4640 OPTICS LETTERS / Vol. 38, No.

22 / November 15, 2013

Concept for three-dimensional optical addressing by

ultralow one-photon absorption method
Qinggele Li, Mai Trang Do, Isabelle Ledoux-Rak, and Ngoc Diep Lai*
Laboratoire de Photonique Quantique et Moléculaire, UMR CNRS 8537, Institut D’Alembert, Ecole
Normale Supérieure de Cachan, 61 avenue du Président Wilson, 94235 Cachan cedex, France
*Corresponding author: nlai@lpqm.ens‑cachan.fr
Received August 5, 2013; revised October 4, 2013; accepted October 8, 2013;
posted October 9, 2013 (Doc. ID 195223); published November 7, 2013
With respect to experimental condition, we have investigated the point spread function of a high numerical aperture
objective lens, taking into account the absorption effect of the studied material. By using a material possessing an
ultralow one-photon absorption (LOPA) coefficient at the excitation wavelength, the light beam can penetrate
deeply inside the material and be tightly focused into a subwavelength spot, almost the same as in the absence
of material. Combining tight focusing and ultralow absorption conditions, we show that LOPA-based microscopy
is thus capable of three-dimensional imaging and fabrication with long penetration depth up to 300 μm. As com-
pared to the commonly used two-photon absorption microscope, the LOPA method allows simplification of the
experimental setup and also minimization of the photodamaging or bleaching effect of materials. © 2013 Optical
Society of America
OCIS codes: (110.0180) Microscopy; (010.1030) Absorption; (170.6900) Three-dimensional microscopy.
http://dx.doi.org/10.1364/OL.38.004640

Far-field optical microscopy plays an important role in
various research domains, in particular for bio-imaging
[1] and micro- and nanofabrication [2,3]. The principle
of this microscopy is based on tightly focusing a light
beam into a micrometer or submicrometer spot in order
to locally excite the material under investigation. How-
ever, two critical limitations may affect the optical
microscope capability. The first one is the well-known
diffraction limit [4], which limits the microscope resolu-
tion at about half of the excitation wavelength due to dif-
fraction. The other one is the limit of penetration depth
inside the material, which is normally related to strong
absorption or scattering [5] phenomena in the material
under study, thus limiting the optical addressing of thick
materials. In recent years, many articles have reported on
different methods to reach a spatial resolution beyond
the diffraction limit. For example, the invention of stimu-
lated emission depletion microscopy [6] and of absorp-
tion modulation optical lithography [7] allowed greatly
enhancing the resolution of optical microscopes for both
imaging and fabrication. Concerning the penetration
depth, we distinguish two different excitation methods,
namely one-photon and two-photon absorption (OPA
and TPA). In the first case, due to linear absorption, the
light intensity decreases exponentially along the propa-
gation direction inside the material. If the material
presents a high absorption at the excitation wavelength,
light vanishes before reaching the focusing spot. The
OPA-based microscope therefore allows us only to deal
with thin materials or with one- and two-dimensional (1D
and 2D) thin structures. The great advantage of the OPA
method is that it requires only a simple optical setup with
a low-cost laser source operating in a continuous regime.
Note that for a particular situation in which the material
does not present a homogeneous absorption, as shown in
Fig. 1(a), this medium is equivalent to a thin absorbing
material. The OPA-based confocal optical system [8] is
then able to excite and to selectively collect the light
emitting from the focusing region only, thus allowing
to obtain a three-dimensional (3D) image. However, in
0146-9592/13/224640-04$15.00/0
the general case, this technique does not allow realiza-
tion of 3D imaging and fabrication of a thick and contin-
uously absorbing material. In order to deal with thick and
absorbing materials, the TPA or multiphoton excitation
method [9,10] has been proposed. In this case, the sample
is selectively and efficiently excited at the focal spot of a
microscope objective only, owing to the quadratic
dependence of the material response with respect to
the excitation intensity. By manipulating the focusing
spot, complex 3D imaging or fabrication can be realized
[2,3,9–11]. However, in order to make use of this TPA
process, two conditions are required, namely a pulsed
femtosecond or nanosecond laser providing a high peak
intensity on one hand and a tightly focused laser beam on
the other hand. The requirement of a femtosecond laser
source makes this method more complicated and more
expensive than the OPA technique and may also induce
photodamage or photobleaching of the studied material.
In this Letter, we investigate the influence of absorp-
tion in a material on the propagation properties of a
light beam tightly focused inside this medium. According
to correlation conditions of the absorption coefficient
and tight focusing, and via a rigorous theoretical
Fig. 1. Light focusing in different media. (a) OPA (blue spots)
in a medium with inhomogeneous absorption, which is equiv-
alent to a thin absorbing medium. The black lines are 1D
absorbing domains. (b) Illustration of light focusing in a
medium in the case of LOPA (green spots) and TPA (red spots).
© 2013 Optical Society of America

calculation of intensity distribution, we propose a novel
concept for 3D imaging and fabrication, which displays
the advantages of both OPA and TPA. Namely, it uses
a simple experimental setup, similar to the conventional
OPA method, and it allows optically addressing 3D struc-
tures as in the case of the TPA method.
The mathematical representation of the electromag-
netic field distribution in the focal region of an objective
lens (OL) has been proposed by Wolf in the 1950s [12].
Thereafter, this representation has evolved to different
forms in order to adapt itself to different experimental
conditions, such as focusing a light beam in refractive in-
dex mismatched media [13], focusing of differently
polarized incident beams [14] or of different beam modes
[15], focusing of a light beam through a mask [16], and so
forth. This theory based on the vector Debye approxima-
tion thus allows calculating and predicting the intensity
distribution as well as the polarization distribution of a
light beam focused inside a material by a high numerical
aperture (NA) OL.
To the best of our knowledge, the influence of material
absorption on the intensity distribution and the focused
beam shape of a propagating optical wave has not been
systematically investigated yet. In this work, we have em-
ployed the mathematical representation proposed by
Wolf [12], taking into account the absorption effect of
the material when a focused light beam propagates
through it, especially in the focal region.
The schematic representation of light focusing in an
absorption medium is shown in Fig. 2. D is the interface
between the transparent material, such as a glass sub-
strate or air, and the absorbing material. For simplicity,
it is assumed that there is no refractive index mismatch
problem arising at any interface, which may exist between
the exit pupil of the OL and the focal plane. The distance
between the D interface and the focal plane is represented
by d. The electromagnetic field near the focal plane is
given in Cartesian coordinates
x; y; z [17] by
ZZ
E−
ikC
T
sA
seik
sx xsy ysz z dsx dsy ;
2π Ω
where C is a constant, k is the wavenumber (k  2πn∕λ), n
is the refractive index of the absorbing medium, λ is the
D
d
Obj.
r z2
O
Fig. 2. Schematic representation of a tightly focused light
beam inside an absorbing medium. σ is the absorption coeffi-
cient of the medium. D is the interface between the transparent
and absorbing media. d is the distance from the D plane to the
focal plane of the OL. r is the distance from an arbitrary point
on the D surface to an observation point located in the focusing
region.
November 15, 2013 / Vol. 38, No. 22 / OPTICS LETTERS 4641
excitation wavelength, Ω is a solid angle corresponding
to the objective aperture, S 
sx ; sy ; sz  is the vector of
an arbitrary optical ray, and T
s  P
sB
s is a transmis-
sion function where P
s is the polarization distribution
and B
s is the amplitude distribution at the exit pupil.
A
s represents the absorption effect of the material,
which is expressed as A
s  exp
−σr, where σ is the ab-
sorption coefficient and r indicates the optical path of
each diffracted light ray in the absorbing medium, which
is defined as the distance from an arbitrary point located
in the D interface to the corresponding observation point,
as shown in Fig. 2. For numerical calculations, r is
determined in Cartesian coordinates by
q

































































r 
x0 − x2 
y0 − y2 
d − z2 ; (2)
where (x0 , y0 , d) gives the position of an arbitrary dif-
fracted light ray located on the D interface.
Essentially, Eq. (1) gives the light distribution resulting
from the interference of all light rays diffracted by the
exit pupil of the OL. However, in practice, light is ab-
sorbed by the material in which it propagates, and its
amplitude decreases along the propagation direction.
Consequently, the light intensity and the focus shape
at the focus region depend strongly on the absorption
term A
s.
The relevant intensity distribution of light in the focal
region is defined as
I OPA  EE : (3)
First, we consider a circularly polarized uniformly
shaped monochromatic light beam (532 nm), which is fo-
cused into an absorbing medium by an OL with NA  1.3
(oil immersion, n  1.515). The numerical calculation
results of light intensity distribution from the absorption
interface D to focal region are shown in Figs. 3(a)
through 3(d). We assumed d  10 μm. Absorption
coefficients are chosen as 105462, 70000, 40000, and
(1) 800
cm−1 , respectively. As expected, the numerical
Fig. 3. Numerical calculation of absorption effects on light
propagation and intensity distribution in the focal region of a
high NA OL (NA  1.3, n  1.515). (a) through (d) Intensity dis-
tributions obtained with different absorption coefficients (σ):
105462, 70000, 40000, 800 cm−1 , respectively. (e) Normalized in-
tensity (I f ∕I 0 ) at the focal plane (O) as a function of the absorp-
tion coefficient. I f and I 0 are the intensities obtained with
(σ ≠ 0) and without (σ  0) absorption medium, respectively.
4642 OPTICS LETTERS / Vol. 38, No. 22 / November 15, 2013
results show that when increasing the absorption
coefficient of the material, light intensity attenuates dra-
matically along the optical axis. With a very low absorp-
tion coefficient, σ  800 cm−1 [Fig. 3(d)], the absorption
is almost negligible and light can be tightly focused into a
focal spot without any evident deformation. However, if
absorption increases, the light intensity decreases when
penetrating inside the material. Even if the light beam can
propagate to the focusing spot, its total intensity at that
region is quite weak as compared with its intensity at the
D interface [Figs. 3(c) and 3(b)]. If the absorption coef-
ficient is very high (e.g., σ  105462 cm−1 for Rhodamine
6G (Rh6G) laser dye measured at λ  532 nm), light is
completely absorbed at the D interface and vanishes in
the focusing region [Fig. 3(a)].
Considering d  25 μm, Fig. 3(e) represents the
dependence of the maximum intensity at the focusing
spot (I f ) with respect to the absorption coefficient (σ).
This intensity is normalized to that obtained in the case
of a transparent medium (I 0 ). Clearly, light intensity
becomes very weak if absorption is important, even with
a tight focusing. The intensity reduces by a factor of
two for an absorption coefficient of 13200 cm−1 (for
d  25 μm).
It is worth noticing that, in practice, the laser wave-
length is often chosen within a high absorption domain
of the studied material in order to enhance light–matter
interaction. It is therefore difficult to work with thick
materials or with 3D structures. According to the results
shown in Figs. 3(a) and 3(b), the conventional OPA
method allows us only to study objects with a thickness
of about 1 μm. For this reason, no 3D imaging or fabri-
cation has been realized using an OPA-based microscope
until now.
However, as shown in Fig. 3(d), if the absorption
coefficient is very low, light can penetrate deeply inside
an absorbing material without significant attenuation.
This behavior is similar to that obtained by focusing light
in a transparent medium. Note that with an ultralow
one-photon absorption effect (LOPA), it may be difficult
to realize a photoinduced physical or chemical change of
material. However, by using a high NA OL, the intensity at
the focusing spot can reach a very high level, one billion
times higher than at other regions located far away from
the focal spot. This intensity at the focal spot is high
enough to compensate the LOPA effect and to fulfill
the required excitation energy.
The LOPA-based microscopy thus allows realization of
3D imaging and 3D fabrication similar to what could be
realized by TPA microscopy. Indeed, by using the LOPA
technique, fluorescence (for imaging) or photopolymeri-
zation (for fabrication) effects can be achieved efficiently
within the focal spot volume only. By moving the focusing
spot inside the material, as shown in Fig. 1(b), we can
realize 3D fluorescence imaging or fabrication of 3D struc-
tures. Figure 4(a) shows the intensity distribution of light
focused at different depths inside the material: d1  5 μm,
d2  22.5 μm, and d3  40 μm. The intensity is very high
at the submicrometer focusing spot, and the focusing
shape remains almost the same at different positions.
Of course, absorption exists, even if the probability is
very small. The penetration depth is therefore limited to a
certain level. This effect exists also in the case of TPA,
Fig. 4. (a) Focusing the light into an ultralow absorption
medium at different d values: d1  5 μm, d2  22.5 μm, and
d3  40 μm. (b) Red curve: normalization of intensity (I f ∕I 0 )
at the focusing spot as a function of d. I f and I 0 are the inten-
sities obtained with and without absorption medium, respec-
tively. Dot curves: zoom on intensity profiles of the focusing
spot along the optical axis, calculated at different d values.
The results are simulated with σ  800 m−1 , λ  532 nm,
NA  1.4 (n  1.515).
but it is more important for LOPA. Figure 4(b) represents
the maximum intensity at the focusing spot as a function
of the penetration length, d. For this calculation, we as-
sumed an ultralow absorption coefficient, σ  800 m−1 ,
corresponding to the absorption of a negative photoresist
SU8 at λ  532 nm [18]. We found that for a distance of
330 μm, the intensity decreases by a factor of two with
respect to that obtained at the input of absorbing material
(D interface). For many applications, this penetration
depth of several hundreds micrometers is fully compat-
ible with the working distance of the microscope OL
(about 200 μm for a conventional high NA OL) or with
the scanning range of the piezoelectric stage (typically,
100 μm for a high resolution).
The first application of the LOPA-based microscope
has recently been validated [18] and allows fabrication
of submicrometer 2D and 3D polymer-based photonics
structures. For this purpose, a commercial SU8 photore-
sist has been structured by using a continuous low-power
laser emitting at 532 nm, a wavelength corresponding to a
very low absorption value of the photoresist. The LOPA
microscopy therefore presents a great advantage as com-
pared with the TPA method because it is very simple and
cheap with similar results. We note that the access rate of
both LOPA and TPA mainly depends on the movement
capacity of the piezo translation stage. The high access
rate may be achieved by using, for example, scanning
mirror techniques.
Finally, we note that other weak effects exist, such as
scattering, which also induces photon losses during the
light propagation inside a medium. However, these ef-
fects are negligible as compared with the absorption
of materials. The scattering effect, for example, is mainly
considered in turbid media by using a Monte Carlo sim-
ulation method [19] neglecting absorption.
In conclusion, we have systematically studied the
influence of material absorption on light propagation
properties and in particular on the intensity distribution
 November 15, 2013 / Vol. 38, No. 22 / OPTICS LETTERS
at the focus region of a high NA OL. If the material dis-
plays a high absorption, the excitation light is almost fully
absorbed at the region close to the absorption interface.
For a moderate absorption, light can propagate deeper
inside the material and reaches the focusing region. How-
ever, the penetration depth is still very limited, the light
intensity is weak, and the focusing spot shape is also de-
formed. By using a material with an ultralow absorption
coefficient at the excitation wavelength, light can be fo-
cused deeply inside the material, up to several hundreds
of micrometers, with a very high intensity. A new concept
of 3D optical addressing based on ultralow linear absorp-
tion (LOPA) is then proposed, by tightly focusing an op-
tical beam inside a thick material displaying a very low
absorption at the operating wavelength. As compared
with the TPA method, this LOPA-based microscopy is
very simple and inexpensive, achieving similar results,
such as 3D imaging and 3D fabrication, as well as 3D data
storage. It also can minimize photodamaging or bleach-
ing of optical materials.
This work has been supported by the Laboratoire
d’Excellence NanoSaclay, in the framework of the pro-
ject ONE-FAB-3D, and by the Triangle de la Physique,
in the framework of the project PUTTON. Q. Li acknowl-
edges the fellowship from the China Scholarship Council,
and M. T. Do acknowledges the fellowship from the Viet-
nam International Education Development 322 program.
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