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Optical limiting properties of a nonlinear multilayer Fabry–Perot resonator

containing niobium pentoxide as nonlinear medium

Article  in  Optics Letters · August 2014

DOI: 10.1364/OL.39.004847

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 August 15, 2014 / Vol. 39, No. 16 / OPTICS LETTERS 4847

Optical limiting properties of a nonlinear multilayer

Fabry–Perot resonator containing
niobium pentoxide as nonlinear medium
Anton A. Ryzhov,1,2,* Inna M. Belousova,1,2 Yanzhi Wang,3 Hongji Qi,3 and Jun Wang3
1
Institute for Laser Physics, S. I. Vavilov State Optical Insitute, Saint Petersburg 199034, Russia
2
Laser Optics Department, University ITMO, Saint Petersburg 197101, Russia
3
Key Laboratory of Materials for High Power Laser, Institute of Optics and Fine Mechanics, Shanghai 201800, China
*Corresponding author: [email protected]
Received May 20, 2014; revised July 15, 2014; accepted July 15, 2014;
posted July 15, 2014 (Doc. ID 212404); published August 13, 2014
The optical limiting effect was numerically simulated and experimentally observed for a 25-layer thin-film Fabry–
Perot microresonator by 7 ns laser pulses at 532 nm. The sample, made by vacuum evaporation and consisting of
alternating Nb2 O5 and SiO2 layers, has an ultranarrow line of transparency at near 532 nm within a wide spectral
band of reflection. By adjusting simulated results in accordance with experimental dependencies of transmittance,
reflectance, and absorbance on incident light intensity, the coefficient of optical nonlinearity of Nb2 O5 was
estimated at
6  1i · 10−12 cm2 ∕W. © 2014 Optical Society of America
OCIS codes: (230.1150) All-optical devices; (230.4170) Multilayers; (250.6715) Switching; (310.6845) Thin film devices
and applications.
http://dx.doi.org/10.1364/OL.39.004847

In a nonlinear Fabry–Perot resonator indices of reflec- We study the potential of multilayer Fabry–Perot
tion and absorption of a medium put between the mirrors resonators in the capacity of quick-response one-
depend on light intensity. Such resonators have been well wavelength optical limiters. Such limiters can be useful
studied since the second half of the 1970s. Theoretically in a variety of laser systems; for example, in a laser range-
predicted effects of optical bistability, differential gain, finder to protect the detector from intensive reflected
and limiting have been experimentally observed for res- (backscattered) radiation. Currently, there is a lack of ex-
onators containing Na vapor [1], nonlinear liquids (liquid perimental works realizing the suggested approach,
crystals, nitrobenzene, CS2 ) [2], solid plates of GaAs [3], whereas interest in optical power limiting is very active.
and InSb [4]. A detailed review of these works have been Husaini et al. [14] have experimentally observed for a
presented in [5]. nonresonant multilayer structure a decrease in the limit-
However, those resonators were laboratory devices ing threshold. The decrease results from an interference
consisting of separate mirrors and a nonlinear medium several-fold increase of optical-field intensity inside the
between them. Multilayer thin-film structures seem to layers with metal nanoparticles. In this case, sharp spec-
be more applicable for creation of low-threshold nonlin- tral characteristics of the structure do not contribute to
ear optical devices because of their small thickness the nonlinear T characteristic, since the operating wave-
(comparable with a light wavelength) and wholeness. length is much above the upper bandgap edge, whereas
Linear multilayer coatings have been well studied and application of a Fabry–Perot resonator enables it to in-
widely used in optical systems for years. A variety of crease field intensity within its middle layer by several
works have dealt with nonlinear properties of both single orders of magnitude.
and multilayer films [6–13]; however, multilayer optical In this Letter, we present the results of an experimental
and numerical study of nonlinear characteristics of a
coatings are still not in use as nonlinear devices.
multilayer resonator at 532 nm. The resonator is made
In general, application of a Fabry–Perot resonator for
creation of a low-threshold nonlinear optical device is as an optical coating composed of 25 alternating layers
promising for two reasons. Firstly, the resonator is a nar- of Nb2 O5 and SiO2 [Fig. 1]. The middle Nb2 O5 layer is
rowband optical filter, for which spectral position of the the thickest and forms the resonator cavity. The formula
line of transparency depends on the optical distance be- of the structure is
tween the mirrors not on the medium resonant proper-
ties. With it a small change in the refractive index of a
HL6 H 2
LH6 ; (1)
medium contained between the mirrors results in a sig-
nificant spectral shift of the line. A small change in the where H and L indicate layers with high and low refrac-
absorption index results in a significant transmittance tive indices, respectively. Both are of λ0 ∕4 optical thick-
(T) change at the peak of the line (however, in this case ness, with λ0  532 nm being the nominal resonant
a decrease in T results more from an increase in reflec- wavelength. The substrate is a 30 mm diameter, 3 mm
tance (R) than from an increase in absorbance (A) of the thickness-fused silica plate. The root-mean-squared
whole structure). Secondly, light intensity at the resonant roughness of the substrate, measured by an optical pro-
wavelength increases many-fold in the space between the filer, is about 0.5 nm.
mirrors by interference, which leads to a corresponding A set of the thin-film resonators was fabricated at the
decrease in the nonlinear threshold. Shanghai Institute of Optics and Fine Mechanics CAS by
0146-9592/14/164847-04$15.00/0 © 2014 Optical Society of America
4848 OPTICS LETTERS / Vol. 39, No. 16 / August 15, 2014

Nb2O5
SiO2
Six pairs of
λ/4 layers

Nb2O5 Middle λ/2 layer

Fig. 3. Transmittance dependence on the angle of incidence at

Six pairs of low-level radiation at 532 nm.
SiO2 λ/4 layers
Nb2O5
beam and attribute this mismatch to lack of collinear
SiO2 substrate beam configuration in the spectrophotometer.
In the absence of absorption, T max of an ideal multi-
Fig. 1. Structure of the studied multilayer resonator. layer resonator is equal to T of the interface between
air and the substrate, i.e., 0.96 at the substrate refractive
ion-assisted ion-beam sputtering. The coating rate was index ns  1.5. In principle, a decrease in T max can be
0.2 nm∕s. The refractive indices of deposited Nb2 O5 caused by two factors: some extinction in the layers
and SiO2 layers at 532 nm are 2.31 and 1.48, respectively. and a difference between reflectances of the mirrors sur-
These values were determined from the T and R spectra rounding the middle layer. In the latter case, only an in-
of corresponding single layers. crease in reflectance of the whole structure will occur.
In Fig. 2 the solid line represents the T spectrum of one By the experimental setup [Fig. 4] we determined 75%
of the samples in a small vicinity of the transparency line, T and 15% R at the peak, which indicates a presence
measured by a spectrophotometer at normal incidence. of both factors.
The figure shows that the real peak of T takes place According to the literary data [15,16], Nb2 O5 films have
at 532.4 nm, which slightly exceeds the nominal a significant index of absorption in the visible region. Cal-
λ0  532 nm. It does not create a barrier for experimen- culating the T and R spectral characteristics, we selected
tal study at 532 nm because it is possible to shift the the imaginary part of the refractive index to model ab-
resonant wavelength a little lower by giving a tilt to sorption. The refractive index of Nb2 O5 was finally set
the resonator. The reason is that the optical length differ- as nH  2.31  2 · 10−4 i, which at 532 nm is equivalent
ence in the middle layer is proportional to the cosine of to the extinction coefficient α  4.8 mm−1 . At the same
the angle of refraction. time, to model a difference between R of the mirrors
Figure 3 represents both the experimental and calcu- and the shift of the peak spectral position (from nominal
lated dependencies of T on the angle of incidence at low- 532 nm to real 532.4 nm), some deviations (under 15%) of
level 532 nm laser radiation. The measurement was taken layer thicknesses from the nominal values were intro-
by using a pulsed Nd:YAG laser at s-polarization. The duced. Finally, calculation parameters of the resonator
maximum of T (T max ) occurs at 4° deviation from the were set in such a way that at low intensities the calcu-
normal incidence position. According to our calculations, lated results correspond to the experimental ones as far
taking into account an inaccuracy of the middle-layer as possible [Figs. 2 and 3].
thickness, at normal incidence to such a resonator the Figure 5 represents both the experimental and calcu-
T max is to be at 532.4 nm, which corresponds to Fig. 2. lated nonlinear dependences of T, R, and A at three dif-
Figure 3 also shows that T max for the laser beam is ferent angles of incidence. A pulsed single-mode Nd:YAG
about 75%. The spectrophotometric measurement has laser was used as a light source (up to 6 mJ pulse energy,
a lower value. We rely on the value given by the laser 7…10 ns pulse length, and 2 mm beam diameter at 0.86
energy level). The incident pulse energy was regulated by
attenuator F1 [Fig. 4].

D2
D3 F2
wedge flat
mirror
Nd:YAG
532 nm
F1 sample
D1
Fig. 4. Experimental setup for synchronous measurements of
Fig. 2. Transmittance spectrum of the sample in the vicinity of T and R nonlinear dependencies. D1, D2, D3—pulse energy
the transparency line at low-level radiation. detectors; F1, F2—calibrated sets of filters.
 August 15, 2014 / Vol. 39, No. 16 / OPTICS LETTERS 4849

with the experimental results in the best way. The non-

linear coefficient was assumed to be n2 
6  1i ·
10−12 cm2 ∕W. Such a high n2 is an interesting result by
itself. The nonzero imaginary part defines nonlinear ab-
sorption. Fitting n2 , we gave preference to a correspon-
dence of 4° characteristics, which were finally well
enough. By that we can also see a good correspondence
of 2° characteristics, but at 5° the experimental points
noticeably deviate from the calculated curve.
According to the calculations, at 5°, as E increases,
T increases, too, but then decreases. R behaves oppo-
sitely, which is easy to understand: Initially the optical
thickness of the middle layer is a bit less than λ0 ∕2,
and the real part of n increases with increasing E,
which means the optical thickness approaches λ0 ∕2
from below for a while, then moves away. At the same
time, the imaginary part of n also increases, partly
leveling the increase in T at the first part. At the n2 value
given above, the calculated T characteristic shows the
increase from 45% to 55%, but we did not observe such
an increase in the experiment. It could be explained by
stronger absorption, but using a larger value of the imagi-
nary part of n in the calculations leads to significant
divergences at 2° and 4°. This fact will be investigated
further.
The maximal pulse energy used in the experiment was
about 2 mJ. Such pulses did not cause any irreversible
change of the sample. At larger energy values damages
of the sample were observed.
In conclusion, the presented results obviously demon-
strate the optical limiting effect, accompanied with the
Fig. 5. Calculated and experimental nonlinear characteristics increase in reflectance, which results from the spectral
of transmittance (upper plot, black lines), absorbance (upper shift of the transparency line. Although the value of n2
plot, gray lines), and reflectance (lower plot) at three different for an Nb2 O5 thin film is not proved by another experi-
angles of incidence. ment, the good correspondence between the experimen-
tal and calculated nonlinear characteristics indicates that
the calculation model is adequate. As opposed to “thick”
The light propagation time through the structure is Fabry–Perot resonators, in which the distance between
several orders less than the pulse duration. The Nb2 O5 the mirrors is several orders longer than an optical wave-
nonlinear response time was also supposed to be much length, in thin-film resonators that distance is of the
less, so that the nonlinear dependences of T, R, and A same order as the wavelength. As a result, a thin-film res-
were initially calculated as functions of instantaneous onator gives a relatively wide transparency line, which is
incident light intensity. To compare these calculated usually the sole one within the bandgap of the mirrors.
characteristics with experimental results, the former At the same time, transparency-line narrowing leads to
were reduced to the dependencies on pulse energy by a decrease in the nonlinear threshold. At a given resona-
area and time integration (taking spatial and time pulse tor interval, the higher the R of the mirrors, the narrower
distributions). the transparency line. R of the mirrors can be raised
In the calculations, SiO2 was assumed to be a linear by increasing the number of layers. Although optical
material and Nb2 O5 a third-order nonlinear material: coatings have been widely used for a long time, making
a high-quality filter with a transparency line under 1 nm
n  n0  n2 I; (2) of width still presents technological difficulties, mainly
based on inadequate precision of film-thickness
where n0 is the linear part of the Nb2 O5 refractive index,
controlling.
I is the light intensity (W∕cm2 ), and n2 is the nonlinear
coefficient (cm2 ∕W). In [17] we described our field- This work was supported by the Russian Foundation
distribution computing method, which takes into account for Basic Research (No. 14-02-00851), the Government
the dependence of n on I. Although for the current work of Russian Federation (No. 074-U01), the National Natu-
we developed the method significantly, having switched ral Science Foundation of China (No. 61178007), and
over to a “right-to-left” computation (i.e., to a calculation Science and Technology Commission of Shanghai
of output–input characteristics instead of input–output), Municipality (Nano Project No. 11nm0502400, Shanghai
for the sake of brevity we do not describe that here. Pujiang Program 12PJ1409400). J. W. thanks the financial
By analogy with the imaginary part of n0 , n2 was fitted supports from the National 10000-Talent Program, CAS
so that the calculated characteristics are in accordance 100-Talent Program.
4850 OPTICS LETTERS / Vol. 39, No. 16 / August 15, 2014

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