68 IEEE PHOTONICS TECHNOLOGY LE'ITERS, VOL. I . NO.

I , JANUARY 1995

Temperature Dispersion in
KTP for Nonlinear Devices
Gorachand Ghosh

Abstract- Thermo-optic coefficients (dii / d T ) determine the
temperature characteristics of the nonlinear optical laser devices.
These coefficients are analyzed critically by using a new model
for the first time to formulate the temperature dispersion which
can predict accurately the temperature bandwidths for various
nonlinear interactions in a flux-grown KTP crystal. This model
is based on the optical bandgaps, such as excitonic, a newly
identified isentropic, and the thermal expansion coefficient.
1. INTRODUCTION
T HE refractive index, its variation as a function of tem-
perature, i.e., the thermo-optic coefficient (dn/dT),and
their dispersion are important characteristics of the nonlinear
crystals which are used in high-power nonlinear optical laser
devices (NLOD's). A part of the transmitted laser power is
absorbed by the crystal which is heated up and ultimately, the
refractive index of the crystal is changed. Also, by changing
the ambient temperature of the crystal, a temperature-tuned
NLOD can be made. Therefore, the representation of refractive
indexes with temperature of the KTP crystal is state-of-the-art
in nonlinear optics.
Potassium titanyl phosphate (KTP) is a superior, frequently
used nonlinear crystal for second harmonic generation (SHG)
of Nd:YAG and other lasers as well as for sum- and difference-
frequency generation at various wavelengths [ 11 even by using
diode lasers [2]. Accurate values of refractive indexes and
their temperature dependence are necessary to optimize the
conversion efficiencies. In this letter, these values are analyzed
critically by using a physically-meaningful model where the
temperature coefficient of the excitonic bandgap, a newly
identified bandgap called isentropic, and the thermal expansion
coefficient are considered. The optimum fitted constants are
used to verify the presently available temperature-dependent
nonlinear optical laser devices more accurately.
(A is the wavelength in pm), where the last term accounts
for decrease in refractive indices due to lattice absorption, the
first and second terms represent respectively the contribution
to refractive indexes due to higher and lower energy bandgaps
of electronic absorption. The normal approach for calculating
these coefficients is to first find the initial values of the
parameters and then to add corrections by an iterative process
so as to minimize the deviation between the measured and
computed values. The choice of the value for E is not critical.
The E value essentially determines the infrared transmission
cut off. The refractive indexes of the KTP crystal [4] are fitted
to evaluate the Sellmeier coefficientswhich are shown in Table
I at room temperature.
111. ANALYSES
OF THERMO-OPTIC
COEFFICIENTS
Thermo-optics coefficients of KTP crystal were fitted by
an empricial formula [5], [6] without having any physical
significance. On the other hand, recently, I observed that the
temperature coefficient of the peak energy in reflectivity, called
the excitonic band gap (Eeg)yields the dominant contribution
to dn/dT in the optical fiber glasses [5]. Also, I observed in
analyzing the thermo-optic coefficients of LiNb03, LiTaO3,
and some standard optical glasses [6] that the fitting bandgap
is invariant under temperature and this bandgap is very near
to the bandgap corresponding to the band-to-band transition.
This bandgap is responsible for the dispersion of thermo-
optic coefficients of the nonlinear crystals. This bandgap
is assigned as the isentropic bandgap (Ejg)of the optical
materials. Therefore, the equation for representing thermo-
optic coefficients can be described in terms of the linear
expansion coefficient a , the excitonic and isentropic bandgaps
as

11. DERIVATION
OF ROOMTEMPERATURE
SELLMEIERCOEFFICIENTS where n, dn/dT, and xe are the room temperature refractive
index, its variation with temperature, and the electronic sus-
The refractive indexes are measured at specific wavelengths
ceptibility. (l / E e g. dEe,/dT) is the temperature coefficient
with greater accuracy. There are various forms of Sellmeier
of the excitonic bandgap. E is the photon energy and Ei, is
equation to represent refractive indexes in the transmission
the isentropic bandgap lying in the vacuum ultraviolet (VUV)
region. The best physically-meaningfulwavelength dependent
or UV region for the optical materials. Equation (2) can be
Sellmeier is of the form [3]
rewritten in terms of the normalized dispersive wavelength R
+ +
n2 = A B/(1 - C/A2) D / ( 1 - E / X 2 ) (1) as
Manuscript received May 9, 1994; revised August 12, 1994.
G. Ghosh is with the Electrotechnical Laboratoly, Light and Radio Waves
Section, 1-1-4, Umezono, Tsukuba-shi, Ibaraki-305, Japan.
IEEE Log Number 9407090. =GR+HR~ (3)
1041-1 135/95$04.00 0 1995 IEEE
GHOSH: TEMPERATURE DISPERSION IN KTP FOR NONLINEAR DEVICES 69

n
lSOa I+ + (722 =
SELLMEIER
TABLE I
COEFFICIENTS
.-I B/(1 - C / X 2 )
AT 20°C
D/(1 - E / X 2 ) )
Y\ Index Sellmeier Coefficients
LD
0 100 - A B C D E
d
W

t-( n, 2.0009584 1.0011186 4.0294037 x10-2 1.7740435 150

a
d

4
50:
ny

n,
2.041 1662

2.2541202
0.9874869

1.0539416
4.3432843 x10-2

5.5303637 xl0-2
1.8828437

2.2516434
150

150

N
6" TABLE I1
I INTERFOLATED
COEFFICIENTSI N DISPERSIONRELATION
O0:2 0:4 ' 0:s 1:O 1:2 1:4
0:6 ' ' ' ' 116
2iidn/dT = G R H?; COMPARISON + OF THEORETICAL AND
' '
EXPERIMENTAL
LINEAR EXPANSIONCOEFFICIENT, THE TEMPERATURE
COEFFICIENT
OF THE EXCITONIC
BANDGAP, ( dE, / d T ) AND
WAVELENGTH (Fm) AND ISENTROPICBANDGAPS
THE EXCITONIC FOR KTP CRYSTAL

Fig. 1. 27z, . y d i i , . / d T versus wavelength for KTP crystal: solid lines are Set lndcx G H Bandgaps o.IIWPCI dEeg/dT[10-4eV/~CI Reference
isentropic excitenic for data. of
the computed curves; points are the experimental values; solid circle [ 6 ] , 110-6PC1 1106PCI (rrm)[eVl [eV1 From Fmm From From n. dn/dT, o
open circle [9], and solid square [5]. Exp Fitting Expt. Fitting & dkg/dT

n. -51.4515 69.8539 0.203 16.11 4 I 6.8 - 11.0 9.6 4 . 0 -1.M) 141. [IO].
I ny -51.6725 75.8440 0.22715.51 41 9.0- 9.8 9.6 -1.74 ( 1 1 1 , [71
.n .7.4595 529338 0.2791441 41 - 1 . 3 - 0.6 1.1 - I .07

L300 n. -51.9928 101.957 0.2131581 4 1 7.8-11.0 95 -2.34 141, 181. 191

200 J1 l v
h

\
II ny
nz
-49.5947
-02.0620
127.882
115.663
0.198 16.31 4 1
0.212 15 81 4 I
9 0 - 9.8
- I 3 - 0.6
9.2
0.3
-2.93
-2.34
1111, 171

-200 2
rD

and is normally negative for the nonlinear crystals (71. This

0 ~ ' ' " ' " ' ~ '
0.2 0.4 0.6 0.8 1.0 1.2 1.4
WAVELENGTH (pm)
Fig. 2. 211 . d u / d T versus wavelength for KTP crystal: solid lines and the
dashed plus curves are the computed curves for y and z axes respectively;
points are the experimental values; solid circle [6], open circle [9], and solid
square [5].
where R = A2/(A2 - A:g), and the constants G and H
are related respectively to the thermal expansion coefficient
cy and the temperature coefficient of the excitonic bandgap
Eeg, respectively, by the relations G = -3aK2, H =
-l/Eeg . dEeg/dT . K 2 and the constant K is related to the
less dispersive refractive index nld at the IR as K 2 = nld' - 1.
It is clear from (3) that the product is controlled by two factors
which normally compete with one another to give positive or
negative values of dn/dT. The first factor, the contribution
from the thermal expansion coefficient a , is negative because
cy is normally positive for nonlinear crystals. The contribution
is also small because Q is of the order of 10-6/oC. On the
other hand, in the second factor, the temperature coefficient
of the excitonic bandgap is of the order of lop4 eV/"C
v
contribution is positive in general and larger than the first one
h to yield positive values of dn/dT.
d
h Normally, from a set of measured (n, dn/dT, A) data
-100 d adopting least squares procedure, the optical constants G
4 and H are evaluated by an appropriate bandgap (Aig) being
N
G scanned from the lowest gap to the highest value. Recently,
the procedure [5] has been described in detail. The optimum
- 0 fitted constants G and H are shown in Table I1 along with
the data sources at 20°C. The experimental points and the
~ ' ' fitted
~ curves are shown in Fig. 1 and Fig. 2 for the thermo-
1.6 optic coefficients along 5 , and y, z axes respectively. The
error bars are also indicated by considering the accuracy of
the thermo-optic coefficients measurement. From the fitted
constants, thermal expansion coefficient a and the variation
of the excitonic bandgap with temperature are calculated and
are also shown in Table 11. Since there is no peak energy in
reflectivity data for KTP crystal, I have used the energy gap
corresponding to the electronic absorption gap for calculating
dE,,/dT. These values are compared with the experimental
values of the available KDP crystal [7] and agree reasonably
well within the experimental accuracy
IV. TEMPERATUREBANDWIDTHS
FOR NONLINEAR
INTERACTIONS
In order to test the validity and accuracy of the foregoing
formulation, I have computed both critical and noncritical
temperature phase-matching bandwidths for various three-
wave parametric interactions in a KTP crystal by using the
optical constants cited in Table I and 11. The phase-matching
~

70 IEEE PHOTONICS TECHNOLOGY LETTERS, VOL. 7, NO. I , JANUARY 1995

TABLE 111 ACKNOWLEDGMENT

CALCULATED AND REPORTEDTEMPERATURE PHASE-MATCHING
BANDWIDTHS FOR SHG, SFG, AND DFG IN KTP The author thanks the Science and Technology Agency,
Japanese Government, for awarding him the STA fellowship.
Wavelength (pm)(d) Phase-Match- AT.L (OC. cm)
ing Angle He is also grateful to Dr. H. Yajima and M. Endo of this
11 12 h3 (e*+) Calculated Observed Refs. laboratory for critical reading of the manuscript. He thanks
Set I Set I1 for Expt. Dr. W. Wiechmann of Sony Corporation for providing the
unpublished data of the refractive indexes against temperature.
0.994X 0.9942 0.497X (900, 900) 173 1 4 6 175 1131
1.06421 0.80682 0.4589X (900, 900) 139 112 122 1141 REFERENCES
1.0642XY 1.06422 0.5321XY (900, 230) 24 26 24 1151, 1161
I .0642X 1.06421 2 0.5321“ (68.60.900) 100
[ 11 J. D. Bierlein and H. Vanherzeele, “Potassium titanyl phosphate: Prop-
98 100 1161
erties and new applications,” J . Opt. Soc. Am. B, vol. 6, pp. 622433,
1.0796Y 1.07962 0.5398Y (900.00) 20 18 20 1171 1989.
1.3188Y 0.65942 0.4396Y (90°, 00) 9.0 8.0 8.5 f0.5 1181 [2] W. Wang and M. Ohtsu, “Frequency tunable sum- and difference-
frequency generation by using two diode lasers in a KTP crystal,” Opt.
1.3382Y 0.6691” 0.4461Y (90°, 00) 10.0 9.0 8 . 5 f 0 . 5 1181
Commun., vol. 102, pp. 304-308, 1993.
1.5791z= 1.0642Y 0.6358Y (75.50, 00) 30 30 29.5 f 0 . 5 1191 (31 G. C. Ghosh and G. C. Bhar, “Temperature dispersion in ADP, KDP,
1.62” 1.54Y 0.78Y (52.10, 00) 70 43 insensitive 121 and KD*P for nonlinear devices,” IEEE J . Quantum Elecfron., vol. 18,
pp. 143-145, 1982.
1.542” 0.78Y 0.52Y (590, 00) 48 46 to temp. 121 [4] K. Kato, “Parametric oscillation at 3.2 p m in KTP pumped at 1.064
pm,” IEEE J . Quantum Elecfron., vol. 27, pp. 1137-1 139, 1991 (and
Note: (d) 1 / X 1 +
1 / X 2 = l / X : $ . The superscripts of the interacting references cited therein.)
wavelengths represent the polarization directions. [5] G. Ghosh, “Temperature dispersion of refractive indexes in some silicate
fiber glasses,” IEEE Photon. Technol. Left., vol. 6, no. 3, 1994.
[6] -, “Thermo-optic coefficients of LiNb03, LiIO3 and LiTaO3
temperature bandwidths are given by [12] nonlinear crystals,” to he published.
[7] R. Onaka and T. Takeda, “Temperature Dependence of the Refractive
Indices of ADP,” J . Phys. Soc. Jap., vol. 51, pp. 3258-3261, 1982.
[8] D. J. Gettemy er al., “Some optical properties of KTP, LiI03 and
LiNb03,” IEEE J . Quantum Elecfron., vol. 24, pp. 2231-2237, 1988.
[9] K. Kato, “Temperature insensitive SHG at 0.5321 in KTP,” IEEE J .
Quantum E k t r o n . , vol. 28, pp. 1974-1976, 1992.
Here A T denotes the temperature bandwidth, L is the crystal [IO] W. Wiechmann et al., “Refractive-index temperature derivatives of
length, and XI, Xz, and A3 are the fundamental (indexes 1 , potassium titanyl phosphate,” Opt. L e f f . ,vol. 18, pp. 1208-1210, 1993
and private communication.
2 ) and second-harmonic or sum-frequency (index 3 ) wave- [ I I ] D. K. T. Chu, J. D. Bierlein, and R. G. Hunsperger, “Piezoelectric
lengths. The terms d n l /dT, dnz/dT, and dn3/dT represent and acoustic properties of potassium titanyl phosphate (KTP) and
the thermo-optic coefficients for the fundamental and second- its isomorphs,” IEEE Trans. Ulfrason. Ferroelect. Frequency Contr.,
vol. 39, pp. 683-687, 1992; in Technical Catalogue, Litton Airtron,
harmonic or sum-frequency light components with the crystal Synoptics Group, USA.
orientation taken into consideration. The computed and the [I21 V. G. Dmitriev and G. G. Gurzadyan, “Applications of nonlinear
cwstals,” Handbook of Nonlinear Optical Cfystals. Berlin: Springer-
experimental values are shown in Table 111, which speaks for
Virlag, 1991.
itself. Therefore, the optical constants, cited in Table I and I1 [13] W. P. Risk et al., “Noncritically phase-matched frequency doubling
can be used to evaluate the temperature-dependent Sellmeier using 994 nm dye and diode laser radiation in KTiOP04,” Appl. Phys.
Lett., vol. 55, pp. 1179-1181, 1989.
coefficients. 141 J. C. Baumert et ul.,“Generation of blue cw coherent radiation by
sum frequency mixing in KTiOP04,” Appl. Phys. Left., vol. 51, pp.
V. CONCLUSION 2192-2194, 1987.
151 T. Y. Fan et al., “Second harmonic generation and accurate index of
I have analyzed the thermo-optic coefficients of KTP crystal refraction measurements in Hux-grown KTIOP04,” Appl. Opt., vol. 26,
in a new, physically meaningful model. The energy gap pp. 2390-2394, 1987.
161 T. Kishimoto, K. Imamura, and M. Itoh, “Temperature stable SHG of
corresponding to the peak energy in reflectivity, called the
Nd:YAG laser by KTiOP04,” in Dig. Annu. Meeting Japan Soc. App.
excitonic bandgap, plays a dominant role in determining the Phy., Tokyo: paper 29p-PB-1 I , 1991.
thermo-optic coefficients. Also, the fitting energy gap which 171 V. M. Garmash et al., “Efficient second-harmonic generation in potas-
sium titanate-phosphate crystals with noncritical matching,” Soy. Tech.
lies very near to the the band-to-band transition, called the Phy.s. Lett., vol. 12, pp. 505-506, 1986.
isentropic bandgap, determines the dispersion of thermo-optic 181 R. A. Stolzenberger et al., “Type I1 sum frequency generation in flux
coefficients. The temperature dispersion equations are capable and hydrothermally grown KTP at 1.319 and 1.338 mm,” IEEE Photon.
Technol. Left., vol. 1, pp. 446448, 1989.
to explain the temperature effect in nonlinear optics more 191 K. Kato, “Parametric oscillation at 3.2 mm in KTP pumped at 1.064
accurately. mm,” IEEE J . Quantum Elecfron., vol. 27, pp. 2043-2046, 1991.