Properties of Nd3+-doped and undoped tetragonal PbWO4, NaY(WO4)2, CaWO4, and undoped monoclinic ZnWO4 and CdWO4 as laser-active and stimulated Raman scattering-active crystals
Alexander A. Kaminskii, Hans J. Eichler, Ken-ichi Ueda, Nikolai V. Klassen, Boris S. Redkin, Ludmila E. Li, Julian Findeisen, Daniel Jaque, José García-Sole, Joaquín Fernández, and Rolindes Balda
Alexander A. Kaminskii,
Hans J. Eichler,
Ken-ichi Ueda,
Nikolai V. Klassen,
Boris S. Redkin,
Ludmila E. Li,
Julian Findeisen,
Daniel Jaque,
José García-Sole,
Joaquín Fernández,
and Rolindes Balda
A. A. Kaminskii and L. E. Li are with the Institute of Crystallography, Russian Academy of Sciences, 117333 Moscow, Russia.
H. J. Eichler and J. Findeisen are with the Optisches Institut, Technische Universität Berlin, D-10623 Berlin, Germany.
K. Ueda is with the Institute for Laser Science, University of Electro-Communications, 182 Tokyo, Japan.
N. V. Klassen and B. S. Redkin are with the Institute of Solid-State Physics, Russian Academy of Sciences, 142432 Chernogolovka, Moscow Region, Russia.
D. Jaque and J. García-Sole are with the Departamento de Fisica de Materials C–VI, Universidad Autonoma de Madrid, Cantoblanco, 28049 Madrid, Spain.
J. Fernandez and R. Balda are with the Departamento de Fisica Aplicada I, Escuela Tecnica Superior de Ingenieros, Universidad del Pais Vasco, Avda, Urquijo s/n 48013 Bilbao, Spain.
Alexander A. Kaminskii, Hans J. Eichler, Ken-ichi Ueda, Nikolai V. Klassen, Boris S. Redkin, Ludmila E. Li, Julian Findeisen, Daniel Jaque, José García-Sole, Joaquín Fernández, and Rolindes Balda, "Properties of Nd3+-doped and undoped tetragonal PbWO4,
NaY(WO4)2, CaWO4, and undoped monoclinic
ZnWO4 and CdWO4 as laser-active and stimulated Raman
scattering-active crystals," Appl. Opt. 38, 4533-4547 (1999)
Spectroscopic, laser, and χ(3)
nonlinear optical properties of tetragonal PbWO4,
NaY(WO4)2, CaWO4, and
monoclinic CdWO4 and ZnWO4 were
investigated. Particular attention was paid to
Nd3+-doped and undoped PbWO4 and
NaY(WO4)2 crystals. Their absorption
and luminescence intensity characteristics, including the peak cross
sections of induced transitions, were determined. Pulsed and
continuous-wave lasing in the two 4F3/2→ 4I11/2 and
4F3/2 →4I13/2 channels was excited. For
these five tungstates, highly efficient (greater than 50%)
multiple Stokes generation and anti-Stokes picosecond generation were
achieved. All the observed scattered laser components were
identified. These results were analyzed and compared with
spectroscopic data from spontaneous Raman scattering. A new
crystalline Raman laser based on PbWO4 was developed for
the χ(3) conversion frequency of 1-µm pump
radiation to the first Stokes emission with efficiency up to
40%. We classify all the tungstates as promising media for lasers
and neodymium-doped crystals for self-stimulated Raman scattering
lasers.
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Generation of SE was discovered and
characterized in our previous investigations; see, for example, Refs.
2, 6, 7, and 12–14.
Investigated in this study.
Table 2
SRS-Active Molybdate and Tungstate Crystals for Raman
Shifters and Self-SRS Lasersa
Refs. 3-8.
For Ln3+ lasing ions see Table 1.
In monclinic crystals
( and
) tungstate octahedron units form
dimer structures (chains, ribbons, etc).
In Ref. 9, 889
cm-1 for KGd(WO4)2 and 901
cm-1 for KY(WO4)2.
In Ref. 10, 911
cm-1 was indicated as an unpublished result.
For determination of the intensity of RT
absorption line strengths for intermanifold
4I9/2 → J′ transitions and
luminescence 4F3/2 →4IJ′
channels, as well as intensity
parameters Ωt, spectroscopic quality parameter
X =
Ω4/Ω6,28,29 radiative
lifetime τrad of the
4F3/2 state, and intermanifold
luminescence branching ratios βJJ′ of
Nd3+ ions in tetragonal PbWO4 crystals.
Data from Ref. 30.
The anisotropy of the PbWO4 crystal
was considered.
Root-mean-square deviation is δ =
0.17 × 10-20 cm2.
The lifetime of metastable
4F3/2 state for PbWO4,
as well as for NaY(WO4)2 crystal has been
measured at low Nd3+ content
(CNd ≈ 0.3 at. %) for which
luminescence concentration quenching was practically absent. This value
is equal to 180 ± 20 µs for disordered tungstate.
Temperature measurements showed that the quantum yield of the
4F3/2 →4IJ′
luminescence is equal to 1, which
means that τrad ≈ τlum for both
crystals.
SE generation
(4F3/2 →4I11/2 and
4F3/2 →4I13/2 channels) as well as effective
peak cross sections of laser transitions of Nd3+ ions in
tetragonal PbWO4 and NaY(WO4)2
single crystals at room temperature.
Measurement accuracy is ±0.0003 µm.
With highly reflecting laser resonator mirrors
[see Fig. 4(a)].
With output laser resonator mirror having
≈2% transmission [see Fig. 4(b)].
SRS-active vibration modes and Raman gain
coefficients for tetragonal PbWO4,
NaY(WO4)2, and CaWO4, as well
as for monoclinic KGd(WO4)2 tungstates for
comparison.
The highest measured values in the visible.
Inhomogeneous-broadened line that is due to
crystal-structure disorders.
Table 7
Spectral Compositions of Multiple Stokes and Anti-Stokes
Generation and SRS-Active Optical Vibration
Modesa
For tetragonal ordered
PbWO4 and CaWO4 as well as for disordered
NaY(WO4)2 tungstates with a scheelite-type
structure and monoclinic ZnWO4 and CdWO4
crystals at RT under picosecond laser excitation at
λf1 = 1.06415 µm and
λf2(SHG) = 0.53207-µm wavelength.
Excitation and polarization directions are
given.
Measurement accuracy is ±0.0003 µm.
For example, the notation
St1-2ASt3-1 is defined as the
first Stokes component with the second vibration mode
ωR2 from the third anti-Stokes emission with
the first vibration mode ωR1.
See lines in Figs. 11–14.
In this pumping condition we also observed
coaxial ring Stokes generation by RFWM.
Tables (7)
Table 1
Known Molybdate and Tungstate Laser Crystals and Their
Generating Activator Ions
Generation of SE was discovered and
characterized in our previous investigations; see, for example, Refs.
2, 6, 7, and 12–14.
Investigated in this study.
Table 2
SRS-Active Molybdate and Tungstate Crystals for Raman
Shifters and Self-SRS Lasersa
Refs. 3-8.
For Ln3+ lasing ions see Table 1.
In monclinic crystals
( and
) tungstate octahedron units form
dimer structures (chains, ribbons, etc).
In Ref. 9, 889
cm-1 for KGd(WO4)2 and 901
cm-1 for KY(WO4)2.
In Ref. 10, 911
cm-1 was indicated as an unpublished result.
For determination of the intensity of RT
absorption line strengths for intermanifold
4I9/2 → J′ transitions and
luminescence 4F3/2 →4IJ′
channels, as well as intensity
parameters Ωt, spectroscopic quality parameter
X =
Ω4/Ω6,28,29 radiative
lifetime τrad of the
4F3/2 state, and intermanifold
luminescence branching ratios βJJ′ of
Nd3+ ions in tetragonal PbWO4 crystals.
Data from Ref. 30.
The anisotropy of the PbWO4 crystal
was considered.
Root-mean-square deviation is δ =
0.17 × 10-20 cm2.
The lifetime of metastable
4F3/2 state for PbWO4,
as well as for NaY(WO4)2 crystal has been
measured at low Nd3+ content
(CNd ≈ 0.3 at. %) for which
luminescence concentration quenching was practically absent. This value
is equal to 180 ± 20 µs for disordered tungstate.
Temperature measurements showed that the quantum yield of the
4F3/2 →4IJ′
luminescence is equal to 1, which
means that τrad ≈ τlum for both
crystals.
SE generation
(4F3/2 →4I11/2 and
4F3/2 →4I13/2 channels) as well as effective
peak cross sections of laser transitions of Nd3+ ions in
tetragonal PbWO4 and NaY(WO4)2
single crystals at room temperature.
Measurement accuracy is ±0.0003 µm.
With highly reflecting laser resonator mirrors
[see Fig. 4(a)].
With output laser resonator mirror having
≈2% transmission [see Fig. 4(b)].
SRS-active vibration modes and Raman gain
coefficients for tetragonal PbWO4,
NaY(WO4)2, and CaWO4, as well
as for monoclinic KGd(WO4)2 tungstates for
comparison.
The highest measured values in the visible.
Inhomogeneous-broadened line that is due to
crystal-structure disorders.
Table 7
Spectral Compositions of Multiple Stokes and Anti-Stokes
Generation and SRS-Active Optical Vibration
Modesa
For tetragonal ordered
PbWO4 and CaWO4 as well as for disordered
NaY(WO4)2 tungstates with a scheelite-type
structure and monoclinic ZnWO4 and CdWO4
crystals at RT under picosecond laser excitation at
λf1 = 1.06415 µm and
λf2(SHG) = 0.53207-µm wavelength.
Excitation and polarization directions are
given.
Measurement accuracy is ±0.0003 µm.
For example, the notation
St1-2ASt3-1 is defined as the
first Stokes component with the second vibration mode
ωR2 from the third anti-Stokes emission with
the first vibration mode ωR1.
See lines in Figs. 11–14.
In this pumping condition we also observed
coaxial ring Stokes generation by RFWM.