Spectroscopy and Material Properties
Coherent-Beam FTIR Spectrometer With No Moving Parts
F. Keilmann and M. Brehm
Max-Planck-lnstitut f* Biochemie, 82152 Martinsried (Munich), Germany
e-mail: keilmaM@biochem.mpg.de
Abstract
A novel type’ of FTlR spectroscopy based on two coherent
frequency combs is demonstrated. All-electronic interferogram
recording allows simultaneous amplitude and phase spectra.
and fast spectrum acquisition in loops (Ips anticipated),
enabling single-event analysis. Diffraction-limited propagation
suggests use in remote sensing, classical microscopy and
scattering-type near-field microscopy.
Introduction
Infrared spectroscopy is of basic importance for the
characterization of materials in many fundamental and applied
sciences. The widely used Fourier-transform infrared
spectrometer (FTIR) commonly relies on an incoherent thermal
source which emits a multi-octave specwm, to cover at least
the 3-30 pm wavelength region where “fingerprint” vibrational
absorption allows chemical identification. The incoherent
spreading of a thermal infrared beam, however, reduces the
application potential of FTlR microscopy, as well as long-
distance environmental probing. Coherent infrared souces can
overcome this limitation. Of these, gas and semiconductor
lasers have the drawback of a limited hming capability, while
free electron lasers require a large installation. Only rectified
ultrashort light pulses have been shown to ConstiNte well-
suited multi-octave infrared (THz) sources, extending from
microwaves‘ well up into the fmgerprint regionz4 and allowing
coherent FTIR in the mid infrared.’ Here I will show that
broadband THz-infrared spectroscopy can be done in a purely
time-domain manner, rendering the cumbersome mechanical
delay methods obsolete which have been limiting the
performance of both incoherent FTIR and coherent THz-
infrared spectrometry.
Microwave dual beam coherent spectrometer
Both FTlR and THz spectrometers handle the task of massively
parallel spectroscopic probing by interferometric detection.
Our concept is to retain the principle of combining two
interferometer beams, but differs in how these are generated.
Instead of splining a common input, we use two inputs from
two independent sources. This allows offsetting their
frequencies to enable multifrequency-heterodyne signal
processing. To understand the principle in a frequency picture,
consider a coherent-frequency-comb beam which contains a
harmonic series of evenly spaced frequencies nf, where n =
I..N. Superposition of a second coherent-frequency-comb
beam with slightly different frequency spacing &’ = f, - A
where A < f, / 2N then forms a “coherent dual b e a d 6 which
exhibits, by interference, unique power modulations at nf, -
n(f,’- A) = nA. Each modulation element nA can be viewed as a
heterodyne signal which uniquely measures one comb
component. All modulations together can be viewed as a time-
domain interferogram which when Fourier-transformed into the
frequency-domain results in a harmonic, radio-frequency comb
spectrum n A which is an exact replica of the dual beam’s
spectrum. The optical system of a coherent-frequency-comb
spectrometer thus consists of a coherent dual beam, a sample,
and a detector. The realization of this concept was earlier
demonstrated with a microwave spectrometer. In this, a
C-7803-84903/04/520.00 @ZOO04 IEEE
M2.
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coherent dual beam covering the 0.01 I THz range was
generated purely electronically, by independent frequency
multiplication (up to N = 300) of two continuous
monochromatic microwaves at nearly identical frequencies,
generated by two synthesizers.’
Mid-infrared dual b e a m coherent spectrometer
Basic to the time-domain coherent FTIR spectrometer reported
here is the very stable repetition frequency f, obtainable with
mode-locked lasers, and the accordingly precise, equidistant
comb of emined optical frequencies?, Our setup” (Fig. 1)
uses two independent, mode-locked Tisapphire lasers. They
emit trains of 20 and 12 fs pulses, respectively, at near-visible
wavelengths around 800 nm,with repetition rates f, I 87 MHz
differing by A I 2 Hz. It is well known that the frequency
combs emitted by such lasers are generally not harmonic;
rather, each frequency nf, in a given comb is offset by a
common offset frequency fo? We use both beams to generate
mid-infrared radiation, by focusing them separately on 0.5 and
Imm thick GaSe crystals, respectively (Fig. 1). Second-order
nonlinearity generates difference frequencies nf, + fo - mf, - 6
= (n-m)f, and n(f A ) + fo’ - m(f, - A ) - b‘ = (n-m)(f, - A),
~
respectively, which not only lie in the mid-infrared’.‘ but most
importantly, constitute harmonic combs because the offsets
cancel exactly. We collimate both mid-infrared beams and
superimpose them on a ZnSe combiner to form the desired
mid-infrared coherent dual beam.
f
f
GaSe 1,:s
laser
Fig. I: Optical system of coherent FTlR spectrometer. Two
femtosecond lasers with slightly different pulse repetition
frequencies generate, by rectification in GaSe, two infrared
beams which are superimposed on a ZnSe combiner. No
mechanically moving part is involved.
Preliminary experimental results
When monitoring the power with a HgCdTe mid-infared
detector we readily observe the anticipated characteristic power
modulations (Fig. Za) which are mid-infrared interferograms.
They appear about twice a second, when the pulses of both
lasers coincide. Note these interferograms arise from a purely
time-domain scanning with no moving parts, contrary to
former FTIR and TH&4 spectrometers.
Fourier-transforming the interferogram Fig. 2a reveals the
radio spectrum Fig. 2b which represents the mid-infrared
spectrum at the impressive frequency-downscaling by the
nominal factor f, / A = 43.500.000.This is a nominal value
only, because the difference A of the repetition frequencies of
87
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the W O free-Nnning Ti:sapphire lasers is not exactly 2 Hz but
fluctuates and drifts by about 1 Hz during several min.
Consecutively recorded spectra exhibit a similar shape but at
slightly varied frequency scaling (as evident from the example
in Fig. 2c). This is caused by a slow fluctuation or drift of A on
a < I s time scale.
frequency
1-
MI0 700 800 900 KHL
J single radio-frequency component nA which represents a single
600 700 800 900 KHZ
Fig. 2 (a) Infrared interferogram recorded by the HgCdTe
detector. (b) Infrared spectrum calculated by Fourier-
transformation. (c) Infrared spectrum from a subsequent
recording; the slightly changed frequency scaling is due to
laser drift.
The similarity of consecutive spectra is evidence that the
frequencies (and amplitudes) of both infrared harmonic combs
remain highly stable on the short time scale needed to acquire a
single interferogram (100 ps). Thus, an intermediate feedback-
loop bandwidth of = 1 KHz applied to stabilize A in a future
setup could well eliminate the frequency-scaling fluctuations;
this will enable averaging over many consecutive
inteferagrams to improve S,", as is accepted practice with
common FTIR.
Infrared filters of low-pass, bandpass and high-pass type were
placed in the beam path before the detector to monitor changes
induced in the radio spectra, and compare them with known
filter functions. From these observations the characteristic
minimum occurs at about 1000 mi', an assignment also
compatible with the known sensitivity function of the detector
which rises from 10% at 720 cm-' to 90% at 800 cm-'. The
frequency scale can in principle be precisely calibrated by gas-
phase molecular absorption lines. Our experiment verifies our
novel concept of using precision lasers to transpose broad
opticallinfrared spectra into the electronic realm. The
demonstrated mid-infrared spectrum spans nearly an octave,
from 750 to 1300 cm-'. It could be extended beyond 2000 cm-'
up to the near-visible using thinner crystals: and certainly
down to the far-infrared, THz and microwave regions using
suitable crystals, antennas, combiners, power detectors, and
sampling methods. Better alignment and summing
interferograms will boost the signal and allow recording much
longer interferograms far increased spectral resolution.
Outlook
Reaching far beyond conventional FTIR, coherent-frequency-
comb FTlR promises microsecond acquisition to study fast,
single event dynamics, e.g. in polymers and biopolymers. Its
88 2004 Joint 29' Int. Conf. an Infrared and Millimeter Waves and 12'" Inl. Coni. an Terahertz Electronics
Spectroscopy and Material Properties
laser-like beam allows long-distance probing for remote
environmental analysis, as well as dimaction-limited focusing
for microscopy. Alternative sample configurations are feasible,
for instance, tatal-intemal-reflection for high-sensitivity
biomolecular screening, or photoconduction for semiconductor
and superconductor research. The unused second output beam
from the combiner (Fig. I) can contribute online reference
interferograms. Finally, the sample can be placed before the
combiner to realize complex-valued FTIR-simultaneous
amplitude and phase infrared spectra--thus enabling complex-
optical constant determination in reflection without recourse to
ellipsometry, and also complex-valued scattering-type near-
field microscopy" far nanometer-resolution chemical analysis
of nanocomposites.
The method of time-domain coherent infrared spectroscopy can
also be used for narrowband spectroscopic and metrologic
applications. In these the procedure of recording an
interferogram with subsequent Fourier-transformation would
be replaced by other means of electronic processing. For
example, lock-in amplification of the detector signal could
enable the continuous monitoring of amplitude and phase of a
infrared frequency nf,.
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