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Journal of Crystal Growth 237239 (2002) 645648

Effect of crystallinity on the bulk laser damage and


UV absorption of CLBO crystals
R. Onoa,*, T. Kamimuraa, S. Fukumotoa, Y.K. Yapa, M. Yoshimuraa,
Y. Moria, T. Sasakia, K. Yoshidab
a
Department of Electrical Engineering, Osaka University, 2-1 Yamadaoka Suita, Osaka 565-0871, Japan
b
Department of Electronic Engineering, Osaka Institute of Technology, 5-16-1 Ohmiya, Asahi-ku, Osaka 535-8585, Japan

Abstract

The inuence of crystal defects on bulk laser damage and UV absorption in CsLiB6O10 (CLBO) crystals was
investigated. A CLBO crystal grown by the solution stirring method had a 2.5-fold higher laser-induced damage
threshold (maximum) than conventional CLBO crystals. This highly damage-resistant CLBO crystal had a lower
dislocation density (best value, 6.6  103/cm2) than conventional CLBO crystals (best value, 15.0  103/cm2). The
temperature increase during UV generation on the output surface of highly damage-resistant CLBzO crystal was lower
than that detected in conventional CLBO crystal. r 2002 Elsevier Science B.V. All rights reserved.

PACS: 81.10; 42.70.M; 42.55.P; 42.55.R

Keywords: A1. Single crystal growth; B1. Borates; B2. Nonlinear optic materials; B3. Harmonic generators; B3. Solid-state lasers

1. Introduction ture bandwidths. In 1999, Kojima et al. [3]


reported the highest output power (20.5 W) of
High-power solid-state ultraviolet (UV) lasers fourth harmonic generation from a Nd:YAG laser.
with nonlinear optical (NLO) crystals are in high Generally, laser-induced damage and thermal
demand for various industrial applications because dephasing of NLO crystals are the main limita-
of their cost-performance and convenient opera- tions for developing high-power solid-state UV
tion. The performance of such UV lasers greatly lasers. Both problems in high-power UV genera-
depends on the ability and reliability of the NLO tion are mainly related to the defects inside the
crystals. CsLiB6O10 (CLBO) crystal, which is NLO crystals. Therefore, improving the bulk
employed for the fourth (266 nm) and fth quality of NLO crystals can effectively reduce the
(213 nm) harmonic generation of a Nd:YAG laser, UV absorption, suppress the thermal dephasing,
[1,2] is a promising NLO crystal due to its small enhance the bulk laser damage threshold, and
walk-off and large angular, spectral and tempera- improve the performance of solid-state UV lasers.
In this study, we developed high-quality CLBO
crystals by the solution stirring method and
*Corresponding author. Tel.: +81-6-6879-7707; fax: +81-6-
6879-7708. investigated the inuence of crystal defects on the
E-mail address: ono@ssk.pwr.eng.osaka-u.ac.jp (R. Ono). bulk laser damage threshold and UV absorption.

0022-0248/02/$ - see front matter r 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 0 2 2 - 0 2 4 8 ( 0 1 ) 0 2 0 2 1 - 8
646 R. Ono et al. / Journal of Crystal Growth 237239 (2002) 645648

2. Crystal growth of CLBO CLBO samples grown by both methods were


investigated for dislocation, bulk laser damage
Conventionally, crystal growth of CLBO has threshold, and UV absorption.
been performed by the Top-Seeded Solution
Growth method (dened as N-TSSG (Normal
TSSG) in this paper) with a rotating seed crystal.
[4] However, the CLBO solution is highly viscous, 3. Dependence of bulk laser damage threshold on
so it was difcult to obtain uniform supersatura- dislocation density
tion during crystal growth. To improve super-
saturation distribution, we introduced an effective We measured the bulk laser damage threshold in
solution stirring technique for the TSSG method several CLBO samples with polished (0 0 1) sur-
(dened as SS-TSSG (Solution Stirring TSSG) in faces. The fourth harmonic of the Nd:YAG laser
this paper) [5,6]. Crystal growth by SS-TSSG was (266 nm with 0.75 ns pulse duration) was employed
carried out under the same growth conditions as in the single shot operation mode for measure-
for N-TSSG. Specically, seed crystals were CLBO ment. The experimental setup is illustrated in
(1 0 0), and the temperature decrease was 0.11C/ Fig. 2. The laser irradiated into the sample was
day. In typical crystal growth using this technique, focused 5 mm below the (0 0 1) surface by a lens
a CLBO crystal was grown to a size of with a focal length f 100 mm. The experiment
12  6  5 cm3 in 16 days (shown in Fig. 1). Several was performed according to the 1-on-1 proce-
dure, i.e., the damage threshold was measured
every time in a new site of the crystal. Bulk laser
damage was identied by visually observing a laser
spark and by the scattering from a coaxial HeNe
laser beam as a real-time indicator. The damage
threshold of N-TSSG crystals ranged from 8.8 to
10.4 GW/cm2. In contrast, the damage threshold
of SS-TSSG crystals was higher than that of fused
silica (10.4 GW/cm2) and N-TSSG crystals. The
average range of the damage threshold was
15.020.0 GW/cm2, and the highest threshold was
25.4 GW/cm2.
To investigate the inuence of defects on
bulk laser damage, we measured the dislocation
density in several CLBO samples with different
Fig. 1. ClBO crystal grown by solution stirring TSSG method. laser damage resistances. Chemical etching was

Energy meter CLBO crystal KTP crystal


Biplanar 4 type I 2 typeII
p hototube
Nd:YAG laser
Oscillator/Amplifier

Oscilloscope
Attenuator Lens f = 100mm Sample

Fig. 2. Experimental setup for the measurement of bulk laser damage threshold.
R. Ono et al. / Journal of Crystal Growth 237239 (2002) 645648 647

employed to reveal defects (hillocks as shown in decreased to 6.6  103/cm2. Thus, improving crys-
Fig. 3) on polished (0 0 1) surfaces of samples. The tallinity can enhance the laser damage threshold of
etching solution was 0.5 l of CH3COOH+0.5 l of CLBO crystals.
H2O+80 g of CH3COONH4, and the etching time
was xed at 20 min. The number of hillocks per
cm2 was estimated as the dislocation density. The 4. Inuence of crystallinity on UV absorption
relation between the dislocation density and the
bulk laser damage threshold is shown in Fig. 4. In high-power UV generation, UV absorption
The lateral axis indicates the ratio of the bulk of NLO crystals decreases wavelength conversion
damage threshold of CLBO to that of fused silica. efciency due to thermal dephasing [7]. To
For CLBO samples with low-damage resistance investigate the inuence of crystallinity on UV
(ratio of about 1.2), the dislocation density was absorption, we measured the temperature increase
15.0  103/cm2. In contrast, the dislocation density of CLBO crystals caused by UV absorption when
of the most highly damage-resistant crystals was generating the fourth harmonic of a Nd:YAG
laser. In this experiment, we prepared CLBO
samples (4HG, Type I) with conventional crystal-
linity (bulk laser damage threshold 10.0 GW/cm2;
dislocation density 15.0  103/cm2) and high
crystallinity (bulk laser damage threshold 15.0
18.0 GW/cm2; dislocation density 7.010.0  103/
cm2). The second harmonic (532 nm) laser was
focused into the crystal using a quartz lens. We
measured the temperature increase using a thermo-
viewer. Since this instrument could not detect the
temperature inside the crystal very well, we
measured the temperature increase on the output
surface of the crystal. The output surface initial
temperature was set at 31.01C. During UV
generation at 5 W, the maximum temperature
Fig. 3. Hillocks on CLBO surface after chemical etching. detected in a high-crystallinity crystal increased
to 37.01C in 5 min, which was 3.01C lower than
that detected in conventional crystallinity crystal.
20 This result indicates that a CLBO crystal with
Dislocation density (10 cm )

fewer defects has lower UV absorption and a


-2

smaller temperature gradient in the crystal. Thus,


15
3

a CLBO crystal grown by SS-TSSG could


effectively reduce UV absorption and suppress
10 thermal dephasing for applications in generating
high-power UV laser light.

5
5. Conclusion
0
We investigated the inuence of crystallinity on
1 1.5 2 2.5
the bulk laser damage threshold and on the
Relative damage threshold (CLBO/fused quartz) absorption of UV laser light. We measured the
Fig. 4. Relationship between the dislocation density and the bulk laser damage threshold for an UV laser
bulk laser damage threshold. (266 nm) in CLBO crystals grown by both
648 R. Ono et al. / Journal of Crystal Growth 237239 (2002) 645648

N-TSSG and SS-TSSG. The maximum damage References


threshold of SS-TSSG crystals was 25.4 GW/cm2,
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Lasers 26 (1999) 93.
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