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Optical Materials 16 (2001) 213220

www.elsevier.nl/locate/optmat

Nd:GdCOB: overview of its infrared, green and blue laser


performances
Daniel Vivien a,*, Frederic Mougel a,b, Frederica Auge c, Gerard Aka a,
Andree Kahn-Harari a, Francois Balembois c, Gaelle Lucas-Leclin c,
Patrick Georges c, Alain Brun c, Patrick Aschehoug a, Jean-Marie Benitez a,
Nicole Le Nain d, Michelle Jacquet d
a
Laboratoire de Chimie Appliqu ee de l'Etat Solide, ENSCP, URA-CNRS 1466, 11 rue Pierre et Marie Curie,
75231 Paris Cedex 05, France
b
Crismatec, B.P. 521, 77794 Nemours Cedex, France
c
Laboratoire Charles Fabry de l'Institut d'Optique, B.P. 147, 91403 Orsay, France
d
Laboratoire d'Optique des Solides, Atelier d'Optique Cristalline, Universit
e Pierre et Marie Curie, 4 place Jussieu,
75252 Paris Cedex 05, France

Abstract
GdCOB (Ca4 GdB3 O10 ) is a new non-linear optical material which can be grown in large sized crystals by the
Czochralski method. In this material, part of the gadolinium ions can be replace by Nd3 without signicant decrease of
the crystal quality. Nd:GdCOB single crystals exhibit laser action in the infrared at 1060 and 1091 nm simultaneously.
The two transitions involved originating from the two Kramers doublets of the 4 F3=2 state, their respective contributions
depend upon the temperature of the Nd:GdCOB crystal. By combining the non-linear properties of the GdCOB matrix
and the laser emission due to ND3 ions, it is possible to generate directly by self-frequency doubling 115 mW of green
laser light at 530.5 nm under diode pumping at 810 nm. It is also possible to self-double the 936 nm emission of
Nd:GdCOB, leading to blue laser emission, but only under pulsed titanium-sapphire laser pumping. However, a CW
blue laser beam is obtained in Nd:GdCOB by self sum-frequency mixing of the 1090 nm laser emission and the residual
pump beam at 812 nm, yielding 1.2 mW of 465 nm laser light, with an optical to optical eciency of 0.3%. This paper
ends with a survey of the Nd:YCOB laser characteristics which are compared to those of Nd:GdCOB. 2001 Elsevier
Science B.V. All rights reserved.

Keywords: Nd:GdCOB; Non-linear optical material; Neodymium laser; Self-frequency doubling; Green laser; Blue laser; Self sum-
frequency mixing

1. Introduction applications including high density data storage,


laser printing, photolithography, cytometry, par-
Diode pumped solid state green and blue lasers ticle size measurements, undersea communica-
are of considerable interest for a wide variety of tions, display systems, etc. They may also replace
argon ion laser which are much less versatile and
have very low electrical to optical conversion e-
*
Corresponding author. ciency.

0925-3467/01/$ - see front matter 2001 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 5 - 3 4 6 7 ( 0 0 ) 0 0 0 8 0 - X
214 D. Vivien et al. / Optical Materials 16 (2001) 213220

Production of laser beams in the 400550 nm non-congruent melting and can only be grown
range can be performed using crystals doped with using ux techniques. It is therefore very expensive
Pr3 [1] or other lanthanides ions (Er3 , Tm3 , . . .) and only available in limited size. This restricts its
through up-conversion processes [2,3]. Recently, practical applications.
gallium nitride diodes [4] have appeared as blue In this overview, we will rst summarize the
laser sources. Another way to generate green or infrared laser properties of Nd:GdCOB crystals.
blue coherent beams is to use the second harmonic Then the production of green laser beams by self-
generation (SHG), through an appropriate non- SHG in these materials will be discussed. In the
linear optical (NLO) crystal, of an incident infra- following section, we will describe the most recent
red laser beam. For the green, Nd:YAG or results obtained in the generation of blue laser
Nd:YVO4 lasers emitting at 1064 nm (4 F3=2 ! emission in Nd:GdCOB either by self-frequency
4
I11=2 Nd3 transition) with frequency doubling in doubling of the 4 F3=2 ! 4 I9=2 Nd3 laser emission,
KDP, LBO or KTP are commercially available. or by self-SFM of the 812 nm Ti:sapphire pump
For the blue, an ecient way is to use SHG of a and 1090 nm Nd3 laser emission. At last a brief
diode pumped Nd:YAG laser emitting at 946 nm summary of the laser properties of ND:YCOB,
(4 F3=2 ! 4 I9=2 Nd3 transition) [5,6]. One must another member of the RECOB family, will be
also mention the sum frquency mixing (SFM) of given.
the 1064 nm laser beam, produced by a neodymi-
um-doped crystal, and the pump laser beam at
800 nm in a suitable NLO crystal such as KTP 2. Infrared laser emission in Nd:GdCOB
[7] or KNbO3 [8].
Some of these systems cannot be diode pumped, One of the main advantages of the (RECOB),
or are poorly ecient. The GaN laser diode use (RE Gd, Y) materials with respect to other NLO
will be restricted to applications in which the laser borates like BBO and LBO is that they can be
beam quality requirement is not too stringent. grown in the form of large single crystals from the
Concerning the other processes, one must point melt, using the Czochralski pulling method [10,13].
out that they require both a laser and a NLO For GdCOB, a survey of the NLO properties can
crystal, each of them being cut in appropriate be found in [10,14] while its structural and thermal
orientation, polished and antireection coated. characteristics are reported in [15]. Since the
In this paper, particular emphasis will be laid on Ca4 ReB3 O10 phase exists for RE Nd as well as
the self-frequency doubling and self-sum frequency Gd and Y [16], it is possible to grow single crystals
mixing processes which have been demonstrated in of Nd:Ca4 ReB3 O10 , RE Gd, Y in which a large
Nd:Ca4 GdB3 O10 (Nd:GdCOB) crystals. Nd3 ions amount of RE is replaced by Nd3 . Due to the self-
are used to produce laser emission through the quenching of the Nd3 uorescence [17], we re-
four levels 4 F3=2 ! 4 I11=2 or three levels strict ourselves to a 10% doping rate in the molten
4
F3=2 ! 4 I9=2 channels, while the GdCOB matrix, bath, leading to 7% Nd3 in the crystal for
which possess an outstanding set of linear and Nd:GdCOB. Absorption, uorescence and uo-
non-linear optical properties [9,10] acts as an in- rescence decay measurements allows to calculate
ternal SHG or SFM medium. It follows that green the absorption and emission cross-section with
and blue coherent radiation are produced within polarization along the three principal crystallo-
only one crystal. Such processes have already been graphic directions of the monoclinic crystal struc-
demonstrated in several NLO crystals, among ture (space group Cm, Z 2). These values,
which the most ecient is Nd:YAl3 (BO3 )4 together with the uorescence lifetime at very low
(NYAB). Under diode pumping [11] this material Nd3 concentration (1019 ions/cm3 ) and the u-
produces 160 mW output in the green by self-fre- orescence branching ratio are gathered in Table 1.
quency doubling and a few mW of 460 nm light For the laser measurements at 1.06 lm, two
by self-SFM under titaniumsapphire laser cubes of Nd:GdCOB doped with 7% and 5%
pumping [11,12]. However, this material has a Nd3 nominal (giving respectively, 5% and 4%
D. Vivien et al. / Optical Materials 16 (2001) 213220 215

Table 1 Table 2
Parameters related to laser action in Nd:GdCOB [17]a Laser performances of Nd 7%:GdCOB under Ti:sapphire
Polarization re ra bJ % s ls pumping at 812 nma
20
10 cm2 10 20
cm2 Pump Slope Laser threshold Output beam
X 4.2 2.3 52 (9/2) direction eciency% (mW) polarization
Y 2.1 1.6 41 (11/2) 98 X 29 288 E//Z
Z 1.9 1.7 7 (13/2) Y 34 90 E//X
a
X, Y, Z are the optical indicatrix directions of the GdCOB Z 29 210 E//X
a
crystal. re the emission cross-section at 1061 nm, ra the 812 nm X,Y, Z are the crystal optical indicatrix directions. The output
absorption cross-section, b the branching ratio for the transi- mirror transmission was either 2% or 4%.
tion 4 F3=2 ! 4 IJ and s the neodymium uorecence lifetime at
very low Nd3 concentration.
1) with a slope eciency and laser threshold of
45% and 90 mW, respectively. Compared to a
Nd3 in the crystal) are cut and polished from Nd:YAG crystal tested in the some cavity, the
the Czochralski boules. Then edges (8 mm) are slope eciency is very similar but the laser
parallel to the three principal axis X, Y and Z. threshold is much higher. This is explained by
Laser tests are performed in a plano-concave the larger uorescence lifetime (250 ls) and
cavity under pumping with a Ti:sapphire laser higher stimulated emission cross-section 6:5
tuned to the absorption maximum of 10 19 cm2 of Nd:YAG compared to
Nd:GdCOB at 812 nm. Laser action is obtained Nd:GdCOB.
for pumping the 5% doped cube along the three When performing the self-frequency doubling
principal directions (Fig. 1). The slope eciency experiments, under diode pumping that will be
and laser threshold are reported in Table 2. reported later, it was found that two wavelengths:
Pumping along Y gives the best results with 34% 1060 and 1091 nm occur simultaneously in the IR
slope eciency. For this direction the 4% laser beam which escape through the output mir-
Nd:GdCOB cube gives even better results (Fig. ror of the cavity [18]. The amount of 1091 emission

Fig. 1. Laser performance (4 F3=2 ! 4 I11=2 transition) of Nd:GdCOB according to the direction of the Ti:sapphire pump beam, for
nominal neodymium content of 7% and 4%.
216 D. Vivien et al. / Optical Materials 16 (2001) 213220

Fig. 2. (a) Inuence of the crystal temperature on the laser power emitted at 1060 and 1091 nm. (b) Part of the Nd3 :GdCOB energy
level diagram indicating the origin of the 1060 and 1091 nm laser emissions.

increases when the pump power and the laser found polarized along Y (Table 2), we decided to
crystal temperature increase (Fig. 2(a)). This can cut the crystal for self-frequency doubling exper-
be understood when considering the Nd3 :GdCOB iments according to the phase matching condition
energy level diagram (Fig. 2(b)) which shows that in the XY plane h 90, / 46 although the
the short wavelength emission originates from the deff NLO coecient for SHG is only 0.5 pm/V
lowest Kramers doublet of the 4 F3=2 state and the (instead of 1 pm/V in the XZ plane). The self-
long wavelength beam from the highest one. frequency doubling emission in the green was
Therefore, a higher crystal temperature favors the reported for the rst time in 1997 [17] using a 8
1091 nm emission through Bolzmann population mm long 4% doped GdCOB crystal cut in the
equilibrium. This also indicates that the gain cross- above-mentioned orientation. Successive optimi-
section is higher at 1091 nm than at 1060 nm since zation of the laser cavity set up and antireection
at 55C, when the power emitted at the two coating of the crystal at the IR and green wave-
wavelengths are identical, only 30% of Nd3 ex- length allowed to reach 64 mW of green output
cited ions are in the highest 4 F3=2 Kramers doublet. at 530.5 nm for 1 W of absorbed pump power
under Ti:sapphire pumping at 812 nm [19].
However, the most signicant improvement arose
3. Green laser emission by self-frequency doubling in from the replacement of the Ti:sapphire laser by
Nd:GdCOB a SDL laser diode having a maximum output
power of 2 W at 810 nm, from a 1  100 lm2
Owing to the properties of Nd:GdCOB re- single stripe. The experimental set-up is depicted
ported above, it was tempting to try to combine in Fig. 3. The best performances were obtained
the infrared laser emission originating from Nd3 using a 7% Nd doped crystal, giving 115 mW of
ions with the NLO properties of the GdCOB green emission for 1.3 W of absorbed pump
matrix. Second harmonic generation (SHG) of an power [18]. As expected, the output power goes
infrared laser beam at 1.06 lm can be achieved quadratically with the pump power. The green
with GdCOB using type I phase matching in the wavelength emitted shifts from 530 nm at low
XY and XZ principal planes [10]. However, since pump power to 545 nm for higher one as an
the laser emission of Nd:GdCOB was never image of the IR laser emission wavelength. It was
D. Vivien et al. / Optical Materials 16 (2001) 213220 217

Fig. 3. Experimental set-up for laser self-frequency doubling experiments in the green. The Nd:GdCOB crystal is cut for type I phase
matching in the XY plane. The afocal is a 6 expander in the direction of the laser diode junction.

easy to obtain the highest output power at each rather low emission cross-sections, at most
wavelength by simply turning the crystal since the 0:54  10 20 cm2 for Z polarization.
/ angles for phase matching at the two wave- For self-frequency doubling experiments, a 4%
lengths dier by only 2. Nd:GdCOB crystal (10 mm long) is cut according
to the phase matching condition at 936 nm in the
XY plane h 90, / 59. At rst, we try to
observe laser emission under CW Ti:sapphire
4. Blue laser emission from Nd:GdCOB pumping, but no infrared or blue light could be
produced at the maximum pumping power (1 W)
In principle, the easiest way to generate a blue available at 812 nm with our equipment. This is
laser beam from a Nd3 doped crystal is the SHG understandable if one compares with a Nd:YAG
of the 4 F3=2 ! 4 I9=2 quasi-three-levels laser tran- crystal whose emission cross-section at the laser
sition. The corresponding uorescence spectrum wavelength (946 nm) is one order of magitude
for Nd:GdCOB is given in Fig. 4. This material is higher than for Nd:GdCOB. Furthermore, the
expected to lase on the highest level of the 4 I9=2 terminating level of Nd:YAG emission is at
ground state, situated at 662 cm 1 , which is the 857 cm 1 from the 4 I9=2 ground state Kramers
lowest thermally populated one [20]. This corre- doublet, it means 200 cm 1 higher than in
sponds to the 936 nm line in Fig. 4, which exhibits Nd:GdCOB.

Fig. 4. Emission spectrum (Z polarization) of Nd:GdCOB corresponding to the 4 F3=2 ! 4 I9=2 transition.
218 D. Vivien et al. / Optical Materials 16 (2001) 213220

Then we decided to use a pulsed Ti:sapphire


laser (7 mJ, 100 ns) as the pump source. The laser
cavity has an output mirror highly reective at 936
nm while both cavity mirrors exhibit high trans-
mission in the blue. With this experimental set-up,
we do observe self-frequency doubling at 468 nm
[20] with a quadratic dependence of the output
energy with respect to the absorbed pump one, as
expected for a second-order NLO process. The
maximum energy per pulse was 0.27 mJ for 4.9 mJ
of absorbed pump, which corresponds to an op-
tical to optical eciency of 5.5%.
Another way to achieve laser emission in the
blue with Nd:GdCOB was explored. This is the Fig. 5. Output power at 465 and 1090 nm for Nd:GdCOB in a
self-sum-frequency-mixing of the pump and Nd3 self-sum-frequency-mixing experiment under 812 nm Ti:sap-
laser emission. This eect has been demonstrated phire laser pumping. The solid lines are quadratic and linear
ts, respectively.
recently in the neodymium-doped borate NYAB.
The laser emission at 1062 nm and the pump laser
beam (originating from a pulsed tunable dye laser) By varying the pump wavelength around 812
can be summed in properly oriented NYAB crys- nm, a few nanometers tunability of the blue beam
tals to give either blue [21] or UV [22] coherent (459466 nm) is obtained [23]. At last, by replacing
light beams, depending upon the particular neo- the Ti:sapphire pump by a 2 W high brightness
dymium absorption band which is pumped. laser diode at 812 nm, 100 lW of 465 nm blue laser
For such experiments in Nd:GdCOB, but under emission was obtained [24]. To our knowledge, it is
CW laser pumping, two crystals 8 and 5 mm in the rst time that self-sum-frequency-mixing under
length, containing respectively, 5% and 7% Nd3 diode pumping is reported.
ions, are cut for type I SFM in the XY plane and
antireection coated for the blue and infrared. The
orientation corresponds to (h 90, / 60) for a 5. Laser emissions from Nd:YCOB
pump at 812 nm and a laser emission at 1060 nm.
However, tuning of the crystal for pump excitation The crystal growth of Ca4 YB3 O10 (YCOB) was
between 720 and 840 nm is possible by rotating the rst reported in 1997 by the group of Sasaki and
crystal in the XY plane so that / angle is varied co-workers [13], although unpublished results ob-
from 69 to 58. Placed in a cavity whose mirrors tained in our laboratory [25] have demonstrated
are both highly reective at 1060 nm and exhibit a earlier that it was possible to obtain single crystals
high transmission in the blue, a strong blue laser of YCOB by the Czochralski pulling method.
emission is observed with both crystals under CW Compared with GdCOB, YCOB is slightly
Ti:sapphire pumping [23]. The highest doped more birefringent so that SHG is possible for
crystal gives the best result, with about 1.2 mW at shorter wavelength: 720 nm against 840 nm for
465 nm (Fig. 5). This proves that the IR laser GdCOB. Furthermore SHG of a Nd:YAG laser
wavelength mixed with the pump is 1091 nm rather beam at 1064 nm is possible using both type I and
than 1060 nm [24]. Simultaneously, despite the type II phase matching (type I only for GdCOB)
high reection of the output mirror in the IR, and 1064 nm + 532 nm sum-frequency mixing
about 70 mW of 1090 nm light escape through it (``frequency tripling'') is achievable in YCOB [13].
for an absorbed pump power of 430 mW (Fig. 5). Otherwise, the properties of GdCOB and YCOB
This indicates that improvement of the eciency are very similar. Recently [26], we have redeter-
of this blue laser, equal to 0.28% at the moment, is mined the refractive indexes and phase matching
possible. conditions for YCOB.
D. Vivien et al. / Optical Materials 16 (2001) 213220 219

4
The infrared laser performance of Nd:YCOB I9=2;11=2;13=2 channels) is coupled to quadratic NLO
was studied by Mougel [14] in a similar way than properties of the matrices. This gives emissions in
for Nd:GdCOB, as reported in Section 2. The laser the blue, green and red, respectively, with only one
emission, under Ti:sapphire pumping, occurs at crystal. Usually such laser beams need two crystals
1060.5 nm whatever is the pump power. The slope to be generated: one for producing the funda-
eciencies of the IR laser emissions for the pump mental laser emission and the second for SHG or
beam propagating along X, Y and Z are very SFM, both crystal needing to be oriented, cut,
similar (3942%). However, the laser threshold is polished and antireection coated. This is obvi-
signicantly smaller along Y indicating that, like ously more complicated and expensive.
for Nd:GdCOB (Table 2), this is the best pumping Nd:GdCOB, which has produced up to 115
direction. Other authors [27] have reported similar mW by self-frequency doubling under laser diode
experiments in which Nd:YCOB is pumped at 794 pumping may already be of commercial interest.
nm by means of a Ti:sapphire laser. They obtained Further studies are in progress in order to in-
68 mW of infrared emission for 311 mW of ab- vestigate the possibility to use phase matching
sorbed pump power and a laser threshold of 163 orientations outside of the principal planes. Ac-
mW. The slope eciency reaches 47%. Under high cording to Lu et al. [31] the direction (h 66:3,
brightness AlGaAs diode pumping at 812 nm, 340 / 134:4) is ve times more ecient than the one
mW of 1.06 lm light is produced for 900 mW of used until now (h 90, /  46) for SHG in
incident pump power (51% slope eciency) [28]. GdCOB. We are also currently investigating the
Self-frequency doubling experiments in Nd: possibility to make diode pumped microchips
YCOB was rst investigated on single crystals green lasers using self-frequency doubling in 1 or 2
grown in Cha laboratory [28,29]. Using a Nd:Y- mm thick Nd:GdCOB crystals.
COB crystal (5% doped) cut for phase matching at
1.06 lm in the XY plane, 62 mW of green laser
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