Fig. 1.9: Schematic representation of the FLICE technique.

12
1.4.3 Channels properties

One of the difficulties in manufacturing is obtaining symmetrical and homogeneous

channels: the continuous flow of solution causes greater etching of the inlet areas,
resulting in the formation of a conical structure with an aspect ratio (length-to-
diameter ratio) that depends on the etching rate of the HF solutions. Which depends
on the incision rate of the nanocracks and non-irradiated regions (Fig. 1.10).

Fig. 1.10: Conical etching, microchannel geometry before (top)

and after (bottom) etching.

To solve the first problem, the concentration of the solution can be varied: at low HF
concentrations there is a decrease in the etching rate leading to a high aspect ratio,
but also to shorter microchannel lengths [38]; at high HF concentrations there is a
decrease in the aspect ratio due to the high chemical etching rate, but the self-
cessation of the process is delayed and longer channels can be obtained [45]. The
concentration of HF also changes the time required to complete the entire structure.
At low concentrations (∼ 2.5-5%), an etching rate of around 50 - 120 µm/h is
measured; values around 400 - 500 µm/h are found for higher concentrations (∼ 20 -
30%). However, a limit of 2 mm remains for any concentration. A second precaution
is the introduction of additional HF inlets (etching channels) at other points in the
waveguide. It is also possible to radiate the volume to be extracted with a line in the
axis of the cylinder or even to create plane cuts whose purpose is to split the glass
and thus facilitate its removal from the channel. For the second problem, a possible
method for compensating conical shapes is to radiate an inverted cone with respect
to the one obtained after etching without compensation. The geometry of the cone
will depend on the size of the desired guides and the HF concentrations used. From
Fig. 1.11, consider 𝛬 as the pitch of two consecutive helices and its value determines
the etching rate: if too large, the acid may slow down due to the non-irradiated
regions; if too small, it is irrelevant. As for roughness (Fig 1.12), usually of the order
of a hundred nanometres, it can be detrimental in most optical applications [46], such
as light scattering, total internal reflection or light confinement [47]. It depends on the
etching conditions [48] and can be decreased by optimizing: pulse energy, electric
13
field polarization, focal point shape or scanning parameters and increasing the
etching time, but there is no dependence on HF concentration [49]. Subsequent heat
treatments can reduce smoothness even by a factor greater than ten [50].

Fig. 1.11: a) Schematic representation of a conical spiral; b) Schematic representation of an

uncompensated microchannel(blue), of the compensating cone (red) and of the final expected
cylindrical microchannel (grey).

Fig. 1.12: Optical images of inner surfaces (a) before and (b) after thermal annealing. Scanning-probe
microscope images of a 10 × 10 µm2 (c) before and (d) after the annealing; (e) and (f) represent the
same surface on a larger area of 50 × 50 µm2 . Here, rugosity was reduced from some hundreds of nm to
few nm [50].

14
15
Chapter two
High-order Harmonic Generation

2.1 Introduction

In this chapter, the HHG will be described in order to understand in detail the
necessity of installing filters in generation setups. We will then focus on the
generation of high-order harmonics in gas-filled hollow waveguides as the filter
fabricated in this thesis will be integrated on a generation chip using technology.

High-order Harmonic Generation is a non-linear optical process that occurs due to

iteration between a sample (gas, plasma or solid) and an intense laser pulse. This
phenomenon generates coherent high-order harmonics of the driving laser frequency
with a time scale duration of attoseconds (10-18 s), then generates XUV (particularly
extreme ultraviolet (EUV) and soft X-rays (SXR)). This radiation, in the form of a
train of pulses, can be used as a probe to study a range of phenomena in atomic,
molecular and solid-state physics, particularly in a recent field of physics: attosecond
science [51, 52].
To understand all the mechanisms that describe the process of generation, it is
necessary to introduce a model based on strong field quantum electrodynamics
(SFQED)[53]. A semi-quantum approach, which does not quantize electromagnetic
fields, has been proposed by Lewenstein [54]. Another semi-classical model is the
one developed by Kulander et al. [55] and Corkum et al. [56]; due to its simplicity
and the completeness of the results obtained it will be the theory we will use and will
be described in the next section. A perturbative approach is not possible since the
electric field of the pulse is comparable to that of an electron in an atom: the electric
field of the laser propagating in the medium bends the potential barrier that binds
the electrons to the atom, so it cannot be considered as a perturbation.

2.2 Physical interpretation: semiclassical model

The semi-classical model of Kulander et al. [55] and Corkum et al. [56] describes the
main physical processes involved in high-order harmonic generation, which are
described in three steps (Fig. 2.1):

1. Tunnel ionization of an atom interacting with a strong electric field.

16
2. Interaction of the free electron with the driving field.
3. Recombination of the electron with the ion: generation of the XUV photon.

Fig. 2.1: Schematic representation of three-steps model for High-order Harmonic Generation: the potential barrier
of the atom is bent by an intense electric field, allowing the electron to tunnel out in the energy continuum. Then,
the electron interacts with the driving laser and recollides with its parent ion, generating XUV burst.

It is a cyclic process: the sum of the optical cycles of the pulse generates an
attosecond stream of XUV radiation. The high-order harmonic spectrum (Fig. 2.2) is
characterized by three regions: initially a drop of two to three orders of magnitude
that continues for a few harmonics; this is followed by a plateau in which the
intensity remains almost constant, extending over hundreds or even thousands of
harmonic orders; this intermediate region is interrupted by a rapid decrease in the
energy of the cutoff photon [57, 58]. One observes the presence of only odd
harmonics of the fundamental frequency.

Fig. 2.2: Schematic representation of a HHG spectrum. Each bar represent one harmonic.
Characteristic plateau and cut off region are highlighted.

17
2.2.1 Ionization

As mentioned above, a perturbative approach is not possible: the electric field of the
guiding laser is comparable to the Columbian field generated in the atom (∼ 1011
V/m). Furthermore, it is assumed that the harmonics are generated by a single atom,
which is a strong simplification as the HHG is the response to laser stimulation of the
medium as a whole, but microscopically it is significant to focus on the response of
the single atom [59]. By means of the Keldysh parameter, it is possible to break down
three photoionization models:

𝐼𝑃
𝛾=√ (2.1)
2𝑈𝑃

where𝐼𝑝 is the ionization potential and 𝑈𝑝 is the ponderomotive energy, defined as:

𝑒 2 𝐸02
𝑈𝑃 = (2.2)
4𝑚𝜔2

which is the mean kinetic energy acquired by an electron oscillating in the laser field.
Where 𝑒 and 𝑚 are the charge and the mass of the electron whereas 𝐸0 e 𝜔0 are the
energy and the frequency of the driver.

1) If 𝛾 >> 1, multiphoton ionization (MPI) occurs: the atom must absorb many photons
to promote electrons to energy levels above the ionization potential.
2) If 𝛾 << 1, we have tunnel ionization (TI): the Coulomb potential is strongly
distorted by the electric field of the laser, allowing the transition of the electron
wave function into the continuum. (Fig. 2.3)

Fig. 2.3: Atomic Coulomb potential when distorted by an intense

laser field in the tunneling regime.

18
If the electrons absorb more photons than are needed to cross the threshold, the
excess energy is converted into the kinetic energy of the photoelectron: the electron
escapes from the atom and becomes an unbound ion and this phenomenon is called
above-threshold ionization (ATI). The transition from one regime to the other is possible
by changing the intensity of the laser pulse, at the same frequency, as equations (2.1)
and (2.2) show. Tunnel ionization is the regime that causes high-order harmonic
generation: this process occurs at low frequencies and high field strengths.
To calculate the ionization rates, hence the ionization probability, we introduce the
theory of Ammosov, Delone and Krainov [60, 61]. This model is only applicable for
noble gas (which are usually employed to generate highorder harmonics), tunnel
ionization and linearly polarized fields [62]:
∗
2 4𝜔𝑝 2𝑛 −1 4𝜔𝑝
𝜔(𝑡) = 𝜔𝑝 |𝐶𝑛∗ | ( ) 𝑒𝑥𝑝 (− ) (2.3)
𝜔𝑡 3𝜔𝑡

where
𝐼𝑃 (𝑒𝐸(𝑡))
𝜔𝑝 = , 𝜔𝑡 = (2.4)
ħ √2𝑚𝐼𝑃

𝐼 ∗
𝑛∗ = 𝑍√ 𝐻 , |𝐶𝑛∗ |2 = 22𝑛 [𝑛∗𝛤(𝑛∗ − 1)𝛤(𝑛∗ )]−1 (2.5)
𝐼𝑃

In the equations (2.3) the quantities already previously defined are used and the
following are defined: the charge after ionization 𝑍, the ionization potential of the
atomic hydrogen 𝐼𝐻 , the Gamma function 𝛤(∙) and the effective principal and orbital
quantum numbers 𝑛∗ . By developing these equations, we obtain the fraction of
ionized atoms, or free electron density:
𝑡
𝜂(𝑡) = 𝑒𝑥𝑝 [− ∫𝑙−∞ 𝜔 (𝑡 ′ )𝑑𝑡 ′ ] (2.6)

The obtained value of this equation is crucial for the generation of attosecond pulses:
the relative proportions of neutral atoms and free electrons determine the phase
mismatch, as will be explained later.

2.2.2 Motion in the Electric Field

After ionization we have free electrons, assumed to be point particles, set in motion
only by the interaction with the oscillating and polarized electric field 𝑬(𝒕) =
𝐸0 𝑐𝑜𝑠(𝜔0 𝑡)𝒖𝒙 . In a semi-classical model, it is possible to evaluate the kinematics of
charged particles by applying Newton's Second Law:
𝑑2 𝑥 𝑒𝐸0
= cos(𝜔0 𝑡) (2.7)
𝑑𝑡 2 𝑛

19
We impose as boundary conditions that 𝑥(𝑡0 )=0 and 𝑣(𝑡0 )=0, i.e. electron initially
stationary and inside the atom, and that the motion is along x, integrating the
previous equation:
𝑒𝐸0
𝑣(𝑡) = cos(𝜔0 𝑡) sin(𝜔0 𝑡) (2.8)
𝑚𝜔0
𝑒𝐸0 𝑒𝐸0
𝑥(𝑡) = − 2
[cos(𝜔0 𝑡) −cos(𝜔0 𝑡0 )] + sin(𝜔0 𝑡0 )(𝑡 − 𝑡0 ) (2.9)
𝑚𝜔0 𝑚𝜔0

The last equation shows an oscillatory pattern of electron motion: varying the initial
phase Φ0 = 𝜔0 𝑡0 results in different trajectories and consequent phenomena. (Fig
2.4). Some trajectories allow the recombination of the electron with the parent ion,
while others cause the final escape from the atom. The figures show that if the
electron emission occurs exactly at the peak of the electric field, the recombination
velocity will be zero (blue trajectory in Fig. 2.4 a, trajectory d in Fig. 2.4 b. It can be
shown that recombination occurs for 0° < Φ0 < 80° and 180° < Φ0 < 260°: a pulse is
generated every optical half-cycle, i.e. between the positive and negative peaks of the
electric field. This is the theoretical demonstration of the presence of only odd
harmonics in the HHG spectrum. In order to classically calculate the amount of
kinetic energy of the electron at the impact, it is necessary to find the return time of
the electron by imposing 𝑥(𝑡) = 0:
𝜋 𝜋
𝜔0𝑡 = − arcsin ( 𝜔0 𝑡 − 1) (2.10)
2 2
1
𝐸𝑘 = 𝑚𝑣 2(𝑡) = 2𝑈𝑝 [sin(𝜔0 𝑡) − sin(𝜔0 𝑡0 )] (2.11)
2

Fig. 2.4: Trajectories for different initial phases, as a function of time (on the left) [58] and in the state space (on the
right) [59].

20
2.2.3 Recombination

In the recombination of the electron with its parent ion, there is the emission by the
atom of a photon whose energy is the sum of the ionization potential 𝐼𝑝 and the
kinetic energy of the incoming electron of the incoming electron:

ℏ𝜔 = 𝐼𝑝 + 𝐸𝑘 (2.12)

From eq. (2.11) it can be calculated that the maximum kinetic energy is equal to
3.17𝑈𝑝 which is equivalent to Φ =17. Knowing therefore the maximum kinetic energy
and the ionization potential, we can derive the shear energy [63]:

𝐸𝑐𝑢𝑡 = 𝐼𝑝 + 3.17𝑈𝑝 (2.13)

Knowing that 𝑈𝑝 ∝ 𝐼𝜆2 , it is possible to increase the cutting energy by increasing the
intensity of the guiding laser or its wavelength. This increase causes a reduction in
the harmonic brightness due to dephasing of the coherent process of the harmonic
field and scattering of the electron wave packet, respectively, resulting in a reduction
in the recombination probability. In addition, there is a saturation level for the
photon energy; this value is reached when the fundamental state population is
completely depleted and must remain in the atom to interact with the returning
electron. If the field is elliptically polarized, the electron does not recombine with its
parent ion and the HHG efficiency decreases. From Eq. (2.11) we obtain two possible
values for 𝑡 − 𝑡0 that result in the same kinetic energy. Thus we have two trajectories,
called "short" and "long" resulting in degeneration for maximum energy and lasting
at most 3/4 of the E cycle. This phenomenon causes a flow of XUV in a time less than
the period of the driving field, thus having a duration of the order of a hundred
attoseconds. Another unfortunate effect is the presence of harmonic frequency
variations (frequency chirps): positive and negative for long and short trajectories
respectively. Such temporal distortions should be compensated in order to obtain a
cleaner final pulse, but no technique is feasible since positive and negative chirp are
present [58]; moreover, these also cause chromatic aberrations [64]. In 1994
Lewenstein et al. [54] proposed an analytical and quantum model for HHG that
describes the atom-electric field interaction using the time-dependent Schroedinger
equation (TDSE). We will not go into the details of this model, which in turn requires
other approximations for analytical analysis, but merely show the final conclusions
as an addition to the three-step model. The most important result is the
interpretation of the generation of attoseconds, i.e. a macroscopic effect due to the
electric field-medium interaction, expressed as polarization:

𝑃⃗(𝑡) = 𝑁⟨𝑒𝑟⟩ (2.14)

21
with N the number of dipoles per unit volume and 𝑟 the position vector, referring to
the moment of the dipole:

⟨𝑟⟩ = ⟨𝜳(𝑟, 𝑡)|𝑟|𝜳(𝑟, 𝑡)⟩ (2.15)

The dipole-electric field interaction provides a new phase term to Eq. (2.11), which
results in the extension of the maximum harmonic obtainable after the cut-off as a
function on driving field intensity:
𝐼𝑝
𝐸𝑐𝑢𝑡 = 𝐼𝑝 𝐹 ( ) + 3.17𝑈𝑝 (2.16)
𝑈𝑝

with 𝐹 = 1.36 for 𝐼𝑝 << 𝑈𝑝 , decreasing down to 1 for increasing 𝐼𝑝 , converging to semi-
classical expression. The results of Eq. (2.16) are shown graphically in Fig 2.5, which
relates the cutoff energy with the driving wavelength for some noble gases. With
short pulses there is a very high intensity with possible saturation before the end of
the pulse [65]. The saturation intensity depends on 𝐼𝑝 so each material shows its own
behavior.

Fig. 2.5: Cut-off energy scaling versus wavelengths for the most common gases used for
an HHG experiment [65].

2.3 HHG in hollow waveguide

In this section we introduce the theory of hollow waveguides, which will be used to
understand the operation and characteristics of filters and describe the advantages of
HHG in these gas-filled waveguides over other techniques.

22
The propagation of the wave along a hollow guide can be modelled as a reflection
series with the inner walls having a grazing incidence. To describe the field
configurations and propagation constants of the normal modes in a circular hollow
waveguide, we start by analyzing a dielectric waveguide described by the
fundamental work of Marcatili et al. [66].
We assume:
- consider cylindrical channels with an internal radius a larger than the wavelength 𝜆
of the free space:
𝑘𝑎 = 2𝜋𝑎 𝜆 >> |𝜈|𝑢𝑛𝑚 (2.17)
- Infinite wall thickness.
- Magnetic permeability equal to that of free space µ0 .
- Only low-loss modes are considered, which are those whose propagation constant 𝛾
are almost equal to that of free space:
𝛾
| − 1 | << 1 (2.18)
𝑘

with, 𝑘 being the propagation constant in free space, 𝑢𝑛𝑚 is the 𝑚𝑡ℎ root of the
equation 𝐽𝑛−1 (𝑢𝑛𝑚 ) = 0 for the Bessel function of order 𝑛 − 1 and 𝜈 = √𝜀⁄𝜀0 is the

complex of the external medium.

There are three types of modes supported by the hollow waveguide:

▪ Transverse circular electric modes 𝑇𝐸0𝑚 : the field lines are concentric circles in the
cross section centred on the axis of the guide.
▪ Transverse circular magnetic modes 𝑇𝑀0𝑚 : the field lines are radially directed.
▪ Hybrid mode 𝐸𝐻 𝑛𝑚 (|𝑛| ≥ 1): both components are present.
All field components are present, but the axial ones are relatively small and are
usually neglected. In particular, when a linearly polarized Gaussian beam 𝑇𝐸𝑀00 is
coupled into a hollow waveguide, the hybrid modes are preferentially excited. As
linear polarization is maintained for 𝑛 = 1, the 𝐸𝐻1𝑚 modes are the most relevant.
The field amplitude in the hollow waveguide varies radially as a function of 𝑟:

𝑟
𝐸1𝑚 = 𝐽0 (𝑢1𝑚 ) (2.19)
𝑎

Considering 𝜆 << 𝑎, the propagation constant can be written as:

𝛾1𝑚 = 𝛽1𝑚 + 𝑖𝛼1𝑚 (2.20)

where

2𝜋 1 𝑢𝑖𝑚 𝜆 2
𝛽𝑖𝑚 = [1 − ( ) ] (2.21)
𝜆 2 2𝜋𝑎

23
e phase constant, that determines guiding effect dispersion for phase matching
conditions, and
𝑢𝑖𝑚 𝜆 2 𝜆2 𝜈2 +1
α=( ) (2.21)
2𝜋 2𝑎3 √𝜈2 −1

is the attenuation constant, where 𝜈 is the ratio between the refractive indices of the
external fused silica and the air. Since 𝑢𝑖𝑚 increases with 𝑚, the mode with the lowest
𝐸𝐻 11 : losses mainly affect higher-order modes and therefore only the fundamental
propagates properly through the guide (Fig.2.6). This, moreover, supports the low-
loss assumption developed in the model just described [66].

Fig. 2.6: Transmission of the EH11 mode and next high-order mode EH12 at 780
nm for a 70 m capillary radius as a function of fiber length [82].

2.4 HHG in gases media

Noble gases, such as helium, argon or neon, are usually used to generate higher
order harmonics, having an ionization potential (between 10 and 25 eV) much higher
than the energy of the driving laser (usually less than 2 eV). The interaction can take
place in different devices, for example, there are many studies for the generation of
high-order harmonics using the interaction of a pump beam focused on a gas ejected
from a nozzle inside a vacuum chamber. Since HHG is a very low-efficiency process,
studies focus on obtaining techniques and devices to increase the conversion
efficiency and brightness of high-order harmonic generation. From a macroscopic
point of view, several factors come into play, such as: gas pressure, beam focusing
angle, beam intensity and non-linear effects. The main problem is phase matching:
the generated wave should maintain a fixed phase relation with respect to the non-

24
linear polarization in order to extract energy in the most efficient way from the
incident wave, i.e., the dispersion curve of the phase velocities between the
fundamental and harmonic frequencies through the non-linear medium must be
evaluated. One could think that since every atom emits harmonics over a broad
range of energies (up to keV) then also the HHG spectrum should show high energy
photons. This is not automatically true, because it is needed that the photon
generated by many atoms coherently add to provide the output beam, as shown in
(Fig. 2.7). This is a well-known issue in nonlinear optics that is usually overcome by
equalizing the phase velocity of the pump light with the generate beams by using
birefringence [67], satisfying the so-called phase-matching condition which is
commonly exploited in frequency conversion experiments.

Fig. 2.7: Representation of an extreme nonlinear up-conversion of a femtosecond

laser in a gas-filled hollow channel. To be successful, phase matched addition of
harmonic produced by each single atom is required.

Unfortunately, in HHG several macroscopic many mechanisms limit the theoretical

achievability such as: phase matching effects or propagation length (Fig. 2.8). Studies,
therefore, show different solutions and limitations, for example: in standard gas-jet
generation, destructive harmonic yield interference occurs and phase matching is
strongly limited by beam divergence [68]. Another relevant problem is the
experimental apparatus used for generation and in particular the solutions to confine
the gas. The system of hollow waveguides allows a valid solution to both the above-
mentioned problems, as we will illustrate in the next paragraphs.

25
 Fig. 2.8: Harmonic intensity as a function of propagation distance for phase
matching (blue line) and no phase matching (red line) conditions, where
𝐿𝑐 = 𝜋/∆𝑘 is the coherence length.

2.4.1 Phase matching in hollow waveguides

For photon energies of the guiding laser below about 130 eV and for a suitable beam
pressure and length: HHG can be easily phase-coupled on the centimeter scale by
balancing the neutral atom scattering with the free electron plasma scattering [69, 70].
In contrast, for higher peak intensities, strong ionization and increased dispersity
(which depends on the gas species and laser wavelength [71]) occurs, inducing a
relative phase shift between the laser and the harmonic field. We define the
absorption length and the coherence length (length over which the harmonic field
constructively accumulates):
1
𝐿𝑎𝑏𝑠 = (2.22)
𝜌𝜎
𝜋
𝐿𝑐𝑜ℎ = (2.23)
𝛥𝑘

where 𝜎 is the ionisation cross section and 𝜌 the atomic density. We then define the
phase mismatch which is expressed as the difference between the propagation
vectors of the fundamental, 𝑘0 , and 𝑞 𝑡ℎ harmonic, 𝑘𝑞 :

𝛥𝑘 = 𝑞𝑘0 − 𝑘𝑞 (2.24)

26
In a model for phase adaptation in a gas-filled hollow waveguide, ∆k is evaluated by
the contributions of the scattering introduced by the waveguide effect, the scattering
due to the neutral gas and the phase velocity change introduced by the plasma
ionization [72]. In Fig.2.9, the decrease in harmonic intensity is shown as the phase
mismatch increases.

Fig. 2.9: Harmonic intensity as a function of the phase mismatch.

The evolution of the number of photons emitted on axis per unit of time and of aria
and for the 𝑞 𝑡ℎ harmonic as a function of the length of the medium is plotted in Fig.
2.10 for different coherence lengths. The conditions for phase matching and optimal
conversion efficiency in a uniform long medium are: 𝐿𝑐𝑜ℎ > 𝐿𝑎𝑏𝑠 and 𝐿𝑐𝑜ℎ > 5𝐿𝑎𝑏𝑠
respectively [70]; this condition is general, not just for gas-filled hollow waveguides.
At high intensities the second condition can only be achieved transiently. Even when
the coherence length is infinite, HHG emissions saturate as soon as the length of the
medium is longer than a few 𝐿𝑎𝑏𝑠 , since harmonics emitted beyond this length are
absorbed as depicted in Fig. 2.10. In general, as 𝐿𝑐𝑜ℎ decreases, the efficiency
saturates at smaller and smaller values. The conditions need the wavefront of the
laser field to vary slowly in order to be fulfilled, as is the case in a hollow waveguide.
It is found that the asymptotic value is independent of the density. As mentioned
before, the phase mismatch will have to be balanced with the different dispersion
terms to obtain a zero phase match for HHG:

∆𝑘 = ∆𝑘𝑁 + ∆𝑘𝑃 + ∆𝑘𝐺 (2.25)

Without going into the details of a specific analysis for each individual contribution,
it is found that: the phase terms of the waveguide (∆𝑘𝑃 ) and plasma ionization (∆𝑘𝐺 )

27
are concordant, while the dispersion term of the neutral gas (∆𝑘𝑁 ) is discordant with
them. The concordant terms therefore cause the phase velocity of the guiding laser to
increase relative to that of the harmonic signal. In order to obtain a tunable phase
match, it is possible to vary some parameters for which the dispersion terms are a
function, such as: the species and pressure of the gas (Fig.2.11), the waveguide size,
the guide wavelength 𝜆0 and the ionization fraction as a function of laser intensity
𝜂 = 𝜂(𝐼). Pressure variation is a widespread technique [72].

Fig. 2.10: On axis photon flux as a function of the medium length [70].

Fig. 2.11: measured (a) and calculated (b) pressure dependence of the harmonic yield
for several gases. In order of increasing optimum pressure, the curves correspond to
xenon, krypton, argon, and hydrogen [79].

28
It is important to note that for low intensities, the plasma dispersion can be neglected
and phase matching can be achieved with a suitable compensation of the waveguide
and the neutral dispersion atoms by tuning the pressure or the cross section of the
waveguide. Furthermore, since a lower gas density is required to compensate for the
waveguide and neutral scattering atom, the optimum pressure required for phase
matching in this regime is lower. For higher intensities, the rapid increase of ∆𝑘 has
to be considered: in fact, after a critical ionization 𝜂𝑐𝑟𝑖𝑡 does not depend on the case
pressure and consequently the balancing of free electron scattering by an optimal
pressure value is not possible. The consequence is that the phase matching conditions
impose a new cut-off energy 𝐸𝑐𝑢𝑡 of the harmonics. Knowing that 𝐸𝑐𝑢𝑡 ∝ 𝐼𝑝𝑒𝑎𝑘 𝜆20 ,
using a longer wavelength 𝜆0 it is possible to overcome this limit, since the intensity
of the guiding laser can be decreased, leading to a reduction of the free electron
density (Fig.2.12). Another possible solution to overcome the cut-off energy is the use
of materials whose atoms have a higher ionization potential, which results in a
reduction of the plasma density (see Fig.2.5). The maximum harmonic energy of 1.6
keV, achieved with the phase matching technique, was achieved in He with a 3.9 µm
driver laser [72], with other techniques it is possible to increase the maximum
harmonic energy [73].

Fig. 2.12: HHG by 50 µJ, 25fs laser pulses of different wavelengths in xenon gas. Focal point size 20µm
FWHM. Laser intensity ∼ 2·1014 W/cm2 . a)0.8 µm, cutoff at 42 eV (27th harmonic); b)1.51 µm from
OPA, cutoff at ∼ 75 eV (91st harmonic); c)1.37 µm from OPA cutoff at ∼ 69 eV (77th harmonic);
d)1.22 µm from OPA, cutoff at ∼ 58 eV (49th harmonic). The HHG wavelength is also tuned by the
driving wavelength from OPA [65].

29
2.4.2 Quasi-Phase matching in hollow waveguides

The previous section highlights a critical problem with non-linear optics: a small
phase change can cause large, unwanted changes in the output. One possible
solution is quasi-phase matching (QPM), a technique that avoids the phase mismatch
that occurs after every length of coherence 𝐿𝑐𝑜ℎ propagation through a periodic
correction, leading to coherent generation of the travelling signal. This technique is
essential for generating high harmonics at the ionization level, which cannot be
produced by phase matching. Only gaseous media are considered as dense media
cause strong absorption at high harmonic frequencies. Several QPM techniques exist,
such as the use of counter-propagating pulses [74, 75], but in this section we will only
analyse devices that use gas-filled hollow waveguides. The reasons for this choice are
clear from the fact that this work wants to show the hollow waveguide fabrication
technique and its potential, and why the XUV-generating chips used with the filters
we fabricate have this technology as a possible development. The QPM technique is
inapplicable for photon energies and ionization levels: the plasma scattering becomes
much larger than the contribution of the neutral gas, and after a coherence length the
generated signal interferes with the out-of-phase radiation formed later in the gas.
Some solutions have been proposed, such as that of Gibson et al. [76]: use of a
modulated hollow waveguide (obtained by glass-blowing techniques) of 150 µm
diameter filled with gas to obtain a variation of the guiding laser. Phase-matching
can be achieved if the pressure and intensity of the laser are tuned. We define 𝐿 as
the propagation distance in a non-linear medium for a harmonic 𝑞 𝑡ℎ :
𝐿
𝐸𝑞 ≈ ∫0 𝐸0𝑛 (𝑧)𝑑(𝑧)𝑒 −𝑖𝛥𝑘𝑧 𝑑𝑧 (2.26)

where n is the order of the nonlinear process, 𝑑(𝑧) is the nonlinear process, defined
as follows:
+∞
𝑑(𝑧) = ∑ 𝐷𝑚 𝑒𝑖𝑘𝑚𝑧 (2.27)
𝑚=−∞

and defining
2𝜋𝑚
𝐾𝑚 = ≈ ∆𝑘 (2.28)
𝛬
where 𝛬 is the periodicity of the waveguide modulation and 𝑚 the order of the QPM
process, it is understood that the improvement of the harmonic signal is possible
with an increase of 𝐾𝑚 . The enhancement of a modulated hollow waveguide over a
straight one is ∼2 magnitudes (Fig.2.13) and by increasing the length of the
modulated waveguide, and by increasing the modulated waveguide length, very
high levels of compensable ionization are achieved (Fig.2.14).

30
Fig. 2.13: Figure 2.10: Harmonic emission from a straight (black) and 0.25-
mm-period modulated (red) 150 µm diameter waveguide filled with low-
pressure Ar (7 torr), at a peak laser intensity of 9·1014 W/cm2. The
emission extends from harmonic order 89 (80 eV) to 115 (180 eV) [76].

Fig. 2.14: Energy of the 95th harmonic order for a large phase
mismatch in the case of a) a straight, unmodified waveguide, and b) a
modulated waveguide [77].

31
For longer coherence lengths it is possible to decrease the modulation period, in fact
the amount of ionization that can be compensated for increases and this also allows
higher order harmonics to be in phase [77] (Fig.2.15). These techniques bring a real
improvement, although they do not completely eliminate the dispersion as the
propagation distance varies.

Fig. 2.15: Differences in harmonic emission in a He gas-filled modulated

fiber, each 2.5 cm in length, at different modulation periods: 1 mm
periodicity (blue line), 0.75 mm periodicity (red line) and 0.5 mm
periodicity (green line) [77].

2.4.3 Quasi-Phase matching in modulated gas density

Other solutions use modulation of gas density to compensate for phase mismatch.
These techniques use multiple and successive gas jets [78]: the plasma generation
leads to a negative dispersion and consequent reduction of the coherence length 𝐿𝑐𝑜ℎ .
A first approach is to vary the distance between the different nozzles injecting gas
into the hollow waveguide; we evaluate the intensity evolution in a gas-filled hollow
waveguide after propagation distance 𝐿 [79]:

𝜋𝑁
𝐼𝑞 ≈ 𝑠𝑖𝑛2 ( ) (2.29)
2𝑁𝑞

with 𝑁𝑞 the maximum density to phase match 𝑞 𝑡ℎ harmonic over 𝐿 and to not cause
destructive interference. By dividing the interaction region into 𝑀 intervals, suitably
separated so that diffraction-induced changes in the phase of the laser and amplitude
between two adjacent sections can shift the phase of the dipole oscillations by 𝜋, we
have that the intensity increases with a factor 𝑀2 and the density by a factor 𝑀 [80]:

32
 𝜋𝑁
1 − (−1)𝑀 𝑐𝑜𝑠( 𝑁 )
𝑞 𝜋𝑁
𝐼𝑞 ∝ 𝜋𝑁 𝑠𝑖𝑛2 ( ) (2.30)
1 + 𝑐𝑜𝑠( ) 2𝑀𝑁𝑞
𝑀𝑁𝑞

The optimization of the division of the interaction length into 𝑀 intervals and the
distance between adjacent regions at high gas densities allows to increase density up
to 𝑀𝑁𝑞 , obtaining the generation of higher harmonics. Fig.2.16 shows the results of
this technique at different source distances. If the distance between the sources is
optimized (d), the harmonic signal strength increases and the energy cut-off shifts
from higher energies.

Fig. 2.16: Harmonic spectra obtained with the use of multiple gas jets at
different distances [80].

In addition to the spacing between the various nozzles, the number of gas sources,
for particular ranges and harmonic orders, also leads to a clear improvement of the
yield, which can be attributed to a partial QPM effect [78]. Fig. 2.17 shows a
schematic of the experimental setup. Comparing the results with a single-slit source,
with and without dispersion effects. In general, an improvement of a factor related to
the number of sources is observed for the first harmonics. As described in Fig. 2.18, at
higher order harmonics (even beyond the 17th), setups experience very high
enhancement factors.
Another approach for generating high harmonics is in the composition of the gas
used: using, for example [81], a composite consisting of ellipsoidal silver
nanoparticles in argon. A periodic modulation of the nanoparticle concentration
provides quasi-phase adaptation, which mitigates the negative effect of significant
phase mismatch.

33
 Fig. 2.17: Schematic of the experimental setup that use multiple and
successive gas jets for HHG [78].

Fig. 2.18: Harmonic yield enhancement factors for different gas-jet source
arrays normalized to the single source configuration. Solid curves:
experimental data; dotted curves: calculated data for a single slit source of
equivalent length in the case of perfect phase matching; dashed curves:
calculated data for a single slit source including phase mismatch effects [78].

34
2.4.4 Advantages of HHG in hollow waveguides

The paper by M. Nisoli et al [82] shows that the use of gas-filled hollow waveguides
leads to harmonic generation efficiencies of the order of 10 -4. Previous work [83, 84]
had shown much lower efficiencies as they had opted for generation by gas in free
space. The advantages of gas confinement in hollow waveguides stem from its
bringing several advantages over free focusing through a gas jet or cell. The hollow
waveguide mechanism, despite relative losses compared to other types of
waveguides, maintains high laser intensity over a long propagation distance, and
this configuration counteracts intensity reduction due to ionization-induced
defocusing and maximizes the region of interaction between the laser field and the
non-linear medium.

2.5 Filtering in HHG experiments

After generation, the collected radiation will consist of UV radiation and the residual
IR radiation, which was used to generate the higher order harmonics Fig 2.19. For a
complete analysis of the HHG technique, it is essential to clean the beam from the
residual IR guide beam.

Fig. 2.19: Schematic representation of HHG with gas cell [89].

Different filtering techniques are available to obtain a UV only radiation, or at least

with a predominance of only this emission (see Table 2.1).
Method IR attenuated XUV preserved References
Al filter 95% 50%-60% [85][87]
Al filter with thinner oxide layers 100% 75% [86]
A pair of Brewster reflections with silicon mirrors 96% - [88]
Three dichroic wedge separators (LAYERTEC GmbH) 85% 85% [89]
Disc fordivergence of the different components - - [90][91]

Tab. 2.1: The table summarizes the various IR radiation filtering techniques, indicating the percentage of IR radiation
removed and the percentage of XUV radiation retained.

35
The most common technique is to use metallic filters, whose potential is shown in
Fig. 2.20.

Fig. 2.20: Measured spectra of the generated XUV light. The full spectrum is plotted in black, while the spectrum filtered
by a 0.2 μm thick aluminum foil is plotted in red. The theoretical transmission of the aluminum filter is shown for
reference and plotted as a gray dashed line [85].

As a general rule, the filter must be able to absorb IR wavelengths (around 780 nm)
and transmit XUV wavelengths (from 2 nm to 30 nm). Some experiments report the
use of a series of filters of different materials as in the work of I. Makos et al [85], thus
achieving complete removal of the IR component (see Fig. 2.21). In addition to the
absorption of the guide radiation, it is also essential to always have an excellent
transmission efficiency for XUV, which is possible by replacing an Al filter with a
thickness of 100 nm with a filter also in Al but with thinner oxide layers, obtaining a
transmission increase of over 40% [86].

Fig. 2.21: Harmonic spectra recorded by FFS after spectral selection by metallic foils. The generation medium was
(a) Xe and (b) Ar gas. In both panels, the blue and red peaks correspond to harmonics after transmission through
150 nm thick Al and Sn respectively, while the red dash-dotted (Al) and black dashed (Sn) are transmission curves
for 150 nm thickness [85].

36
A "pre-filtering" is often performed, as in the work of Makos et al [85] or P Billaud
[87], by incidenting the generated XUV co-propagating with the IR towards a silicon
(Si) plate placed at the specific Brewster angle. This plate significantly attenuates the
IR and usually reflects about 50-60% of the XUV radiation by deflecting the XUV
beam towards the chosen filter. Other works use only reflection as a filtering system:
they use a series of mirrors to transmit most of the NIR radiation, but in some cases
also attenuate and transmit the UV: it is therefore possible to see its working
principle as the inverse of that of a metallic filter. This approach is for example used
by F.Reiter et al [88] who use a pair of Brewster reflections (74° at 750 nm) with
silicon mirrors. Actually, they combine it with a pre-filtering that exploits the
intensity of the IR components: the s-polarized component is relatively weak
compared to the p-polarized component (s:p ratio ∼10-3) but comparable to UV
radiation, so it is suppressed before the conversion from NIR to UV by passing
through a series of thin 2 μm polymer films installed at the Brewster angle. After
generation it uses the mirror pair, as in Fig. 2.22.

Fig. 2.22: Setup with a mirror pair as filter.

The result is that the two filtering schemes allow suppression of NIR pulses up to
∼50 nJ and shift their central energy to ∼2 eV (622 nm) due to the spectrally non-
uniform reflectivity of the silicon mirrors. The energy of the transmitted UV pulses is
300 nJ. Another working group [89], opts for other possible solutions such as the use
of three dichroic wedge separators (LAYERTEC GmbH): reflecting the NIR and
transmitting the UV (all wavelengths below 350 nm are reflected). The attenuation of
the NIR pulse energy by 4 orders of magnitude (residual energy 28 nJ) is achieved by
retaining more than 85% of the energy. In contrast to the previous system, the
reflectivity of the separators in the deep UV spectral region is greater than 85% for
both s-polarized and p-polarized laser beams, allowing both linear and circular UV
radiation to be reflected.

37
An innovation technique exploits the geometry of the output beam, in particular the
divergence of the different components. This results in a reflecting disc consisting of
an outer ring that shapes and focuses the high divergence IR pulses, and a core that
is responsible for shaping and focusing the low divergence XUV/soft X-ray pulses.
The lower divergence of the XUV/soft X-ray pulses is attributed to the higher energy
of the photons [90, 91].
As is summarized in Table 2.1, in general, there is a high level of attenuation of IR
pulse and transmissivity of XUV radiation. In chapter 4, however, we will describe
the limits of all these technologies and the innovations of the filters we manufacture.

38
Chapter three
Experimental Apparatus
In this chapter are described the main experimental apparatus used for this thesis.
Each section is devoted to a specific stride of the activity: FLICE, hollow waveguide
characterization and HHG/filtering set-up.

3.1 Fabrication set-up

This section describes the FLICE technical equipment for the production of fused
silica filters. In Fig.3.1 shows the setup for Femtosecond Laser Micromachining with
the related devices.

Fig. 3.1: Schematic experimental apparatus for femtosecond laser writing. The red line represents the IR line, at 1030 nm: TM -
turning mirror; L1 - 75 mm focal length lens; L2 - 150 mm focal length lens; L3 - 400 mm focal length lens; HWP - λ=2
waveplate; P - polarizer; LBO - Lithium Triborate crystal. For the green line, at 515 nm: TM - turning mirror; L4 - 800 mm focal
length lens; SH - mechanical shutter; CAM - imaging camera; OBJ - focusing objective; SM - glass sample; TS - translation
stages.

39
3.1.1 Laser source

One of the operating principles of the FLM, as described in chapter 1, is the need for
the available femtosecond laser to have a flexible repetition rate. The laser source for
micromachining is provided by a Satsuma HP2 (Amplitude Systemes S.A): an air-
cooled commercial femtosecond laser system with an ultra-fast diode-pumped fiber
amplifier and an electro-optical pulse picker, which allows pulses to be delivered at a
repetition rate from 1 MHz to 40 MHz. The pulse duration can be adjusted from 230
fs to more than 10 ps and its central wavelength is 1030 ± 5 nm. A beam quality of M2
< 1.2, a beam circularity > 87%, a beam pointing stability of < 25 µrad/°C, a long term
mean power stability of < 2 µrad/°C and a long Term Mean Power Stability of < 1 %
rms over 100 hours with a warm-up time of < 30 min. The beam power is measured
to be in the order of 10 W at 1 MHz and can be adjusted by an internal attenuator.
The laser is vertically polarized with respect to the optical table. An ambient
temperature of 22 ± 1 °C and humidity around 40% must be maintained for optimal
working conditions and all laser parameters are monitored by external software.

3.1.2 Beam steering

At the output of the source, the femtosecond laser beam is guided with a system of
optical elements, the purpose of which is to focus the beam into the fused silica
substrate at a precise wavelength, polarization, and power. After the source, two
mirrors deflect the beam towards two lenses that form a telescope necessary to shape
the cross-section of the beam before it enters the next stage. The beam enters a half-
wave plate which is mounted on a rotating gear stage followed by a polarizer. The
combination of these two systems allows the power to be varied by rotating the plate.
For our fabrications, the sample will receive a power between 50 and 320 mW which
can be adjusted by remotely controlling the rotation of the half-wave plate with the
A3200 software. A calibration of the rotating stage is necessary for each production
run, as the output power is not an absolute value and can change slightly due to
environmental factors. The power is then measured by means of a power meter close
to the target position, with an uncertainty of a few mW, and each desired power can
be associated with a specific position of the half-wave plate that is translated into a
numerical value, which enters as an input into the control software. A calibration of
the rotating stage is required for each manufacture, as the power output is not an
absolute value and can change slightly due to environmental factors. Power is
therefore measured by means of a power meter close to the target position, with an
uncertainty of a few mW, and each desired power can be associated with a specific
position of the half-wave plate which is translated into a numerical value, which
enters as input into the control software. Subsequently, a mirror sends the beam to
the second harmonic generation (SHG) stage, resulting in a wavelength 𝜆 = 520 nm.
40
This step is performed because a shorter wavelength increases the ionization process.
The laser, consequently, is focused with a lens into a Lithium Triborate (LBO) crystal
that generates the second harmonic. To optimize the SHG, the LBO is kept in an oven
at a suitable temperature, being a birefringent crystal whose refractive index depends
on temperature and in order to obtain type I phase matching conditions: due to the
laws of conservation of energy and momentum, the second harmonic has a
polarization orthogonal to the fundamental, i.e. a vertical polarization. After the
crystal, another lens is placed to collimate and widen the second harmonic beam, so
as to fill the entire aperture of the objective that irradiating the sample. The SHG
stage is followed by an electromechanical shutter Uniblitz which is operated by the
A3200 software in synchrony with the translational stage to select the sample
irradiation window: the closing and opening time is ∼ 10 ms. Finally, the beam is
focused into the sample with a Zeiss® 63x dry objective of 0.65 numerical aperture,
which has a correction collar for spherical aberrations.

3.1.3 Translational stage

To obtain a specific three-dimensional structure, you have a mechanism that moves

the sample relative to the target, in this case a 1D stage that ensures the movement of
the target along the z axis and a 2D Aerotech stage (ANT130-035-L-ZS-PLUS and
ANT95-50-XY-CMS-ULTRA) that moves the sample in the xy plane. Due to the
imposed polarization of the laser beam, the x-direction is the preferred writing
direction, along which the generated nanograins are aligned (see section 1.3.2). The
maximum stated travel in both x and y directions is 50 mm, with a motion accuracy
of 100 nm and a maximum speed of 150 mm/s. Alignment between the beam and the
sample is made possible by the use of machine vision system (CCD camera).The
motion of the stages is imposed by a sequence of G-CODE instructions or thanks to a
custom MATLAB program: it generates a code for a point-by-point translation of the
stages following the desired geometry.

3.1.4 Wet chemical etching

The second step of the FLICE technique is chemical etching, the previously irradiated
fused silica sample is exposed to an aqueous solution of hydrofluoric acid (HF) in a
dedicated environment. The aqueous solution of hydrofluoric acid, has a
concentration varying between 10 % and 20 %. The solution with the sample is
contained in polymer beakers, which are placed in an ultrasonic bath at about 35 °C
to increase the effect of the acid. These steps have to be performed under a fume hoof
to remove the toxic fumes produced by the HF reactions.
After the etching process the sample is washed with a solution of Isopropyl alcohol
in deionized water, again in an ultrasonic bath, to remove residual chemicals and

41
any glass fragments trapped within the channels. After drying with compressed
nitrogen, the sample can be handled unprotected and the result of the etching is then
evaluated with an optical microscope.

3.2 Hollow Waveguide characterization set-up

As will be extensively described in the next chapter, the hollow waveguide

filters have been optically characterized in order estimate the coupling losses and to
acquire the fundamental mode intensity profile, to be compared with the theoretical
prediction. For this purpose, a coupling set-up was assembled as shown in Fig. 3.2.

Fig. 3.2: Schematic experimental apparatus for hollow waveguide characterization, with optical elements operating at 780
nm: TM - turning mirror; HWP - half-wave plate; P - polarizer; L1 - 20 cm focal length lens; TS - translation stage; SM -
sample; L2 - aspheric 40x lens; CAM - collecting camera.

The source providing the beam to be coupled is a Toptica laser (FemtoFiber bCARS)
with a central frequency of 780 nm +/- 10 nm (like that used for HHG), pulse duration
> 3.4 ps, 80 MHz repetition frequency, polarization > 95 %, horizontal and air-cooled.
The power used is of the order of 100 mW and is always controlled by a half-wave
rotating plate followed by a polarizer. A biconvex lens is inserted to improve the
energy coupling with the 𝐸𝐻11 guided mode. The coupling is performed manually by
moving the sample that is placed on a specially made sample holder (Fig. 3.3) which
is placed on a manipulation stage with a micrometric resolution that allows
horizontal and vertical translation with respect to the laser beam and tilting in the
same directions. For optimization of the coupling and acquisition of the mode, the
light is collected by a 40x aspherical lens (NA = 0.55), also placed on a translational
stage, with on a Spiricon CCD camera, which sends the image to external software.
Thanks to a defined grating, it is possible to translate the number of pixels into units
of length. The efficiency of the filter is calculated by measuring the power before and

42
after the collecting lens and taking the ratio, introducing a correction factor for the
output value, due to the dissipation of the lens.

Fig. 3.3: Drawing and photo of the filter holder used in the characterization.

3.3 High order harmonic generation

In order to verify the efficiency of the fabricated filters in removing residual IR

radiation from the XUV radiation generated in HHG processes, we are planning to
mount the filter in a HHG setup. Since extreme ultraviolet (EUV), and soft X-ray
radiation (SXR) is strongly absorbed in air, HHG generation performed in vacuum
chambers. In Fig. 3.4, a scheme of the setup used for HHG is reported including the
laser source, the interaction chamber and the spectrometer. The system described in
the following section was installed for HHG generation without the presence of
filters; in Chapter 5 the new devices introduced for measuring filter efficiency and for
other measurements and experiments will be explained.

(( ))
Fig. 3.4: High-order harmonic generation and acquisition schematic setup [96].

43
3.3.1 Laser source

To generate high-order harmonics, ultra-short and ultra-intense laser pulses

interacting with a gaseous medium are used. Ti:Sapphire lasers source is used :to
generate femtosecond pulses In our measurements, 25- fs pulses are used, delivered
at a repetition rate of 1 kHz, with an energy of 1 mJ each. The pulses are spectrally
broadened in a 1 m long hollow-core fiber and temporally compressed by chirped
mirrors. The compressed pulses have a duration of 10 fs and an energy of 300 uJ. The
pulses are sent into the generation vacuum chamber and focused by a 30 cm
focusing mirror inside the capillary.

3.3.2 Vacuum chamber

The generation setup is composed of 4 vacuum chambers:

1. interaction chamber where the chip is placed;
2. chamber containing a first toroidal mirror;
3. chamber with a toroidal and a spherical mirror;
4. chamber housing a diffraction grating and an MCP detector.

Generation phase
The beam enters the vacuum chamber through a glass window. An iris is used
for the alignment of the beam into the chamber. In standard working conditions the
pressure inside the generation chamber is 10-5 mbar A mirror focuses the beam at the
entrance to the central hollow channel of the chip (small focal length 30 cm). The
HHG chip is placed on a specially holder designed to connect the chip to the gas
pipeline. The mounting of the chip is composed of a metal holder and a transparent
plexiglass cover that is directly interfaced to a gas pipe. The chip is sealed to the
cover by a Viton O-ring. The mounting is placed on a motorized 5-axis
stage (Newport, 8081 motorized tilt aligner) capable of translating along the three spatial
directions (x, y, z, with z parallel to the optical axis) and rotating along x and y. A
preliminary alignment of the chip on the laser beam direction is performed in air by using
the 5-axis stage in a manual mode. A fine tuning of the position is made in vacuum
conditions by operating the stage in a motorized mode. The chip is filled with gas by means
of a pipeline. The gas pressure is controlled by needle valve and a pressure gauge.
The spatial quality of the waveguide mode coupled inside the chip is checked on a
screen. To check the coupling in vacuum, we used a diagnostics optical beamline
composed of a wedge mounted on an electronically rotating support that can be
inserted into the laser beampath to send the beam outside the chamber on a CCD.

44
XUV spectrometer
The optical design of this instrument is based on three chambers containing of
grazing incidence optics. In the first chamber, a plated toroidal mirror generates an
intermediate focus used for HHG-based pump-probe experiments. The toroidal
mirror has tangential and sagittal radii of curvature chosen to achieve unitary
magnification with coma correction in the second chamber. The third chamber
contains two interchangeable mirrors with grazing incidence: a toroidal mirror used
to focus the harmonics on the image plane and a spherical mirror to observe the
divergence of the image, which allows the divergence of harmonics along the vertical
direction to be observed (stigmatic or astigmatic configuration). In the last chamber,
two SVLS (Spherical Varied-Line-Space) gratings can be selected: one that covers the
120-5 nm range at low energies and a second that scatters radiation down to 1 nm
(1keV).

MCP and phosphor screen, CCD camera

The gratings spectrally dispersed the HHG signal, which impinges on a vacuum-
compatible detector consisting of a single-stack microchannel plate (MCP) that
transduces the optical signal into an electronic signal. This is followed by a phosphor
screen: electrons multiplied by the MCP hit the screen and are converted back into an
optical signal that is collected by a focusing lens and finally acquired by an Apogee
Ascent A2150 CCD camera.

45
46
Chapter four
Lab on a chip for HHG

4.1 Introduction

In this Chapter we will deal with the integration into a glass device of two main step
of XUV radiation: HHG and filtering. In the first section we will discuss the fused
silica chip devoted to the generation of High order harmonic, although it has not
been developed during this thesis it constitutes the starting point for the design and
development of the filtering device. In fact, both will be integrated into the same
platform. It will continue with the study of the fused silica integrated device for the
manipulation of the IR and XUV radiation devoted to the filtering of the XUV. We
will study different aspects in detail like the theoretical aspects of the idea, the
fabrication parameters and the different configurations.

4.2 HHG in glass chip

The manipulation of HHG beams takes place in grazing incidence on bulky and
expensive optics that require careful alignment and also active stabilization systems
[92][93]. The proposed solution for ultrafast technology can be achieved by
miniaturization: compact sources generating high-order harmonics in capillaries of a
few centimeters length made of gas-filled glass, which behave as hollow waveguides.
Hollow waveguides are already widely exploited in the field of HHG, leading to
impressive results allowing hundreds of times improvement of the intensity of the
harmonics to be achieved [93] and spectral components up to keV of photon energy
[71] in tabletop systems. The flexibility, precision and 3D capabilities of the FLICE
technique to fabricate micro-devices to manipulate gas flows have already been
established for years, the next step is to use the same technique and to guide laser
beams through micro-channels to fabricate fused silica generation chips. The
proposed geometry from A. G. Ciriolo et al. [95] is designed to allow the driving
IR laser beam to propagate in a hollow waveguide homogeneously filled with a
gas and thus the generation of High-order Harmonics. The device micromachined
using the FLICE technique is shown in Fig. 4.1. A parallelepiped-shaped reservoir of
dimensions 2 × 4.7 × 0.1 mm3 is made inside a fused silica plate of dimensions 10 × 8 ×
1 mm3. This reservoir is used as a camera for distributing the gas within an

47
embedded microchannel that acts as a hollow waveguide for ultrashort lasers. The
microchannel extends along the 8 mm length of the glass and has a diameter of 130
µm. The diameter and length must be chosen carefully to achieve an efficient HHG
process.

Fig. 4.1: Design of the micro-chip of generation [95].

In the work of Marcatili et al. [66] it is shown that in hollow waveguides filled with
fused silica gas the lowest loss mode is the hybrid 𝐸𝐻11 mode, whose intensity profile
as a function of radial coordinate r is given by:
𝑟
𝐼(𝑟) = 𝐼0𝐽02 (2.405 ) (4.1)
𝑎

where 𝐼0 is the laser peak intensity, 𝐽0 is the zero-order Bessel function and 𝑎 is the
radius of the capillary. From the field attenuation constant present in Eq. (2.21)
derived that 𝛼 ∝ 𝜆2 ⁄2𝑎3 we can state that the losses can be set arbitrarily small by
choosing 𝑎 ≫ 𝜆, but in contrast it must be small enough to ensure the peak intensity
required for efficient HHG, so there are values of 𝑎 must be between 10 µm and 200
µm. In section 2.4.1 we have already introduced the conditions between 𝐿𝑐𝑜ℎ and 𝐿𝑎𝑏𝑠
for phase matching, it is also observed that there is a saturation of the harmonic
signal for an average length 𝐿𝑚𝑒𝑑 greater than a few 𝐿𝑎𝑏𝑠 : the harmonics emitted
beyond the first are reabsorbed, even for perfect phase matching (𝐿𝑐𝑜ℎ → +∞), and
does not depend on the gas density. It is found that to reach the optimal conditions
for phase matching it is necessary that 𝐿𝑐𝑜ℎ > 5𝐿𝑎𝑏𝑠 and 𝐿𝑚𝑒𝑑 > 3𝐿𝑎𝑏𝑠 . As Fig. 2.10
illustrates, for low coherence lengths the signal is suppressed by absorption.
Considering that the typical absorption length of noble gases is less than 1 mm [70],
the desired waveguide should be longer than 3 mm. A value of 8 mm is selected for
this device, it constitutes a good compromise in order to have a compact device. It is
connected to the reservoir through four equidistant microchannels, whose relative
distance is 1.2 mm, with a diameter varying from about 50 µm (at the base of the
reservoir) to about 40 µm (at the surface of the hollow waveguide surface). The
48
device has been designed to work under vacuum and is directly connected to a
continuous gas tank. The gas flow was modelled using simulation software. The
simulation results found that the velocity magnitude has a uniform profile in the
central part of the channel which is directly filled by the small injection channels.
However, an abrupt change in behavior occurs at the outlets to the vacuum chamber,
where the gas undergoes significant acceleration. The micro injection channels, being
uniformly distributed, allow an almost uniform gas density in the central part of the
hollow waveguide, which extends over a length of 3.6 mm (Fig. 4.2). The gas density
within the channel scales linearly with the pressure in the reservoir: by monitoring
the support pressure, it was possible to achieve accurate control of the gas density in
the hollow waveguide. This is of paramount importance as the control of the
generating medium is crucial for phase-matching and consequently for applications
such as HHG and APG, which are strongly influenced by collective effects due to the
density and spatial distribution of the generating medium. This device has a high
degree of flexibility, making it possible to achieve different density profiles by
varying the number, shape and position of the microinjectors.

Fig. 4.2: Numerical simulation of helium-gas fluidics inside the micromachined device, showing (a) the gas
velocity and (b) the gas density along the central axis as a function of the backing pressure [95].

Fig. 4.3 shows different spectra of harmonics generated inside the helium-filled
device at different backing pressures with an energy of the ultrashort pulses used to
drive HHG of 500 µJ. It is observed that as the pressure increases, the spectrum yield
at shorter wavelengths undergoes an improvement compared to the longer
wavelengths. In Fig. 4.4 we show the HHG spectra normalized to a pulse energy of

49
respectively 420 µJ and 500 µJ, respectively. In both cases, the pressure dependence
of the cutoff is non-linear and a maximum HHG extension can be observed for
intermediate pressures. As far as the generation yield is concerned, a considerable
improvement can be observed by increasing the pressure up to 400 mbar, beyond
which saturation occurs. From these spectra it is concluded that for helium, the
energy of the driving pulses does not significantly influence the shape of the HHG
spectrum, but by increasing the energy of the pulses, the XUV spectrum becomes
broader, extending up to 200 eV. The pressure dependence shown by the HHG yield
is due to the combined effect of phase-matching with the phase mismatch between
the fundamental and harmonic fields and absorption by the gas, which increases
with increasing pressure.

Fig. 4.3: HHG spectra generated by 500 µJ in helium at different backing pressures
(from 25 to 1000 mbar) [95].

Fig. 4.4: Log-scale HHG spectra (not normalized) at the cutoff plotted to
the photon energy. The pulse energy is respectively 420 µJ and 500 µJ.
[95].

50
Comparing the HHG output inside the gas-filled microchannel with that obtained in
the more most used interaction geometry involving a gas jet: a higher generation
yield is obtained in the microchannel, where the overall spectral intensity is more
than 20 times that obtained with the pulsed jet. A further improvement in harmonic
generation can be achieved by overcoming the limitations of phase-matching, such as
the exploitation of Quasi Phase Matching (QPM), which has already been
demonstrated.

4.3 Integrated X-UV filter idea

As already partially described in section 2.5: at the output of the HHG stage, the
fundamental (IR) and generated (XUV) beams overlap. This fact prevents the
possibility of using only the XUV radiation, as required, for example, by attosecond
experiments. In the same section, we have already illustrated the various filters that
are used to remove the residual IR beam: traditionally, metallic filters are installed,
which transmit 70% of the generated beam and attenuate the fundamental by a factor
of 106 . These filters have many limitations:

• they transmit a limited HHG bandwidth;

• they require periodic replacement due to their damaging by the high
laser intensity used;
• they are relatively bulky: several filters are often used in series and
require space for beam propagation.

Other filtering methods illustrated above also have some disadvantages, such as the
multi-mirror transmission system, which requires a lot of installation space. The
main aim of this thesis, therefore, is to create highly efficient filters, even with
higher performance than conventional ones, which do not have the limitations just
mentioned.
The filters manufactured should have the following characteristics:
1. be made of materials less prone to optical damage so as to be replaced
much less frequently;
2. the operating principle shall be independent of the bandwidth of the
HHG;
3. be very small in size to create a compact system.

In addition to these main features, one can add the possibility of preserving the IR
beam from absorption (used for experimental or diagnostic purposes), instead of
being absorbed as is the case with traditional filters.
To avoid the damaging of the filtering device we will exploit the principle of a
hollow optical waveguide fabricated in fused silica. In fact, we can manipulate and
51
 deviate the IR residual light coupling it into an “empty” hollow waveguide. This
working principle is broadly used in ultrafast-high intensity laser systems [82] and
demonstrated their robustness.
To ensure no bandwidth limitations for the transmission of the XUV radiation we
will exploit the co-propagation characteristic of the generated and driving field. By
studying the properties, propagation and profile of the beam exiting the generation
chip [91, 97, 98], it is observed that the center of the beam is composed of the
generated radiation, whereas the co-propagating IR pulse is distributed at the
extreme end of the wavefront profile. From this analysis it is concluded that the
radius of the co-propagating XUV beam is smaller than the radius of the IR beam.
The distribution of the radiation suggested that it was possible to guide the IR
driving field and deviate it from the generated beam, that will continue to propagate
in the generation direction along a dedicated empty channel. This allows the IR beam
not to be destroyed, but to be diverted and guided to another system for exploitation.
The architecture of the designed filter is in Fig. 4.5 and Fig. 4.6.

Fig. 4.5: Design of the filter.

52
 Fig. 4.6: Path of the copropagating beams in the integrated filter with
generation chip [96].

We have a curved hollow waveguide with a diameter of 130 µm to guide the IR

radiation and a much smaller straight one, centered in the XUV path, in which the
harmonic signal propagates. We will manufacture UV radiation channels with
different diameters to test experimentally which value is optimal for maximizing the
transmission of the radiation generated and deflecting the IR radiation (Fig. 4.7).

Fig. 4.7: Filtering idea [96].

The part of the IR radiation that propagates in the XUV channel will have very high
losses and will therefore be strongly attenuated. From the article [96] we find that
simulation the radius of the XUV profile varies between 10 and 30 µm (Fig. 4.8), so
we will vary the diameter of the guides around that range. Another parameter to
evaluate is the radius of curvature of the IR guide. It is known that as the radius of
curvature increases, the attenuation decreases significantly, as shown in Fig. 4.9 [99].
From this consideration, a radius of curvature value of 300 mm was chosen and an
inclination respect to the straight guide of 2.5°: this value is an excellent compromise
53
to reduce losses and have a real division between the two guides, considering that
the filter is 1.9 mm long.

Fig. 4.8: XUV radiation intensity profile simulation [96].

Fig. 4.9: Attenuation as a function of radius of

curvature [99].

4.4 Filtering chip fabrication

The fused silica slabs that contain the filters are 1.9 mm long, 5 mm wide and 1 mm
high (Fig. 4.10), therefore a very small chip, as required in the third characteristic.
54
During the etching phase, the non-irradiated area is also corroded by the HF, so the
surface is affected by the acid and this results in a reduction of several micrometers
in the size of the chip. For perfect alignment with the generation chip, on which the
filter will be integrated, the channels are positioned at the same depth, i.e. 0.33 mm
from the surface.

Fig. 4.10: Dimensions of device.

4.4.1 IR waveguide parameters

For the fabrication of the IR waveguide, we will follow the strategy of irradiating the
surface which will be subsequently etched and separated from the fused silica sheet.
This cylindrical surface will be divided into adjacent continuous lines along the x-
direction, separated from each other by an angular distance of 1.5° (Fig. 4.11). In
order to avoid the beam passing over previously irradiated areas, the deepest line
will be irradiated first and then the lines composing one half-surface of the cylinder
will be irradiated, from bottom to top. The lines making up the other half-surface will
be formed in the same way. One of the main issues we had to analyze and correct is
the strong asymmetry in the cross section of the waveguide [13]. The beam focused
on the sample has a Gaussian profile: perpendicular to the direction of propagation
of the beam, the size of the waveguide is given approximately by the focal diameter
of the beam diameter 2𝜔0 , while along the direction of propagation, it is given by the
confocal parameter 𝑏 = 2 𝜋𝜔02 /𝜆. For focal diameters of the order of a few
micrometers, this results in a large difference in waveguide size in the two directions.
To compensate for this asymmetry, the rays of the transverse profile will not be
identical, but we will have an elliptical profile whose largest radius will be along y
being the direction with the smallest focal radius. An optimum value was found for

55
the radii in the x-y plane to obtain a circular guide in relation to the mean etching
time: 55 µm along y and 45 µm along z.

Fig. 4.11: Steps for radiating the cylindrical surface. Step 1: irradiation of the deepest line; step 2: irradiation, from the
bottom upwards, of the lines that make up one half of the surface of the cylinder; step 3: irradiation of the lines that
make up the other half of the surface, again from the bottom upwards.

A further fundamental consideration is the focusing position in the sample. When a

laser beam is focused inside a glass plate of refractive index 𝑛 by means of a
microscope objective, the focus position is different from that obtained with the same
focus in air. This well-known effect is due to the refraction of light beams as they
pass through the air-glass interface. It can be shown that the depth of focus in the
glass plate is equal to 𝑛 times the depth it would have if only air were present [99].
This fact translates that all translational movements in the longitudinal direction (z
axis) must be reduced by a factor 𝑛 = 1.46, which is the refractive index of fused
silica. The guide was divided into an initial straight section s1 3 mm long (in this
channel, IR e XUV co-propagate), a curved section s2 (division zone between XUV
and IR) and a further straight section s3 to the end of the sample as shown in Fig.
4.12. The s1 section has been designed straight to optimize coupling with the filter.
The irradiation power was 300 mW, with a writing speed of 1 mm/s. During the
etching phase, the HF will remove the irradiated part, then the outer surface of the

56
channel, allowing the inner glass volume to be removed, by ultrasound, from the
sample and create a hollow waveguide. In order to reach every point of the
irradiated volume and to have a homogeneous incision, microchannels were created
perpendicular to the guide, starting from the surface and arriving at the bottom of
the guide. Being on the surface, they will empty first and act as acid injectors along
the entire length of the guide. (Fig. 4.13). They were always manufactured at a power
of 300 mW, at a writing speed of 0.3 mm/s, spaced 0.5mm apart. During
manufacture, it was decided to irradiate a line perpendicular to the center of the
guide to facilitate removal of the non irradiated glass.

Fig. 4.12: IR channel subdivision.

Fig. 4.13: Microscopic image of the microchannels, showing their size and distance.

57
4.4.2 UV channel optimization of radius and profile

The XUV channel is straight and it is fabricated from the end of the s1 section and the
end of the sample. The fabrication technique for XUV channels, due to their small
size, is different from that for IR guides. As shown in Fig. 4.14, several parallel lines
are irradiated in the y-direction equally spaced by a gap of 0.001 mm (with a few
exceptions, as Fig. 4.14), at a speed of 0.3 mm/s and at different powers.
The size of the channels will therefore be a function of the power in the z-direction
and the number of lines and the gap value between them in the y-direction, all other
parameters being equal. Further factors influencing the size of the channels are:
writing speed, etching time and HF concentration.

Fig. 4.14: Irradiated glass with 5 parallel lines with a gap of 3 µm.

An important task was to experimentally find the parameters to manufacture

channels with the desired diameter and circularity. The strategy was to play with the
combination of laser power and number of adjacent lines in order to modify
the width (dy) and thickness (dz) of the XUV channels. Before analyzing the data in
detail, it is necessary to point out some important factors. The etching time affects
both the XUV and the IR channel, so an optimum etching value was found at the
same time for both channels: 1 h and 45' with variations of 10 minutes more or less
depending on the sample. The asymmetrical transverse profile of the irradiated areas
must also be taken into account when manufacturing XUV channels. In the following
section we will experimentally analyze the link between the power and depth of the

58
channel and the number of adjacent lines and the transverse radius. As already
mentioned, this study will be necessary in order to derive parameters allowing the
replication of circular channels. Microchannels, always 5 mm apart, were also
fabricated for the XUV guides to facilitate acid entry throughout the irradiated
section. Fig. 4.15 show a filter after the irradiation.

Fig. 4.15 Filter after process of irradiation

First sample (Table 4.1) was made as a reference to find the best parameters of the
XUV channels, therefore it only has and an etching time of 1h and 25' (slightly less
than that the one normally used for the whole device).

Average intermediate Final values Final edge values Final edge values Power Number of
values alog y (µm) along y (µm) along y (µm) along z (µm) (mW) lines
not formed not formed not formed not formed 40 1
not formed not formed not formed not formed 50 1
not formed not formed not formed not formed 50 3
25 2 1 3 60 1
27 2 1 3 60 1
30 6 4 7 80 3
35 10 7 8 80 5
37,5 13 10 9 80 7

Tab 4.1 The table summarizes the data obtained from a sample to assess the relationship between powers, number of
lines and dimensions. The results obtained were used as a reference for XUV channels.

The first observation is that below 60 mW are no channels present, we can therefore
state that below this power we have no changes in the of the fused silica (Fig. 4.16 A).
From Fig. 4.16 B and C it can be observed that the channel size along y is not
constant, in particular a larger value is observed near the microchannels and a strong
narrowing is observed at the ends of the sample. This phenomenon was found in all
the samples, accentuated especially in the smaller diameter guides. Considering the
channels irradiated with a power of 80 mW, it can be observed that as the lines
increase, a linear increase in the maximum value along y is created (Fig 4.17). The
increase of the diameter along y is linear and with a similar trend at different points
along the channel, as shown in Graph 4.1. The depth of the channels remains more or
less constant with the same power and as expected there is an increase with
increasing power; this fact will be more evident in the next analysis.

59
Fig. 4.16: Sample of reference. A below of 60 mW, the guide is not formed; B and C show the inhomogeneous of channels.

Fig. 4.17: Sample’s edge of reference a) channel 80 mW and 3 lines b) channel 80 mW and 5 lines c) channel 80 mW
and 7 lines.

Graph 4.1: The graph shows the variation of the diameter along y for different positions of the channel:
intermediate, in the end and at the edge. These measurements are related to the number of irradiated lines.

60
Table 4.2 summarizes a series of filters in which we managed to obtain almost
circular channels with very similar etching times (Fig. 4.18).
Average intermediate Final values Final edge values Final edge values Power Number of Figure
values along y (µm) along y (µm) along y (µm) along z (µm) (mW) lines
48 40 44 48 200 10 Fig. 4.18 A
33,5 32 29 31 100 9 Fig. 4.18 B
33 34 28 26 90 7 Fig. 4.18 C
32 30 18 18 80 5 Fig. 4.18 D
25,5 19 16 17 70 3 Fig. 4.18 E
20,5 11 12 15 65 3 Fig. 4.18 F

Tab. 4.2: The table shows the measurements of filters with different diameters of the XUV channel, also considering the
circularity obtained. The powers and the number of lines required for their manufacture are then shown.

Fig. 4.18: XUV channels for different filters. A) channel 200 mW and 10 lines, B) channel 100 mW and 9 lines, C)
channel 90 mW and 7 lines, D) channel 80 mW and 5 lines, E) channel 70 mW and 3 lines, F) channel 65 mW and 3
lines.

From these data we observe the phenomenon already mentioned above, as the power
decreases there is a greater inhomogeneity along the XUV channel. As noted earlier,
the depth decreases as the power decreases, although it is not possible to identify a
specific trend (Graph 4.2). On the contrary, the width of the guide varies almost
linearly as the lines and powers vary (Graph 4.3); this was also found previously. It is
interesting to note that the 70 mW and 65 mW filters almost all have very different
values from the filters produced with slightly higher powers. It can be assumed,
considering that at values below 60 mW no channels are formed, that these powers
are a manufacturing limit zone where plasma formation phenomena are inconstant
and not complete. Observing the intermediate values of these filters, it can be
deduced that it was not possible to obtain channel diameters of less than 20 µm with

61
this technique: two filters with KOH are therefore being manufactured to try to
obtain channels with diameters below 20 µm.

Graph 4.2: The graph shows the variation of the diameter along z (depth) at the edge of the
filter in relation to the power.

Graph 4.3: The graph shows the variation of the diameter along y (width) at the edge of the filter in
relation to the number of lines.

62
To solve or at least diminish the problem of inhomogeneity, increasing the number of
channels could be considered in the future. This development could show if indeed
there is a problem of inefficiency in FLM processes or acid fluidity in the structure.
In chapter 5 we will show the results of the characterization of some filters, and for a
first study of the influence of the XUV channel on the propagation of the IR
radiation, some straight and curved rails without XUV channels have also been
manufactured.
A chip with two straight guides equidistant (1mm) from the filter was also fabricated
to have a reference in the generation phase (Fig. 4.19).

Fig. 4.19: the picture shows the photo of the filter with the reference channels and
the microscope details.

4.4.3 IR filtering optimization: double IR waveguide.

The design of the filters described so far could be modified to increase the profile of
the guided IR beam and thus increase the filtering efficiency. The IR beam has lateral
"tails" which are not guided by the IR channel, thus resulting in a loss of this area of
the intensity profile. This unguided portion can undergo various processes, such as
scattering and reflection, and thus reduce the purity of the XUV beam. A possible
solution is the addition of an additional channel to collect and guide this part of the
beam as well. Therefore, a modification of the filter architecture was considered, no
longer one channel for the IR radiation, but two identical channels curving in
opposite directions as shown in Fig. 4.20. We called this filter "Bifurcated". A first
prototype was fabricated which maintains the same dimensions as the previous
filters, with the radius of the IR guide still about 65 µm and the radius of the XUV
channel about 16.5 µm. This prototype will be analyzed and compared with the other
filters in the next chapter, to understand the actual improvement of this new
geometry. This sample underlines another fundamental aspect: the ductility and
63
potential of the FLICE technique. This technique allows you to create increasingly
complex geometries relatively easily, while maintaining the same setup and
manufacturing process. In this prototype, for example, it was sufficient to add an
identical channel to the single-channel IR filter program by inverting the degree of
curvature; other parameters and processes remained identical.

Fig.4.20: Microscope image of the “Bifurcated” filter

from above (x-y plane) and at the edge (y-z plane).

64
65
Chapter five
Towards lab on a chip for HHG and XUV
filtering

5.1 Introduction

In this chapter we will present the characterization of the filters and preliminary
results on filtering. The characterization of hollow waveguides fabricated using the
FLICE technique consists of coupling laser light into the waveguide to measure
significant parameters such as the intensity profile of the guided mode and insertion
losses. To perform waveguide laser light coupling, a suitable laser wavelength must
be selected according to the specific application of the device. A target is used to
focus the laser beam into the entrance of the hollow waveguide; this method is called
end-fire. As far as measurements on the attenuation of the filter integrated in the
generation chip are concerned, only one measurement was possible with a
preliminary filter. The measurements were to be carried out by another research
team, but for technical reasons and some unforeseen events the new setup for the
new generation and filtering experiments is not yet available at the time of delivery
of the final work.

5.2 Optical characterization of the integrated filters

From the work of Marcatili et al. [66] it follows that the coupling of a laser beam
propagating in free space in a hollow waveguide can be described by the projection
of the incident field profile onto the proper modes of the hollow waveguide.
Without describing the steps involved in this phenomenon, it is derived that in order
to have 98% of the energy (maximum value) coupled in the 𝐸𝐻11 mode the
condition:
𝜔1
= 0.6435 (5.1)
𝑎

where 𝜔1 is the beam radius before entering in the hollow waveguide, or beam waist,
and 𝑎 the radius of the hollow waveguide, must be satisfied. To obtain the condition
described above, it is necessary to insert a lens whose focal length allows this ratio to
be achieved, focusing the beam in the channel. The available characterization setup is
designed to use a lens with a focal length of 200 mm. The purpose of the
66
characterization performed is to collect absolute maximum transmittance values and
compare, under the same conditions, the different filters manufactured in order to
understand which dimensional and geometrical parameters allow a maximum
relative efficiency. This choice is also supported by the working conditions in which
the filter will be used, which are not currently replicable. The filter, as described in
section 5.3, is in fact placed in contact with the generation chip in such a way that the
output channel of the chip is aligned with the input channel of the filter. Therefore,
no optical elements are provided to maximize the coupling and therefore the
optimization conditions would not be met anyway.
The characterization of the waveguide is done by analyzing the intensity profile of
the guided mode at the output of the device with appropriate Spiricon software.
Such software approximates the beam as a Gaussian function, even if it corresponds
to a Bessel function; in particular the intensity profile diameter of the waveguide
mode intensity profile of the waveguide mode is measured where the peak intensity
is reduced by a factor of 1⁄𝑒 2.

The coupling and measurement process occurs in the same way for all filters or
simple hollow waveguides. The first step is the coupling of the pulse into the
waveguide, using the image collected by the CCD. As described at the beginning of
this section we know from theory [66] that the mode with the least loss is 𝐸𝐻11 , so we
try to find the intensity profile (Fig. 5.1) (see paragraph 4.2) of this mode.

Fig. 5.1: Mode profiles 𝐸𝐻11 , 𝑇𝑀01 𝑎𝑛𝑑 𝑇𝐸01 .

The next step is to measure the power before and after the waveguide with a power
meter, to quantify the losses due to the curvature of the waveguide [100], the
propagation in the waveguide [101] and to a small extent to the coupling. As each
optical element has an inherent loss, the loss due to the pick-up lens was quantified
by finding approximately 7.2% attenuation. The output power was therefore
increased by this loss. In order to separate the part of the power leaving the IR guide
from that which is not guided but still passes through the glass, the geometry of the
filter is used. Since there is no loss in air, we measure the output power at about 40
cm from the collecting lens: at this distance the separation between the deflected IR

67
radiation and the unguided one (which continues straight into the sample) is such
that we can measure one or the other without having the overlapping of the beams.
We also measure the power immediately after the collecting lens to quantify the part
that propagates into the filter without being deflected.
The first characterized samples consist of a single IR channel with an average radius
between 67 µm and 70 µm. There is one sample in which the guide is straight. The
other two, on the other hand, have a curved guide, with the same radius of curvature
(300 mm), but with bending angles of 1.5° and 2.5° (as in the filters) with respect to
the x-axis. They are designed to discriminate between losses due to propagation in
the guide and losses due to bending. All samples have the first straight section of the
rail (s1), with radius variation below 4.5%, and therefore the losses due to coupling
are identical. The data obtained are summarized in Table 5.1. As expected, the
transmissivity decreases with increasing curvature. In Fig. 5.2 the obtained mode
profiles are shown, it is observed the survival of modes higher than 𝐸𝐻11 , being the
multi-mode guide, which did not allow to find the lowest order hybrid mode profile.
Sample Average IR (µm) XUV (µm) T(%)
Straight channel 70 - 83,25
Curved channel, 1.5° 70 - 75,09
Curved channel, 2.5° 67 - 63,66
Table 5.1: Show results of samples without the channel XUV.

Fig. 5.2: Mode profile for IR channels with different angles of bending.

Filters with different values for the XUV channels (diameters ranging from
approximately 20 µm to 40 µm) were selected from all the devices produced, also
considering homogeneity and circularity. As the IR dimensions were relatively
similar for each sample, on average below 5%, they were not a main selection
parameter. This choice derives from the fact that the first parameter we want to check
is the influence of the XUV channel radius on the filtering efficiency of the chip.
Table 5.2 summarizes the measured efficiency data and Fig 5.3 and Fig 5.4 show the
profiles obtained. In Tab. 5.2 there is also the column "unguided power", with this

68
 abbreviation we indicate the part of radiation that is collected at the end of the
sample without being guided by the IR channel.

Looking at filters A, B and C we observe a decrease in transmission as the diameter

of the XUV channels increases, as graph 5.1 also shows. The differences between the
filter diameters are between 10% and 15%. We can therefore say that, in these
samples, the increase in the size of the XUV channel causes a decrease in the guided
IR radiation: a part propagates straight into the XUV channel. Part of the decrease in
transmissivity can also be attributed to variations in the radius of the IR guide, as
these variations are relatively small, especially compared to the large variations in
the size of the XUV channels, their contribution remains minimal.

We then reported, again in Tab. 5.2, the results for two filters (D and E) that do not
follow the trend described above. Observing their dimensions, we are unable to
provide a real interpretation. For filter D, for example, given the small size of the
XUV channel, we expected a much higher transmission value. Even considering, in
this case, a larger difference in the radius of the IR guide, the data obtained point to
manufacturing problems that were not found. Even for the E-filter it is possible to
think of manufacturing problems, considering the different cleaning treatments and
the measurements taken. The unguided power for the first three filters shows an
inverse trend in transmission, higher and higher values are measured as the size of
the XUV channel increases. This result was expected: part of the unguided power
propagates in the XUV channel and is transmitted outside the sample. This data does
not reflect the part of the power lost, as mentioned there are several factors
influencing the losses, but decrease in guided power causes a consequent relative
increase in unguided power. Comparing the losses of traditional filters with the
unguided power we find similar values, around 5%. The results just described are
very important and relevant, but they will have to be re-evaluated under real
working conditions to see if the coupling between filter and chip will confirm this
trend.

Sample Radius IR (µm) Diameter XUV (µm) T(%) Unguided power(%)

Filter A 70 33 61,52 5,16
Filter B 67 38 57,29 7,87
Filter C 63 41 37,25 8,00
Filter D 60 21 21,46 10,19
Filter E 65 31 15,86 11,16

Table 5.2: Show results of filter con different radios of guide IR and the channel XUV.

69
Fig. 5.3: Mode profiles for filters A, B and C.

Fig. 5.4: Mode profiles for filters D and E

Graph 5.1: Relations between diameter of XUV channel and transmissivity.

Graph 5.2: Relations between diameter of XUV channel and “unguided power”.

70
From the characterization of the bifurcated filter (IR beam of 68 micro and XUV beam
of 33 micro) a transmittance of 61.11% is measured. The channel size of the XUV is
identical to that of the A-filter and furthermore both samples have a practically
identical transmittance. The new design does not increase the efficiency of the filter,
so different developments will be required for the geometry initially designed. The
measured transmittance is that obtained by trying to characterize both guides. The
individual powers for the two guides were then measured, and it was found that the
radiation is not equally distributed, but in one channel there is 25% of the total
guided power and in the other 75%. It was possible to preferentially direct the
radiation in one guide over the other, by coupling it, without significantly increasing
the losses: the filter behaves like a prototype optical circuit. The profile found is
shown in Fig. 5.5.

Fig. 5.5: Mode profiles for filter “Bifurcated”.

5.3 Experimental apparatus for HHG and XUV filtering

in chip

From the generation setup described in Chapter 3, new devices are introduced for
filter characterization with the spectrometer. The laser pulse is propagated in a 1 m
long hollow fiber to obtain a self-phase modulation effect: a spectrum broadening to
reduce the time width of the pulse. A pair of check-mirrors are then inserted to
rephase the spectrum and compress the pulse, resulting in a duration of 10 fs with a
power about 200 μW. A set of several mirrors is installed in the generation chamber
to compensate for the delay, and a spherical mirror with a focal length of 30 cm
focuses the beam into the generation chip. The previous tilt has been replaced by a
pair of motorized tilts (8081 Motorized XYZθxθy Tilt Aligner - Newport

71
Corporation): one for the chip, the other for the filter; manual coupling is always
possible. The filter is placed immediately after the chip and is fixed with a metal
support and Teflon screws (Fig. 5.6). A prism on a rotating system is used as an
attenuator.

Fig. 5.6: Filter on the holder integrated with the generation

chip in the vacuum chamber.

5.4 Preliminary results of XUV filtering

A preliminary measurement was carried out, using a 1.5 cm long filter with an IR
guiding capillary of 75-μm radius and an XUV microchannel of 10-μm radius (Fig.
5.7).

Fig. 5.7: Filter used for preliminary measurement.

72
The filter was aligned with respect to the main beam coming out of the microfluidic
chip used for generating high-order harmonics. Harmonic generation is performed
with a source similar to that described in section 3.3.1 and the setup described in
section 3.3.2 was used for the measurements. The pulse repetition rate was 1 kHz,
and the pulse energy used is approximately 300 μJ and a pulse duration of 30 fs.
Argon gas at a backing pressure of 90 mbar was used for generation.
To quantify the IR rejection on the XUV path we measured the driving pulse energy
at the entrance of the filter and at the output of the XUV channel. The attenuation
after the filter, calculated as the ratio between the output and the input energy, is
found to be a factor of 10-2. Although the performances of this device are quite far
from those of metallic filters, these results are extremely promising and better
performances are expected from the new devices fabricated during this thesis work.

The HHG spectra obtained are shown in Fig. 5.8. From the spectrum in Fig. 5.8 a, the
comparison between the intensity of the radiation generated with and without the
filter can be observed. The attenuation introduced by the use of the filter is not
uniform, in particular there is a factor of 2 for low order harmonics and a factor of 20
for higher order harmonics. This attenuation can be attributed to the interaction of
the HHG beam with the glass during the propagation along the microchannel.
Indeed, in Fig. 5.8 b you can see, on the y-axis, the comparison between the harmonic
radial profile with and without the filter. The XUV spectrum shows a strong
attenuation of the lateral components of the harmonic radiation with the introduction
of the filter. This result is probably due to the divergence of the XUV radiation, since
as it travels through the channel, the field interacts with the walls, resulting in a loss
of power.

Fig. 5.8: spectrum of XUV a) the comparison between the intensity of the radiation generated with and without the filter b) the
comparison between the harmonic radial profile with and without the filter.

73
74
Conclusions
In the course of this thesis, the great flexibility of the FLICE technique to fabricate
very complex hollow structures in fused silica has been demonstrated several times.
The parameters that it is essential to control and the associated problems to obtain
the designed devices were then highlighted.
Another aspect present in this work is the very high potential of hollow waveguides,
which can be used in many fields and applications.
Thanks to the FLICE technique and the theory of hollow waveguides, it was possible
to create workable filters, although they require further study and development.
Future measurements will be able to indicate the real efficiencies of the fabricated
filters.
The idea of integrable filters using a principle based only on the geometry of the
device has been studied for the HHG, but may find other fields of application.
Future measurements and new filter architectures will be able to show the maximum
performance that can be achieved and overcome the limitations of the filters used so
far.

75
76
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EXECUTIVE SUMMARY OF THE THESIS

Femtosecond Laser Micromachining of glass integrated

devices for XUV filtering in High-order Harmonic Generation
MASTER OF SCIENCE IN ENGINEERING PHYSICS - NANOOPTICS AND PHOTONICS

AUTHOR: ALESSANDRO PALETTI

ADVISOR: PROF. ROBERTO OSELLAME

CO-ADVISOR: DR. REBECA MARTÍNEZ VÁZQUEZ

ACADEMIC YEAR: 2020-2021

the results obtained were used to obtain circular

1. Introduction
The thesis work focused on the fabrication, by
Femtosecond Laser micromachining followed by
Chemical etching (FLICE) of fused silica chips
used as integrable filters for high-order harmonic
generation (HHG). The generation chip is based
on the interaction, inside a hollow waveguide,
between a noble gas molecules and intense
ultrashort IR laser pulses (800 nm). At the output
of this source, there is residual IR radiation that
co-propagates with the generated XUV radiation.
The filter aim to remove this residual radiation
exploiting again the hollow waveguide guiding
principle. It will consist of two hollow channels,
one curving channel to guide the IR radiation and
spatially displace it from the main direction, and a
straight one to allow the transmission of the XUV
radiation. Several devices were manufactured,
varying the size of the channels in order to study
the best geometrical configuration. In the process,
channels and set parameters useful for the
replicability of the devices. The filters were then
characterized to assess their ability to guide IR
radiation, and to understand the optimization
parameters. The prospect of these devices is to
replace the filters traditionally used in HHG and
to pave the way to a future lab on a chip for XUV
spectroscopy experiments.
2. FLICE technique
The FLICE technique is a combination of
Femtosecond Laser Micromachining followed by
chemical etching and allows the fabrication of
hollow structures of the order of micrometers.
FLM was first introduced by K. M. Davis et al [1]
1996. It is a nonlinear phenomena that allows to
induce permanent changes in glass by focusing a
femtosecond laser beam inside it.
Executive summary
2.1. FLM
In the FLM, near-IR photons are absorbed non-
linearly by the glass. Since the photon energy is
less than the energy of the bandgap between the
valence band and the conduction band in the
electronic structure of the glass a multiphoton
absorption process is needed in order to trigger
the process. The focal volume of the laser beam is
the only finite region of space in which changes
are induced, in fact, only the pulse peak will have
such an intensity to reach the non-linear
absorption threshold of the material. The
absorbed energy will allow the excitation of
electrons from the valence band, resulting in the
formation of a plasma. The laser intensity and
frequency will discriminate the plasma generation
mechanisms: multiphoton ionization and tunnel
ionization. These processes are followed by the
main mechanism: avalanche photo-ionization. The
laser pulses must be in the sub-picosecond regime
to have a deterministic and uniform process. It is
necessary to focus the laser pulse, through an
optical system, to form a micrometric focal point
on the material to allow the threshold intensity to
be exceeded. In the present work the transverse
writing technique is used: the sample is translated
orthogonally to the laser beam, so the length is not
limited by the working distance and this allows
writing to depths of even millimeters, which is
essential for creating 3D optical circuits. The
disadvantage of this writing mode is the
formation of channels with high cross-sectional
asymmetry, which is caused by the relationship
between depth of focus and spot size. To
overcome this problem, we find several possible
solutions in the literature. The relative motion and
speed between the sample and the beam
determine the energy deposited on the material
and are important parameters in determining the
final device structure. At intensity peaks around
1012 W/cm2 the so called “nanogratings” formation
takes place that will locally increase the material
etching speed (~ 700 µm/h), thus allowing to
create embedded empty channels.
2.2. Chemical etching
It is known that the overall chemical reaction of
silica in diluted HF solution can be summarized
by:
SiO2 + 4HF → SiF4 + 2H2O (1.1)
2
Alessandro Paletti
The origin of the higher etching speed in fs laser
irradiated regions is probably from ionization,
which favors protonation and from the presence
of nanograting (result of the evolutionary process
of hot-spots), which increase the fluidity of the
acid in the channels. When the polarization of the
field is perpendicular to the direction of
translation, the nanoplanes are parallel to the
writing axis and stretched: the etching rate of the
solution is increased. From reaction (1.1), it can be
seen that there is a rapid saturation of the HF
solutions, this requirement presents a difficulty
for the renewal of the solution in the deep
microchannels. To facilitate this renewal, the
process takes place in an ultrasonic bath. The
concentration and temperature of the solution can
be optimized to accelerate the speed of chemical
etching. An alternative to HF chemical etching
process is KOH etching, which presents a higher
selectivity but also a lower etching speed (~200
µm/h).
One of the difficulties in FLICE manufacturing is
obtaining symmetrical and homogeneous
channels: the continuous flow of solution causes a
greater incision of the inlet areas, with the
consequent formation of a conical structure. These
problems can be solved by varying the
concentration of the solution, the geometry of the
irradiated area and the introduction of additional
HF inputs (incision channels) in other points of
the structure.
3. High-order Harmonic
generation
The HHG is a highly nonlinear effect which
generates coherent radiation in the form of high-
order harmonics of the driving laser frequency
with a duration of attosecond (10−18 s) timescale. It
allows the production of extreme ultraviolet
(EUV) and soft X-ray (SXR) radiation in the form
of a train of attosecond pulses, both spatially and
temporally coherent, which can be used as a
probe to investigate a number of phenomena in
atomic, molecular and solid-state physic. Its origin
is understandable with a three-phase semiclassical
model:
1. Tunnel ionization of an atom interacting with
a strong electric field.
2. Interaction of the free electron with the pilot
field.
Executive summary
3. Recombination of the electron with the ion:
generation of the XUV photon.
It is a cyclic process: the sum of the optical cycles
of the pulse generates an attosecond flux of XUV
radiation. Its spectrum is characterized by three
regions: initially a drop of two or three orders of
magnitude for a few harmonics; a plateau follows
in which the intensity remains almost constant,
extending over hundreds or even thousands of
harmonic orders; followed by a rapid decrease in
the energy of the cutoff photon. Only the odd
harmonics of the fundamental frequency are
observed.
3.1. HHG in hollow waveguide
The fundamental work of Marcatili et al. [2]
explains the wave propagation along a hollow
guide, modelled as a series of reflections with the
inner walls at grazing incidence. It is shown that
when a linearly polarized Gaussian beam is
coupled in a hollow waveguide, the hybrid modes
are preferentially excited and above all only the
fundamental 𝐸𝐻 11 propagates correctly, with
very low losses, through the guide.
3.2. HHG in gases media
HHG is a very low-efficiency process, so mainly
noble gases are used to generate it as they have a
much higher ionization potential than the energy
of the pilot laser. In order to extract energy most
efficiently from the incident wave, the phase
matching condition must be met: the generated
wave must maintain a fixed phase relationship
with respect to the non-linear polarization. This
condition is limited by phase matching effects or
propagation length. From the theory we derive, in
general, the condition for optimal phase matching
is 𝐿𝑐𝑜ℎ > 𝐿𝑎𝑏𝑠 (3.1) and the condition for
conversion efficiency in a uniform long medium
is 𝐿𝑐𝑜ℎ > 5𝐿𝑎𝑏𝑠 (3.2), where 𝐿𝑎𝑏𝑠 is the absorption
length and 𝐿𝑐𝑜ℎ is the coherence length (length
over which the harmonic field constructively
accumulates).
However, for condition (3.1) we have that even
having the coherence length infinite, HHG
emissions saturate as soon as the length of the
medium is longer than a few 𝐿𝑎𝑏𝑠 , and condition
(3.2) at high intensities is reached only transiently.
3
Alessandro Paletti
To obtain a tunable phase concordance, pressure
variation is a popular technique, as in the
generation chip on which our filter will be
integrated, but it is possible to vary other
parameters such as the gas species or the
waveguide size.
3.3. HHG in gas-filled hollow
waveguide
There is a strong improvement in generation
efficiency in gas-filled hollow waveguides if
compared to the traditional generation is gas jets.
These improvements result from the fact that,
despite the relative losses compared to other types
of waveguides, there is a high laser intensity over
a long propagation distance, as it counteracts the
reduction in intensity due to ionization induced
defocusing. In addition, the structure maximizes
the region of interaction between the laser field
and the non-linear medium.
4. Filters in HHG
The basic requirement for filters used in HHG
setups is that they must absorb IR wavelengths
(780 nm) and transmit XUV wavelengths (2 nm to
30 nm). The most common filters are made of
different metals, also used in series: they absorb
IR radiation and transmit XUV. Other systems use
mirrors that either absorb or transmit IR radiation
and reflect XUV radiation. The problem is that in
some cases there is also attenuation or
transmission of part of the XUV radiation. Some
mirrors are inefficient at s-polarizing XUV, but
there are some systems that have very good
reflectivity even for this component, such as
dichroic wedge separators. In general, the
attenuation of IR radiation is greater than 95%
and the maximum conservation of the XUV pulse
is about 85%. All these filters have common
limitations:
• they transmit a limited HHG bandwidth;
• rapid optical damage causing periodic
replacement;
• they are relatively bulky.
Moreover, after the filtering step is not possible to
use the residual IR light.
4.1. Innovative filters for HHG
Executive summary Alessandro Paletti

In the thesis work, filters were designed and built

that could overcome these limitations, while
maintaining, or even increasing, filtering
performance. In order to overcome the band
limitation and preserve the IR radiation, the
operating principle of the filter is based only on
hollow waveguide propagation. A detail analysis
of the generated to observe that the core is Fig. 5.1: Filter, with microscopic photos of some details.
composed of the generated radiation, while the
co-propagating IR radiation is distributed at the
end of the wavefront profile. The radius of the IR
5.1. IR guide manufacturing
beam, in particular [3] from computational
The surface of the cylindrical volume of the guide
simulations we know that in our generation
is irradiated, dividing it into adjacent continuous
configuration the radius of the XUV profile varies
lines along the x direction, separated from each
between 10 and 30 µm. In Fig. 4.1 is shown the
other by an angular distance of 1.5 °. To avoid
scheme of our filtering idea, it is composed of a
overwriting, the deepest line will start to be
straight hollow waveguide that separates into a
irradiated and then, to rise, the lines that make up
130 µm diameter bending hollow waveguide and
a semi-surface of the cylinder will be irradiated.
a straight much smaller central (tens of µm)
The lines that make up the other half-surface will
centred in the XUV path, in which the harmonic
be formed in the same way. In order to
signal is transmitted. The XUV channel will have
compensate for the asymmetry of the focused
diameters to maximize transmission, but still such
gaussian beam of the fs laser, the rays of the
that the IR will not propagate as well.
transverse profile will not be identical, but we will
This geometry makes it possible to guide the IR
have an elliptical profile whose largest radius will
radiation in another direction and pass the XUV
be long and, being the direction with the smallest
radiation in the direction of propagation, with the
radius. An optimal value was found to obtain a
result of separating the two components and thus
circular guide in relation to the average etching
filtering them. Moreover, this system makes the
time: 55 µm along y and 45 µm along z. The
IR radiation available for other applications.
diffraction between air and glass causes a
Again, the propagation of IR in hollow waveguide
different focus position in the sample. A
reduce the optical damage and permits to have a
correction must therefore be introduced on all
compact system.
translational movements in the longitudinal
direction (z axis), i.e. they are reduced by a factor
n = 1.46, which is the refractive index of the fused
silica. The guide was divided into a first straight
section s1 3 mm long (in this channel, IR and XUV
co-propagate), a curved section s2 (division area
between XUV and IR) and a further straight
section s3 up to the end. The irradiation power
was 300mW, with a write speed of 1mm / s.
Fig. 4.1: representation of the idea of filtering. During the etching step, the HF will remove the
irradiated part, then the external surface of the
5. Filtering chip fabrication channel, allowing the internal glass volume to be
ultrasonically removed from the sample and
The device is fabricated in fused silica glass using create a hollow waveguide. Micro-channels
the FLICE technique. perpendicular to the guide have also been
The fused silica plates containing the filters are 1.9 inserted, starting from the surface and reaching
mm long, 5 mm wide and 1 mm high (Fig. 5.1) For the bottom of the guide, to homogenize the arrival
perfect alignment with the generation chip, the of the HF to the irradiated channels.
channels are positioned at the same depth, i.e. 0.33
mm from the surface.

4
Executive summary
5.2. Manufacture of UV channel
The XUV channel, being of small size, is
fabricated by radiating several parallel lines in the
y-direction equally spaced by a gap of 0.001 mm,
at a speed of 0.3 mm/s and at different powers.
The size of the guide will therefore be a function
of the power in the z-direction and the number of
lines and the value of the distance between them
in the y-direction, all other parameters being
equal. The objective is to find experimentally the
parameters to produce a guide with the desired
diameter and circularity. The strategy was to play
with the combination of laser power and number
of adjacent lines to modify the width (dy) and
thickness (dz) of the XUV channels. it is important
to stress that we must take into account in the
fabrication that the etching time affects both the
XUV and IR channels. For our production, the
samples are etched for approximately 1 h 45'.
A reference sample was manufactured with only
XUV channels. It was observed that below 60 mW
no channels are present, below this power we
have no changes in the fused silica. A strong
inhomogeneity was found along y, with higher
values near the microchannels. This phenomenon
is especially pronounced in the smaller diameter
guides. By increasing the number of lines with the
same power, we measure an increase in the
maximum value along y and an increase along z
by increasing the power. Table 5.1 summarizes a
series of filters in which we managed to obtain
almost circular channels. The same phenomena as
previously mentioned were observed. It is
interesting to note that the 70 mW and 65 mW
filters have very different values from the filters
produced with slightly higher powers,
considering that at values below 60 mW no
channels are formed. In order to reduce the
problem of inhomogeneity, we could consider
increasing the number of channels in the future.
Edge values along y (μm) Edge values along z (μm)
44 48
29 31
28 26
18 18
16 17
12 15
Tab. 5.1: Measurements and manufacturing parameters
of the XUV channels of some filters.
Alessandro Paletti
5.3. Setup of fabrication
The laser source for micromachining is provided
by a Satsuma HP2 (Amplitude Systemes S.A):
(Amplitude Systemes S.A.), which allows pulses
to be emitted with a repetition rate of 1 MHz to 40
MHz. The pulse duration can be adjusted from
230 fs to more than 10 ps and its central
wavelength is 1030 ± 5 nm. The laser is polarized
vertically with respect to the optical table. At the
output of the source, the femtosecond laser beam
is guided with a system of optical elements, the
purpose of which is to focus the beam into the
fused silica substrate at a precise wavelength,
polarization and power. The beam enters a half-
wave plate which is mounted on a rotating gear
stage followed by a polarizer. Next, a mirror
sends the beam to the second harmonic
generation (SHG) stage, resulting in a wavelength
λ = 520 nm. This step is performed because a
shorter wavelength increases the ionization
process. As a result, the laser is focused with a
lens into a lithium triborate crystal (LBO), which
generates the second harmonic. The SHG stage is
followed by a Uniblitz electromechanical shutter
that is operated by the A3200 software in
synchrony with the translational stage to select
the sample irradiation window: the closing and
opening time is ∼ 10 ms. Finally, the beam is
focused into the sample with a Zeiss® 63x dry
objective of numerical aperture 0.65, which has a
correction collar for spherical aberrations.
In order to obtain a specific three-dimensional
structure, a mechanism is used to move the
sample relative to the target. Due to the imposed
polarization of the laser beam, the x-direction is
the preferred writing direction, along which the
nanograins are aligned. The alignment between
the beam and the sample is made possible by the
use of a machine vision system (CCD camera).
The second step of the FLICE technique is
Power (mW) Number of lines chemical etching. The previously irradiated fused
200 10 silica sample is exposed to an ultrasonic bath with
100 9
90 7 a solution of between 10 % and 20 %
80 5
70 3 concentration. After the etching process, the
65 3
sample is washed with a solution of isopropyl
alcohol in deionized water, again in an ultrasonic
bath, to remove chemical residues and any glass
fragments trapped in the channels. After drying
with compressed nitrogen, the sample can be
handled unprotected and the result of the incision
evaluated with an optical microscope.
5
Executive summary Alessandro Paletti

6. Towards lab on a chip for HHG 83% whereas for the more inclined one it is 63%.
Filters were then characterized with different
and XUV filtering values for the XUV channels and also considering
homogeneity and circularity. Table 6.1
A preliminary optical characterization of the summarizes the measured efficiency data and we
devices will help in understanding which defined "unguided power" as that radiation which
dimensional and geometrical parameters allow is collected at the end of the sample without being
maximum relative efficiency. guided by the IR channel.
We will acquire with a CCD camera the near field Sample Radius IR (µm) Diameter XUV (µm) T(%) Unguided power(%)
Filter A 70 33 61,52 5,16
of the output modes and measure the insertion
Filter B 67 38 57,29 7,87
losses. The filters geometry (with an initial Filter C 63 41 37,25 8,00
straight portion) ensures that the coupling losses
Tab. 6.1: Transmission and 'unguided power' for filters
will be identical for all of them regardless of the with different channel sizes.
UV channel dimension. We can also make an
A decrease in transmission is observed as the
estimation of the IR light that passes through the
straight channel without being deflected diameter of the XUV channels increases, as also
shown in Graph 6.1. The differences between the
measuring the power in the straight direction.
filter diameters are between 10% and 15%. We can
therefore say that, in these samples, the increase
6.1. Setup of characterized
in the size of the XUV channel causes a decrease
in the guided IR radiation as part of it propagates
The source providing the beam to be coupled is a
directly into the XUV channel. As the variation of
Toptica laser (FemtoFiber bCARS) with a centre
the radius of the IR guide is relatively small, only
frequency of 780 nm +/- 10 nm (as used for HHG),
a small part of the losses can be attributed to these
pulse duration > 3.4 ps, repetition rate of 80 MHz
variations. The unguided power shows higher
and the power is always controlled by a half-wave
values for filters with larger XUV channel sizes.
rotating plate followed by a polarizer. A biconvex
This result was expected: a part of the unguided
lens with a focal length of 200 mm is inserted to
power propagates in the XUV channel and is
improve the coupling. The coupling is performed
transmitted outside the sample, although this
manually by moving the sample: the sample is
figure does not fully reflect the part of the power
placed on a specially designed sample holder that
lost. Comparing the losses of conventional filters
is placed on a micrometer-resolved manipulator
with the unguided power we find similar values,
stage allowing horizontal and vertical translation
around 5%, validating the goodness of our
with respect to the laser beam and tilting in the
devices from this point of view.
same directions. For coupling optimization and
mode acquisition, the light is collected by a 20x
aspherical lens (NA = 0.55), also placed on a
translation stage, with a Spiricon CCD camera on
top, which sends the image to an external
software.

6.2. Results of characterized

The first characterized samples consist of only one

IR guide: one has a straight guide, while the other Graph 6.1: Transmission trend in relation to the
two are curved with the same radius of curvature diameter of the XUV channel.
(300 mm), but with angles of curvature of 1.5° and
2.5° (as in the filters) with respect to the x-axis. 6.3. Preliminary results of XUV
They are designed to discriminate between losses
filtering
due to propagation in the guide and losses due to
bending. As expected, the transmissivity
A preliminary measurement was carried out
decreases as the curvature increases, in fact for the
using a 1.5 cm long filter with a 10 μm XUV guide
straight sample we have a transmissivity of about
beam integrated into the generation chip. The

6
Executive summary Alessandro Paletti

imposed repetition rate was 1 kHz, with a pulse

energy of approximately 300 μJ and a pulse
duration of 30 fs. Argon gas at 90 mbar was used
for generation. The IR rejection on the XUV path
is found to be a factor of 10-2. With the
introduction of the filter, the spectra of the
generated radiation show a non-uniform
attenuation; in particular, for the plus harmonics,
there is a factor of 20 and a strong attenuation of
the lateral components of the harmonic radiation
is found, probably the interaction of the field with
the filter walls.

7. Conclusion
The thesis work has demonstrated the enormous
potential of the FLICE technique and hollow
waveguides. The ability of the filters to guide IR
radiation was shown, and from the first
measurement also to be able to filter, although
further measurements and developments will be
needed to reach the standards of traditional
filters.
A wider field of application for the fabricated
filters is envisaged, given the principle of
operation and the filtering technique.

8. Bibliography
[1] K. M. Davis et al. Writing waveguides in glass
with a femtosecond laser. Opt. Lett., 21(21):1729–
1731, Nov 1996.
[2] E. A. J. Marcatili et al. Hollow metallic and
dielectric waveguides for long distance optical
transmission and lasers. Bell System Technical
Journal, 43(4):1783–1809.
[3] A. G. Ciriolo et al. Integrated Filter for the
Separation between XUV and IR Beam in High-
order Harmonic Generation in a chip. The
European Conference on Lasers and Electro-
Optics 2021, Munich Germany, 21–25 June 2021,
ISBN: 978-1-6654-1876-8.

9. Acknowleggements
This thesis work was possible thanks to Prof.
Osellame and his fantastic team. In particular for
the infinite work, effort and help of Dr. Martínez
Vázquez, to whom all my gratitude goes.