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Abstract
Recent development of high-power solid-state UV radiation by nonlinear optical (NLO) borate crystals is reviewed.
The performance of such UV light sources has rapidly improved in the past ve years because of the superior NLO
properties of CsLiB6 O10 (CLBO) crystals. The performance of such UV light sources also depends on the reliability of
the NLO crystals. The relation between the bulk laser-induced damage threshold (LIDT), dislocation density and UV
absorption of CsLiB6 O10 (CLBO) was investigated. A newly developed synthesis process allows the growth of CLBO
crystals with LIDT 2.5-fold higher than those grown by the conventional top-seeded solution growth (TSSG) technique.
High-quality CLBO possesses lower dislocation density and smaller absorption of UV light (k 266 nm) than con-
ventional CLBO. Reduction of the dislocation density can suppress absorption of UV light that helps to enhance the
resistance of CLBO to laser-induced damages, to alleviate thermal dephasing during high-power generation of UV light
and thus strengthen the reliability of CLBO for UV light generation. 2002 Elsevier Science B.V. All rights reserved.
0925-3467/02/$ - see front matter 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 5 - 3 4 6 7 ( 0 1 ) 0 0 1 9 4 - X
2 Y. Mori et al. / Optical Materials 19 (2002) 15
both 1064 and 266 nm. According to the general bulk LIDT, dislocation density, and UV absorp-
mechanism of laser-induced damage, some kinds tion were carried out and compared. CLBO sam-
of defects inside the optical materials are impor- ples with dimensions of 5 11 2 cm3 were
tant for UV laser-induced damage. Such defects broached from the center of the single crystal in
increase the photon absorption and decrease the (0 0 1) direction. Then, the (0 0 1) surfaces of
resistance of optical materials against laser-in- 5 11 cm2 were optically polished for the mea-
duced damage. Therefore, improving the crystal- surement of the bulk laser damage threshold. The
linity of CLBO crystals is supposed to reduce the 4x of Nd:YAG laser (0.75 ns pulse duration) was
UV absorption and enhance the LIDT in the bulk employed by operating at the single shot mode.
of CLBO. Detailed description of the measurement of LIDT
We have developed a new crystal growth pro- is reported elsewhere [25]. The damage threshold
cess for obtaining CLBO with high bulk LIDT by of the conventional CLBO ranged from 8.8 to
solution stirring [23]. CLBO crystal grown by such 10:4 GW=cm2 . In contrast, the damage threshold
a technique was found to have 2.5-fold higher of the high-quality CLBO crystals was higher than
bulk LIDT than that of the fused silica and con- that of the fused quartz (10:4 GW=cm2 ) and the
ventional CLBO. The CLBO crystals employed for conventional CLBO crystal. The average of the
investigation were grown by conventional top- damage threshold is about 15.020.0 GW/cm2 , and
seeded solution growth (TSSG) [24] and solution the highest in the sample was 25:4 GW=cm2 .
stirring [23] techniques. The saturation tempera- The relationship between crystallinity of CLBO
tures were varied from 844.0 to 842.6 C. The and the bulk LIDT was then examined. Chemical
synthesis temperatures were decreased by 0.1 C/ etching of polished CLBO surface was used for
day during growth. CLBO (1 0 0) was used as the revealing the dislocation density. The composition
seed crystals for both techniques. The CLBO of the etcher for the plane (0 0 1) of CLBO crystals
crystals with dimensions 12 6 5 cm3 were was: 0.5 l of CH3 COOH 0:5 l of H2 O 80 g of
typically grown in 16 days. The characterization of CH3 COONH4 , the time of etching was about
4 Y. Mori et al. / Optical Materials 19 (2002) 15
20 min. Typical dislocation density can be esti- Type-I fourth harmonic CLBO crystals that have
mated from the number of hillocks per square conventional crystallinity and high-crystallinity
centimeter by optical microscopy. For high-quality were used in the generation of the UV light.
CLBO crystals, the dislocation density ranged During the generation of fourth harmonic light,
from about 6.6 to 15:0 103 cm2 . The relation- UV photons were absorbed and the photon energy
ship between the dislocation densities and the bulk was dissipated as heat. This can be indicated by an
LIDT is shown in Fig. 3. The lateral axis repre- increase of the temperature of the crystal. Since
sents ratios of the LIDT of CLBO to LIDT of determination of internal crystal temperatures is
fused quartz; i.e., at a ratio of unity LIDTCLBO not easy, we chose to measure the temperature at
LIDTfused silica 10:4 GW=cm2 . For CLBO crys- the output surface with a thermo-viewer. The re-
tals that have relatively low LIDT (ratio was about sults are shown in Table 1. At UV output of 0.6 W,
1.2), the dislocation density was 15 103 cm2 . the temperature around the output laser beam spot
On the other hand, dislocation density of the is about the same despite of the dierence of
CLBO crystal that has high LIDT was crystallinity. The initial temperatures were 20 C,
6 103 cm2 . In short, the LIDT of CLBO in- and the mean temperatures after 5 min of UV light
creased with the decrease of dislocation density. generation were 23 C for both type of CLBO
Thus, the improvement of crystallinity enhances samples. However, at UV output of 5 W, the
the resistance of CLBO against bulk laser-induced maximum temperature detected on the high-qual-
damage. ity crystals was 30% lower than that measured on
The inuence of crystallinity on UV absorption the conventional CLBO. The initial temperatures
was then investigated as a function of UV were 31 C and the mean temperatures after 5 min
(k 266 nm) output power. For this purpose, of UV light generation were 40 and 37.0 C for
conventional and high-quality CLBO crystals, re-
spectively. This result indicates that high-quality
CLBO has lower UV absorption and thus lesser
thermal generation and smaller temperature gra-
dient along the NLO interaction bath of the laser
beam. This means, high-quality CLBO crystals
could eectively reduce UV absorption and sup-
press thermal dephasing for the generation of
high-power UV light.
3. Conclusion
Table 1
Inuence of crystallinity on the crystal temperatures generated by UV absorption
Generated UV power Initial temperature Detected maximum temperature (C)
(W) (C)
Conventional CLBO High-quality CLBO
0.6 20.0 23.0 23.0
5.0 31.0 40.0 37.0
Y. Mori et al. / Optical Materials 19 (2002) 15 5
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