Broadly tunable infrared parametric oscillator using AgGaSe2

R. C. Eckardt, Y. X. Fan, R. L. Byer, C. L. Marquardt, M. E. Storm, and L. Esterowitz

Citation: Applied Physics Letters 49, 608 (1986); doi: 10.1063/1.97055
View online: http://dx.doi.org/10.1063/1.97055
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infrared parametric oscillator using AgGaSe2
R. C. Eckardt, Y. X. Fan, and R. L. Byer
Applied Physics Department, Stanford University, Stanford, California 94305
C. L. Marquardt, M. E. Storm,a) and L. Esterowitz
Naval Research Laboratory, Washington, DC 20375
(Received 30 June 1986; accepted for publication 21 JUllY 1986)
The first successful operation of a AgGaSe
1
infrared parametric oscillator is reported.
Continuous tuning ranges of 1.6-1.7 f-lm, 6.7-6.9 f-lm, and 2.65-9.02 f-lm were achieved using
1.34-f-lm neodymium and 2.05-f-lm holmium pump lasers. Pulse energies exceeding 3 mJ, peak
powers near 100 kW, and conversion efficiencies of 18% were obtained. Operation of the
parametric oscillator was possible well below the 13-40 MW /cm
2
surface damage threshold of
this nonlinear material.
We report the first successful operation of a silver selen-
ogallate (AgGaSe
z
) infrared optical parametric oscillator
(OPO). Tuning ranges of 1.6-1.7 f-lm and 6.7-6.9 f-lm were
demonstrated using a 1.34-f-lm neodymium-doped yttrium
aluminum garnet (Nd:YAG) pump laser. Continuous tun-
ing between 2.65 and 9.02 f-lm was obtained using a 2.05-f-lm
holmium-doped lithium yttrium fluoride (Ho:YLF) pump
laser. Pump powers up to five times OPO threshold were
employed without damage to the AgGaSe
2
crystal. OPO
output energies exceeding 3 mJ (8 X 10
16
photons) per pulse
at 4.8 f-lm were achieved with the Ho:YLF pump laser, cor-
responding to peak power of 90 kW and conversion effi-
ciency of 18%. Peak power of 30 kW and conversion effi-
ciency of 18% were also obtained at 1.66 f-lm using the
Nd:YAG pump. An optimally designed AgGaSe
z
OPO
pumped by a 2.05-f-lm laser should be continuously tunable
from about 2.5 to 12 f-lm.
Parametric oscillators provide a convenient method of
generating tunable radiation over broad spectral ranges, but
utilization of this technique outside the visible region has
been hampered by the lack of suitable optical materials. I The
only nonlinear material previously available in sufficiently
high optical quality to function as an OPO in applications
such as infrared spectroscopy and remote sensing has been
LiNbO
j

2
However, the tuning range of a LiNb0
3
OPO is
fundamentally limited to wavelengths shorter than 4.4 f-lm
because of intrinsic absorption of the material. AgGaS
2
,
AgGaSe
z
' Tl,AsSe" and CdSe are some of the most promis-
ing nonlinear materials for use as OPO's at longer wave-
lengths. CdSe has been operated as an infrared OPO over
limited tuning ranges, but broadband continuous tuning is
not possible in this material because of phase matching limi-
tations.
3
Large single crystals ofTl
3
AsSe, have recently been
grown for use in second harmonic generation of lO-f-lm CO
2
laser radiation; use of these crystals for parametric oscilla-
tion is being considered.
4
Recent improvements in the
growth oflarge high quality single crystals of ternary chalco-
pyrites have led to demonstrations of infrared parametric
generation in AgGaS
z
,5.6 and efficient doubling of 1O-f-lm
CO
2
laser radiation in AgGaSez-' The present letter reports
the first demonstration of an infrared OPO using AgGaSe
z
.
Parametric oscillation was achieved using two different
lasers as pump sources: a Nd:Y AG laser operated at 1.34f-lm
., Sachs/Freeman Associates, Landover, MD 20785.
and a Ho:YLF laser operated at 2.05 f-lm. Both lasers pro-
vided linearly polarized Q-switched pulses in a nominal
TEMoo mode. Spatial profiling with a scanning slit con-
firmed that the pump beams followed Gaussian distributions
within 5% in power density. The 1.34-Jim Nd:YAG laser
was operated at 10Hz, with typical pulse energy of 5 mJ and
pulse width of 23 ns. The pulse repetition frequency of the
2.05-f-lm Ho:YLF laser could be varied continuously
between 1 and 50 Hz with typical pulse energy of 30 mJ and
pulse width of 50 ns. Pump energy incident on the OPO was
selected by means of optical attenuators. Coaxially pumped,
singly resonant parametric oscillator configurations were
used with both pump wavelengths. For Nd:YAG pumping,
the OPO cavity consisted of two flat mirrors separated by
approximately 3 cm. The input mirror had a reflectance of
greater than 98% over the range 1.5-1.7 f-lm; the output
mirror had reflectance - 52 % over the same wavelength
range. Both cavity mirrors had reflectances less than 2% at
the 1.34-f-lm pump wavelength. Collimated pump light hav-
ing a beam diameter -0.7 mm was introduced through the
high reflectance mirror without focusing.
Two OPO cavity configurations were used with the
Ho:YLF pump laser. An unfocused configuration similar to
that described above for the Nd:YAG pump employed two
flat mirrors separated by about 5.3 cm. Collimated pump
radiation at 2.05 f-lm wavelength and a beam diameter of 1.8
mm was introduced into this cavity through the high reflec-
tance mirror. A focused configuration was also used, in
which the pump beam was focused prior to introduction into
the cavity in order to more nearly match the pump beam to
the spatial mode of a plano-convex OPO resonator. In the
plano-convex resonator, the high reflectance mirror had a
lO-m radius of curvature and the output coupler was flat.
The high reflectance mirrors used in both configurations had
reflectance greater than 98% over the range 2.9-4.1 f-lm.
Two output couplers, having reflectances of 65% and 80%
over the same wavelength range, were used in both configu-
rations. Parametric oscillation was observed in both configu-
rations and with both output couplers.
All AgGaSe
2
crystals used in these experiments were
grown at the Stanford University Center for Materials Re-
search as described previously. 7 The crystal used in the
Nd:YAG-pumped OPO (crystal No.1) was lOx lOX20
mm long and cut for type I phase matching over the 77_90
range. Both end surfaces were dielectric coated with ThF 4
608 Appl. Phys. Lett. 49 (11),15 September 1986 0003-6951/86/370608-03$01.00 @ 1 986 American Institute of Physics 608
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broadband antireflection (AR) coatings centered at 1.6pm.
The two crystals used for the Ho:YLF-pumped OPO were
both cut to al10w type I phase matching to a 2.0S-pm pump
over the range 43.3-49.8. One of these crystals (crystal No.
2; lOX lOX 18 mm long) was AR coated between 2.4 and
4.0 pm. However, subsequent reflection and transmission
measurements revealed that crystal No. 2 had bulk losses
throughout the mid-infrared region exceeding 30% per pass,
presumably due to internal scattering. The other crystal
(crystal No. 3; lOX lOX21 mmlong) had bulk lossesofless
than 2% per pass. OPO experiments were first performed on
this uncoated crystal, and then repeated after the application
of a broadband AR coating. Tunable OPO output was ob-
tained from aU AgGaSe
z
crystals in spite of the large intraca-
vity losses in crystal No.2 and the uncoated crystal No.3.
Damage thresholds were determined by SUbjecting coat-
ed and uncoated "companion" samples, cut from adjacent
portions of the AgGaSe
z
boule, to 100 laser shots at 10 Hz
and detecting damage by visual inspection. A Q-switched,
1.06-pm Nd:Y AG laser was used for damage measurements
on crystal No.1; the 2.05-pm Ho:YLF Jaser described
above, for crystals Nos. 2 and 3. In situ damage measure-
ments were also performed on crystal No.3 by intentionally
increasing the pump !power beyond the anticipated damage
limit during OPO operation. Damage thresholds for all sam-
ples fell in the range of 13-40 MW /cm
2
, the AR. coated sam-
ples generally having somewhat higher damage thresholds.
In all cases, including OPO operation, damage occurred first
on the entrance surface (facing the pump Jaser).
Angle tuning of the AgGaSe
2
OPO was achieved with
both 1.34- and 2.0S-pm pump wavelengths, and was charac-
terized by dispersing the OPO output in a 0.2S-m grating
spectrometer. The experimental results are shown in Figs. 1
and 2, together with tuning curves calculated from index of
refraction data
R
using Sell meier equations. In Fig. 2 the cal-
culated phase matching angles have been decreased by 0.7 in
order to obtain agreement between the shapes of the ca1cu-

10
E
::I... 8
:r:
r-
(!)
z
6 w
...J
W


4
2
60
AgGoSe2 OPO
TYPE I TUNING CURVE
>'p= I .34 J.Lm
70 80
PHASE MATCHING ANGLE (degrees)
90
FIG. I. Angle tuning of a singly resonant, AgGaSe2 OPO pumped by a Q-
switched, 1.34-,um Nd:Y AG laser. Solid lines are calculated tuning curves.
Data points were obtained from crystal No. 1 at laboratory ambient tem-
perature.
609 Appl. Phys. Lett .. Vol. 49. No. 11. 15 September 1986
12
AgGaSe2 OPO
TYPE I TUNING CURVE
E
10
Ap = 2.05 J.Lm
::I...
:r: 8
r-
(!)
z
w
6
...J
W
4
__ ___ ___
43 45 47 49
PHASE MATCHING ANGLE (degrees)
FIG. 2. Angle tuning of a singly resonant AgGaSe
2
OPO pumped by a Q-
switched 2.05-,um Ho: YLF laser. Solid line is the calculated tuning curve in
which all angles have been adjusted by O. T. Data points were obtained at
laboratory ambient temperature using crystal No.3 after AR coating.
lated and measured tuning curves. This adjustment is well
within the indeterminacy introduced by systematic errors in
crystal orientation and inaccuracies in the index of refrac-
tion data. In both Fig. I and Fig. 2, the observed tuning
ranges are considerably narrower than the potentially
achievable ranges derived from the phase matching condi-
tion and transparency of the material. The experimentally
observed wavelength range of the Nd:Y AG-pumped OPO
(Fig. 1) is restricted primarily by practical limitations of
angle tuning due to beam walk-off and geometrical factors.
For Ho:YLF pumping (Fig. 2) the tuning range of 2.6S-
9.02 pm for crystal No.3 with AR coating appears to be
limited only by the spectral reflectance of the OPO cavity
mirrors. In the present experiments there is no indication of
any material property of crystal No.3 which would preclude
tuning over the entire 2.S-12pm range. In the case of crystal
No.2 and the uncoated crystal No.3 the observed tuning
range was damage limited. High internal scattering losses of
crystal No.2 and Fresnel losses at the uncoated surfaces of
crystal No.3 restricted tuning to the range 3.3-5.6 pm. As
the OPO is tuned away from degeneracy the decrease in gain
eventually raises the OPO threshold above the damage
threshold. The presence of a large intracavity loss reduces
the effective gain by a constant term, thereby narrowing the
damage-limited tuning range. Elimination of these losses in
the cavity by AR coating crystal No.3 increased the tuning
range to 2.65-9.02 pm, limited by the spectral range of the
OPO mirrors.
Conversion efficiency and pulse shape measurements
were performed on the Ho:YLF-pumped OPO at a tuning
angleof49.2 (A.
p
= 2.05pm,A.s = 4.84pm,A., = 3.55I1m).
The pump, signal, or idler wave was selected using appropri-
ate bandpass filters; pu]se energy and temporal profile were
measured using a pyroelectric energy meter and a fast (3 ns
rise time) gold-doped germanium detector. Figure 3 shows
an example of conversion efficiency as a function of pump
energy for pump energies up to four times OPO threshold.
For the unfocused configuration the observed threshold
around 4 m] and the maximum conversion efficiency of 18%
are in reasonable agreement with calculated values.
6

9
Use of
the focused configuration lowered the energy threshold to
about 2.S mJ, but had little effect on the maximum conver-
sion efficiency. Saturation of the conversion efficiency curve
Eckardt et at. 609
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20

AgGoSe2 0PO

Ap = 2.05 fJ-m
>-
TUNING ANGLE =49
0
u
z
w
,./- u
l.L ", . .
l.L
10

w
z
,.
Q

U1
0::
W

>

z
0

u
0

0 5 10 15
PUMP ENERGY (mJ)
FIG. 3. Conversion efficiency, (E, + E, )/Ep, as a function of pump pulse
energy Ep for the singly resonant AgGaSe
2
OPO pumped by the 2.05,um
Ho;YLF laser. Measurements were made on crystal No.3 (AR coated), at
tuning angle of 49.2; A, = 4.84 ,urn; Ai = 3.55 ,um; Tp = 60 ns. The OPO
resonator is in the unfocused configuration with the R = 80% output
coupler. The solid line is a least-squares linear fit to the data points.
was not observed in either configuration and is expected to
lie above the damage threshold. In all measurements the ob-
served conversion efficiencies increased monotonically with
increasing pump power up to about six times threshold, as
expected for a Gaussian beam.1O At higher pump powers
damage was observed after a few hundred pulses indicating a
damage threshold of 25 MW Icm
2
at the crystal surface.
Pulse shapes of the signal, idler, and depleted pump
were measured at various conversion efficiencies for an input
pump pulse width of 50 ns. Signal and idler pulse widths
varied between 10 and 30 ns depending on conversion effi-
ciency. Pumping at five times the OPO threshold, which. is
still below the damage threshold, the AgGaSe
2
OPO deliv-
ered 90 kW peak power in the signal pulse (4.84,um) and
116 kW in the idler (3.55 ,urn).
Similar measurements performed on the Nd:Y AG
pumped OPO showed thresholds of 1-2 mJ the
range shown in Fig. 2. The maximum conversIOn effiCIency
of 18% was limited by available pump power rather than
damage or intracavity losses. The maximum pulse energy
produced in the idler wave was 0.3 mJ at 1.66 ,urn, corre-
sponding to idler and signal peak powers of 30 and 8 kW,
respectively.
The pulse energy, spectral content, and temporal
ofthc signal wave were examined for pulse-to-pulse stabIlIty
in the case of the Ho:YLF-pumped OPO. By pumping the
OPO at two to three times the threshold energy, the signal
energy reached a stability commensurate with the energy
stability of the pump laser. For example, with the pump en-
ergy optimally stabilized, at 8% conversion efficiency the
standard deviation in signal energy was about 11 %, as com-
pared with 5% for the pump laser. Spectral output and tem-
poral profile were found to be equaIly unstabl.e at all pump
energies below the damage llimit. Typical spectral output of
the signal wave consists of two or three lines separated by
about 10 cm I, each line having a spectral width around 10
cm I. When pumped with structureless single Q-switched
pulses, temporal profiles of the OPO signal wave usually
exhibited a multipulse structure, especially at high pump
610 Appl. Phys. Lett., Vol. 49, No. 11, 15 September 1986
energies. The shot-to-shot variations in temporal profile and
spectral content of the signal pulse appear to be consistent
with known bandwidth instabilities in the Ho:YLF pump
laser. II No attempt was made to eliminate these instabilities
during these preliminary investigations,
The spatial distributions of the Ho:YLF-pumped OPO
outputs were determined for both focused and unfocused
configurations using a linear pyroelectric array wi th l00-,um
resolution. In both cases the signal and idler beams had
Gaussian-like distributions and could be focused to near-
diffraction-limited spots having diameters less than 50,um.
However, the measured beam widths for the focused config-
uration indicated that the actual OPO cavity mode was sig-
nificantly smaller than the focused pump beam widths. Thus
the conversion efficiency attained in the focused configura-
tion is probably reduced by overfilling the cavity mode with
the pump laser. It may be possible to obtain a significant
increase in the OPO efficiency by using larger, higher quali-
ty, AR-coated AgGaSe
2
crystals in a focused configuration
in which the pump laser is optimally matched to the cavity
mode.
In summary, we have demonstrated the first successful
operation of a AgGaSe
2
infrared OPO. Continuous tuning
ranges of 1.6--1.7 ,urn and 6.7-6.9,um were achieved using a
1.34-,um Nd: Y AG pump laser. A continuous tuning range of
2.65-9.02,um was demonstrated using a 2.05-,um Ho:YLF
pump laser, and there appears to be no material-imposed
limitation precluding tuning over the entire predicted range
of 2,5-12 ,urn. Pulse energies exceeding 3 mJ and peak pow-
ers near 100 kW were obtained in Gaussian-like signal and
idler waves, Conversion efficiencies as high as 18% were
demonstrated. Some of the results were limited by the sur-
face damage thresholds of the AgGaSe
2
crystals, which were
in the range 13-40 MW / cm
2
Substantial increases in damge
resistance, output power, and conversion efficiency should
be attainable by improvements in AgGaSe
2
crystal growth
and surface coating, and by optimization of the OPO pump-
ing configuration.
The authors wish to acknowledge the contributions of
R. K. Route and R. S. Feigelson who provided the AgGaSe
2
crystals. The Stanford University contribution to this work
was supported in part by the U.S. Army Research Office and
the Office of Naval Research.
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Eckardt et al. 610
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