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nonlinear-optical crystals
Ilya A. Kulagin*, Rashid A. Ganeev, Valery A. Kim, Alexander I. Ryasnyansky,
Renat I. Tugushev, Timurbek Usmanov, Alexander V. Zinoviev
NPO Akadempribor of Academy of Sciences, Akademgorodok, Tashkent 700125, Uzbekistan
ABSTRACT
The measurements of nonlinear refractive indices and third-order susceptibilities responsible for self-action effects in
nonlinear-optical crystals (KDP, KTP, BBO, LiNbO3) in various spectral ranges (1064 and 532 nm) were carried out
by the Z-scan method. It was obtained that investigated media (excepting KTP crystal at =1064 nm) had self-
focusing properties. The significant values of nonlinear losses were recorded at =532 nm. The analysis and
comparison of experimentally and theoretically obtained values of nonlinear susceptibilities are given. The angular
and polarization dependencies of Kerr nonlinearities were analyzed.
1. INTRODUCTION
Investigations of nonlinear refraction and nonlinear absorption in nonlinear-optical crystals used for effective
frequency conversion are of particular interest nowadays due to investigations of various second-order nonlinear-
optical processes (second harmonic generation, parametric waves generation and amplification, wave mixing, electro-
optical effect, etc.) in femtosecond scale range. The development of femtosecond pulse amplification technique
stimulated the growth of laser radiation intensity and led to the necessity of high-order nonlinear-optical processes
influence on second-order ones to be taken into account1,2. Such high-order nonlinear processes can be caused by self-
action of laser radiation, i.e. the processes connected with refractive index change and light absorption in a strong
electromagnetic field. For the analysis of spatial, spectral and temporal parameters variations of a high-power laser
radiation it is necessary to know the nonlinear-optical characteristics responsible for self-action processes, such as self-
focusing, self-induced phase modulation in nonlinear medium etc. There are no detailed investigations of high-order
nonlinearities of quadratic nonlinear crystals. The third-order nonlinear susceptibilities were measured only for the
some spectral ranges and only for some crystal orientations3-5.
In this work we present the measurements and analysis of the third -order nonlinear susceptibilities, nonlinear
refraction indices and nonlinear absorption coefficients of KDP, LiNbO3, BBO, and KTP crystals at the wavelengths
of 1064 nm and 532 nm using the Z-scan method. The analysis of obtained experimental dependencies of a
normalized transmission as a function of sample position in closed aperture Z-scan scheme was carried out by the
different methods (method of Gaussian decomposition, paraxial approximation, numerical method). The comparison
of measured nonlinear susceptibilities with calculated ones on the basis of developed empirical model was carried out.
The angular and polarization dependencies of Kerr nonlinearities were analyzed.
There exist the different determinations of nonlinear susceptibilities nowadays that can be distinguished by constant
coefficients and connected with the different field determination. In this work the same determination of the field and
nonlinearity as in the reference6 was used (E=[Eexp(-it+ikz)+c.c.]/2 and Pn=(3/4)(3)(; ,-,):E3). In order to
describe the refractive index change of a medium with cubic nonlinearity (3)(;,-,)= k(3) two nonlinear
coefficients (n 2 and ) are used that are connected with the refractive index variations via field amplitude and
intensity:
*
kulagin@mail.tps.uz; phone +998 71 1621345; fax +998 71 1690124
182 Nonlinear Frequency Generation and Conversion: Materials, Devices, and Applications II,
Kenneth L. Schepler, Dennis D. Lowenthal, Jeffrey W. Pierce, Editors, Proceedings
of SPIE Vol. 4972 (2003) 2003 SPIE 0277-786X/03/$15.00
Conventional empirical model based on the assumption of single dominant effective transition was used for estimation
of Kerr nonlinearity values. Frequency transition and matrix elements of dipole moment operator (0-1 0) were
determined on the basis of refractive index value and its dispersion. Refractive index value and its dispersion were
taken at the same frequency in opposite to earlier developed approximations 3,7. In the assumption about single
dominant optical transition, the refractive index can be determined as follows
2 f ( 0 , 0 , ) 02
n02 = 1 + N, (2)
ch 01 1
where f(0,0,) is the parameter taking into account the local field amendment, N is the oscillators density. By
n02
determining unknown values from (2) and , one can obtain the following expression for third-order nonlinear
susceptibility
(
2 n 0
)
2
1
k(3) = n 2
0 1 . (3)
32 3 chN
Eq. (3) allows to determine the Table 1. Calculated values of nonlinear-optical parameters of crystals
Kerr nonlinearity dispersion
using refractive index Wavelength =1064 nm
Wavelength =532 nm
dispersion. Calculated values Works of other
This work This work
of nonlinear susceptibilities for authors
k(3),
some nonlinear crystals at two Crystal k(3), n2, , n2, n2, -14 n2, ,
10
wavelengths (1064 nm and 10-14 10-13 10-20 10-13 10-16 10-13 10-20
esu
532 nm) are presented in esu esu m2 W-1 esu cm2 W-`1 esu m2 W-1
Table 1. The refractive index 1.353
dispersion was determined on KDP (o) 3.50 2.20 6.15 1.92 1.18 3.22
2.84*
the basis of Sellmeier 3
0.85 0.81
KDP (e) 1.18 0.763 2.18 1.28 2.32
equations8. It is seen from the 1.64* 6
table that for all crystals the BBO (o) 3.89 2.22 5.61 4.62 2.60 6.49
radiation wavelength decrease BBO (e) 1.41 0.860 2.34 4.15** 2.40 1.45 3.92
leads to the nonlinearity values LiNbO3 (o) 26.2 11.5 20.7 59.4 24.1 43.4
increase, i.e. their dispersion is LiNbO 3 (e) 19.4 8.49 16.5 42.6 18.0 33.7
positive except -component of KTP(=0,x) 7.46 4.02 9.70 4* 16.1 8.51 20.0
49
KDP crystal. Decreasing of KTP (=0,y) 8.24 4.45 10.7 18.1 9.56 22.4
284* 515**
k with wavelength
(3) KTP(=90,x) 8.26 4.48 10.8 10 3* 18.2 9.62 22.7
decreasing in the region far KTP (=90,y) 13.7 7.38 17.7 31.5 16.6 38.8
*
crystal orientation is undefined; ** - =850 nm, =29.2
from resonance is not usual
case. In this model this k(3) decreasing is due to frequency change of effective transition.
k(3) =
1
[3( 1111 + 1122 ) + (1111 1122 )cos 4 ]cos 4 + 3 2233 sin 2 2 + 3333 sin 4 , (4)
4 2
and the Kerr nonlinearity of the crystal with 3m symmetry can be presented as
( )
k(3) = 31122 cos 4 + 4 1123 1 4 cos 2 sin sin cos 3 +
3
2
2233 sin 2 2 + 3333 sin 4 . (5)
Taking into account the Kerr nonlinearity dispersion increases the number of independent components up to 5
( 42m symmetry) and 6 (3m symmetry).
Measurements of crystal nonlinearities were based on the Z-scan method. This simple method allows to measure
various nonlinear-optical parameters with high sensitivity 4,9. For the experimental results interpretation of radiation
normalized transmission trough the aperture with respect to the sample position, the Gaussian decomposition
method9 was used. Also the paraxial approximation 10,11 and numerical calculations were used. To agree the results
obtained in the paraxial approximation and in numerical calculations the fitting factors were used. In the paraxial
approximation the factors of 21/2 and 3-1 x 2-1/2 were defined for diffraction length and radiation intensity respectively.
The Z-scan method based on non-homogeneous phase shift in the different beam regions with different radiation
intensity was used. The phase shift in nonlinear media along with self-action effect (we call it as the "self-action
channel") can be due to different parametric processes. In anisotropic media possessing a high value of second order
susceptibility responsible for second harmonic generation, the competing channel of induced phase shift is the
processes of direct and reverse frequency conversion 12 (the processes of the second and sub-harmonic generation). We
call this channel as the cascade channel.
The efficiency of second harmonic generation and phase change of the fundamental radiation are determined by the
phase mismatch k = 2k 1-k2 (k1,2 are the wave numbers of fundamental and harmonic radiation). There exists the
critical value of phase mismatch at which both channels of phase distribution (second harmonic and sub-harmonic
generation and self-action processes) contribute to the same phase change. At a small energy exchange approximation
2
cn03 k
(fundamental radiation intensity I < , here (2) is the second-order nonlinear susceptibility) and high
210 5 ( 2)
values of phase mismatch (k>L-1, L is the medium length), the value of phase mismatch kc at a weak-focused
radiation interaction can be written as:
(8 ( 2 ) ) 2
k c = . (6)
3n0 k(3)
From (6) it is seen that the relation between the different phase shifts channels does not depend on radiation intensity
and nonlinear medium length and is determined by linear and nonlinear optical parameters of nonlinear medium only.
It makes difficult to separate two channels of nonlinear phase variations. The effective susceptibility responsible for
self-action processes caused by second-order effects can be written as:
The third-order nonlinearities responsible for the self-action can be measured at restricted crystal orientation and laser
radiation polarization when the phase mismatch magnitude exceeds critical one. The calculations showed, that the
cascade channel influence in KDP is lower at =532 nm than at =1064 nm. In KDP crystal the detuning from phase -
matching angle by several degrees can lead to the prevailing of self-action channel (Fig.1, a). The most considerable
restricted influence of cascade process in KTP must be observed at =1064 nm (Fig.1, b).
Picosecond Nd:YAG laser (=55 ps) with pulse repetition rate of 2 Hz was used in the experiments. Nonlinear-optical
characteristics of crystals were investigated at the fundamental wavelength ( =1064 nm, E=2 mJ) and its second
harmonic (=532 nm, =0.2 mJ). Laser
radiation was focused by 25 cm focal length lens
FL (Fig.2). The investigated samples S were
moved by translation stage TS along the Z axis
through the focal point of focusing lens. Energy
of laser pulses was measured by photodiode PD 1
and registered by digital voltmeter DV1. 1-mm
aperture A transmitting 3% of laser radiation
was fixed at the distance of 120 cm from the
focal plane (closed aperture scheme). The
photodiode PD2 was kept behind this aperture
for measurement of output radiation. The signal
from it was directed to the digital voltmeter DV2 . Fig.2. Experimental set-up
Closed aperture scheme allowed to determine the
sign and magnitude of nonlinear refractive index (n 2) and third-order nonlinear susceptibility k(3). For measurements
of nonlinear absorption coefficient (), the aperture A was removed (open aperture scheme). The detector was kept at
In BBO and LiNbO3 crystals the phase shift is also positive, i.e. these media possess self -focusing properties. It should
be noted that near =90o the phase shift in LiNbO 3 crystal, which was due to self-action, slowly exceeds the one of due
to cascade process. The peculiarity of T(Z) dependence for LiNbO3 crystal is a high expressed asymmetry. We
considered it to be due to the nonlinear losses. The measurements in an open aperture scheme allowed to estimate the
value of nonlinear absorption coefficient. The analysis of the valley width of normalized transmittance at different
intensities allowed to come to the conclusion about the nonlinear absorption nature. The nonlinear absorption
coefficient was calculated in the frames of the method 9. The four-photon process was found to be responsible for the
nonlinear absorption. The value of four-absorption coefficient was 1.7 10-32 cm5 W-3. It should be noted that the
influence of high-order nonlinear absorption leads to the decreasing of the distance between the maximal and minimal
transparencies in closed aperture scheme and suppresses the valley width of transmission in open aperture scheme.
The absence of nonlinear absorption at the wavelength of 1064 nm was observed in KDP and BBO crystals. In KTP
crystal of II type the measured values of nonlinearity had negative sign and was -12 10-14 esu. Thus the KTP crystal
had self-defocusing properties. In this spectral range according to the calculations the KTP crystal must have self-
focusing properties. Such disagreement between calculated and measured behavior was explained by influence of
cascade channel of phase shift variation (Fig.1, b). In this case according to (7) the sign of the measured effective
nonlineatity must be determined by value of phase mismatch k.
The results presented in Table 2 indicate that the growth of in KDP crystal leads to the decrease of Kerr
nonlinearity. These data correlate with the calculations based on empirical method (Table 1). With growth the
contribution of e-polarized wave component can become higher than that of o-polarized one. It should be noted that in
accordance to (4) the Kerr nonlinearity is determine by both and angles. In the case of |1122|<<|1111| with growth
of angle the value of the nonlinearities for all polarized wave components is decreased in angular range from 0 up to
45 degrees and is increased in the range from 45 up to 90 degrees. In the case |2233|<<|3333|, |1111|, the growth of
must decrease the value of the nonlinearity for e-polarized wave component in angular range closed to 0 degree and
increase it in the range closed to 90 degree. In other words there is a minimum value of the nonlinearity in this
angular range. In the case
|2233|>>|3333| there is a maximum 1,3 1,2
value of the nonlinearity. The relation
between the nonlinearity components
Normalized Transparency
In BBO and LiNbO3 crystals the phase shift is also positive, i.e. these media possess self -focusing properties. It should
be noted that near =90o the phase shift in LiNbO 3 crystal, which was due to self-action, slowly exceeds the one of due
to cascade process. The peculiarity of T(Z) dependence for LiNbO3 crystal is a high expressed asymmetry. We
considered it to be due to the nonlinear losses. The measurements in an open aperture scheme allowed to estimate the
value of nonlinear absorption coefficient. The analysis of the valley width of normalized transmittance at different
intensities allowed to come to the conclusion about the nonlinear absorption nature. The nonlinear absorption
coefficient was calculated in the frames of the method 9. The four-photon process was found to be responsible for the
nonlinear absorption. The value of four-absorption coefficient was 1.7 10-32 cm5 W-3. It should be noted that the
influence of high-order nonlinear absorption leads to the decreasing of the distance between the maximal and minimal
transparencies in closed aperture scheme and suppresses the valley width of transmission in open aperture scheme.
The absence of nonlinear absorption at the wavelength of 1064 nm was observed in KDP and BBO crystals. In KTP
crystal of II type the measured values of nonlinearity had negative sign and was -12 10-14 esu. Thus the KTP crystal
had self-defocusing properties. In this spectral range according to the calculations the KTP crystal must have self-
focusing properties. Such disagreement between calculated and measured behavior was explained by influence of
cascade channel of phase shift variation (Fig.1, b). In this case according to (7) the sign of the measured effective
nonlineatity must be determined by value of phase mismatch k.
The results presented in Table 2 indicate that the growth of in KDP crystal leads to the decrease of Kerr
nonlinearity. These data correlate with the calculations based on empirical method (Table 1). With growth the
contribution of e-polarized wave component can become higher than that of o-polarized one. It should be noted that in
accordance to (4) the Kerr nonlinearity is determine by both and angles. In the case of |1122|<<|1111| with growth
of angle the value of the nonlinearities for all polarized wave components is decreased in angular range from 0 up to
45 degrees and is increased in the range from 45 up to 90 degrees. In the case |2233|<<|3333|, |1111|, the growth of
must decrease the value of the nonlinearity for e-polarized wave component in angular range closed to 0 degree and
increase it in the range closed to 90 degree. In other words there is a minimum value of the nonlinearity in this
angular range. In the case
|2233|>>|3333| there is a maximum 1,3 1,2
value of the nonlinearity. The relation
between the nonlinearity components
Normalized Transparency
1,0 1,0
corresponded to three-photon absorption
mechanism. So, the nonlinear absorption in
KDP and BBO crystals were corresponded to
0,8 0,8
three-photon absorption, whereas for LiNbO3
crystals it was two-photon one. The three-
photon absorption coefficients were
0,6 0,6
determined to be 5.4 10-22 cm3 W-2 and
2.1 10-21 cm3 W-2 for KDP and BBO crystals
respectively. It should be noted that these
large values are in contrary to results of
0,4 0,4
second harmonic generation studies at high
-6 -4 -2 0 2 4 6 -6 -4 -2 0 2 4 6
intensities in KDP crystals 1,2. This
Z, cm Z, cm disagreement can be explained by the
a b influence of other nonlinear processes, in
particular by second harmonic generation of
Fig.5. Normalized transmittance dependence as a function of BBO the radiation at 532 nm, on the measurements
crystal position in open aperture scheme at different laser of nonlinear losses. For LiNbO3 crystal, the
radiation intensities (the a and b figures are obtained at value of two-photon absorption coefficient
intensities ratio of 0.4:1.) was determined to be 2.1 10-10 cm W-1 (the
values reported in works15,16 were 1.5 10-10
cm W and 1.6-2.9 10 cm W respectively).
-1 -9 -1