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Optical Materials 19 (2002) 15

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Recent development of nonlinear optical borate crystals


for UV generation
Y. Mori *, Y.K. Yap, T. Kamimura, M. Yoshimura, T. Sasaki
Department of Electrical Engineering, Sasaki Laboratory, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan

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.

1. Introduction (k  1 lm) solid-state lasers by using nonlinear


optical (NLO) crystals. Until 1975, most NLO
Ultraviolet lasers are viewed as clean energy crystals were based on the PO, IO and NbO
sources for the synthesis and processing of ma- bonds like those in KDP (KH2 PO4 ) [1,2], LiIO3
terials. High-power coherent UV output is mainly [3,4] and LiNbO3 [5]. Because of the relatively
available from excimer lasers (e.g., XeCl, KrF high resistance against laser-induced damage and
and ArF). However, these bulky lasers use cor- higher transparency in the UV region, NLO
rosive gases, require high voltage gaseous dis- crystals with BO bonds are presently employed
charges and regular maintenance. A compact, for high-power UV light generation. The rst
maintenance-free, all-solid-state alternative is borate crystal described for UV generation was
therefore desired. An eective technique for the KB5 O8  4H2 O (KB5) [6]. However, intense re-
generation of UV light is cascaded sum-frequency search on borate crystals was initiated only after
generation pumped by the output of near-IR the development of b-BaB2 O2 (BBO) [7]. A review
on borate crystals is recently reported elsewhere
[8]. In this paper, we discuss the important factors
*
Corresponding author. Tel.: +81-6-879-7707; fax: +81-6-
that aect the development of such solid-state UV
879-7708. light sources, i.e., the ability and reliability of the
E-mail address: mori@pwr.eng.osaka-u.ac.jp (Y. Mori). NLO crystals.

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

2. Results and discussion

2.1. The ability factor of NLO crystals

The performance of such solid-state UV lasers


depends on the ability of the NLO crystals that are
employed for laser frequency conversion. Until
1993, many borate and nonborate crystals have
been examined for UV harmonic generation of the
Nd:YAG lasers [9]. In 1995, BBO was shown to
generate 3.5 and 1.3 W of fourth (4x, k 266 nm)
and fth (5x, k 213 nm) harmonics of Nd:YAG
lasers [10]. The discovery of CsLiB6 O10 (CLBO)
[11,12] crystals has further enhanced the perfor-
(Ref. 14)
mance of such solid-state UV light sources. The
superior abilities of CLBO crystals for generating
4x and 5x of Nd:YAG lasers were clearly dem- (Ref. 15)
onstrated at 10 Hz [1315], 100 Hz [15,16], 1 kHz
[17] and 10 kHz [18,19]. For example, the 266 nm
output from CLBO is 2.5 times higher than that
generated from high-quality BBO (super-BBO/S-
BBO) [17]. Besides, an average output of 20.5 W at
k 266 nm was recently achieved by means of
CLBO crystals [18,19]. The CLBO crystal is no Fig. 1. Progress of average UV output power from NLO
doubt the most eective NLO crystal for deep-UV crystals in the past two decades.
light generation. This is due to the relatively small
walk-o angle of CLBO (related to its moderate 2.2. The reliability factor of NLO crystals
birefringence) that produces better spatial over-
lapping of the mixing beams. Its relatively large Beside the property of NLO crystals, the reli-
angular, spectral and temperature acceptance ability issues are important for the practical ap-
bandwidths favor CLBO for stable UV light gen- plication of solid-state UV light source. In general,
eration [13]. The improvement on average UV thermal dephasing and laser-induced damage of
output power generated by NLO crystals in the NLO crystals are the main limitation for the de-
past two decades are summarized in Fig. 1. As velopment of high-power solid-state UV light
shown, the progress of output power is drastically sources. The alleviation of thermal dephasing was
improved in the past ve years. demonstrated to improve performance of CLBO
It is noteworthy that CLBO was demonstrated by 2.3-fold [16]. Ion beam etching was shown to
to produce deep-UV light at k 193 nm by 8x enhance the laser-induced damage threshold
generation of the Er3 -doped ber amplier [20]. (LIDT) of the CLBO surface [21]. However, there
The conversion eciency from the fundamental remained some unknowns about LIDT in the bulk
wavelength of 1547 nm was 7% by using the of CLBO. At a laser wavelength of 1064 nm, LIDT
CLBO crystal as the eighth harmonic generator at the bulk of conventional CLBO is 29 GW=cm2 ,
(x 7x). The conversion eciency was 1.3% higher than that of fused silica (damage threshold:
when CLBO was replaced by LiB3 O5 (LBO) 25 GW=cm2 ) [11,12]. However, the LIDT of a
crystal. The schematic layout of this experiment is CLBO at laser wavelength of 266 nm was about
shown in Fig. 2. This is the most eective gen- 9 GW=cm2 , lower than that of fused silica
eration of 193 nm light from an all-solid-state (10:4 GW=cm2 ) [22], despite the fact that both
system. materials have insignicant photon absorption at
Y. Mori et al. / Optical Materials 19 (2002) 15 3

Fig. 2. Experimental setup for deep-UV light generation at 193 nm.

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

As a summary, we have reviewed the recent


development of high-power solid-state UV light
sources using NLO crystals. Clearly, the perfor-
Fig. 3. The relationship between dislocation densities and the mance of such light sources strongly depends on
bulk LIDT of CLBO. the properties of NLO crystals employed. The

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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