Lpor 200710008 PDF

Laser & Photon. Rev. 1, No. 2, 93–177 (2007) / DOI 10.1002/lpor.
200710008 93
Abstract After a brief examination of known insulating laser crys-

tals and the stimulated emission channels of their generating acti-
vator ions, this article reviews recent advances in the development
of novel lasing crystals and ceramics, as well as inorganic and or-
ganic nonlinear-laser crystals for χ(3) and cascaded χ(3) ↔ χ(2)
frequency converters. Several new modern attractive technologies
in the physics and techniques of crystalline lasers are also dis-
cussed.
Section of the crystal structure of Na3 Li(SeO4 )2 · 6H2 O, rep-

resenting one sheet of [Na3 O7 (H2 O)6 ] groups together with
the linking tetrahedral groups [SeO4 ] and the double tetrahedra
[O3 SeOLi(H2 O)3 ], that are formed by [SeO4 ] and [LiO(H2 O)3 ].
Hydrogen atoms are marked with spheres.
© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Laser crystals and ceramics: recent advances

Alexander A. Kaminskii*
Institute of Crystallography, Russian Academy of Sciences, 119333 Moscow, Russia
Received: 31 January 2007, Accepted: 25 February 2007

Published online: 3 May 2007
Key words: laser crystals; nonlinear-laser crystals; laser ceramics; crystalline lasers; Raman lasers; ceramic lasers; laser physics
PACS: 42.55.-f, 42.65.-k, 78.20.-e, 78.45.+h
1. Introduction crowave maser [3, 4], and when Schawlow and Townes
(1958) predicted the real possibility for the design of an
The development of the physics and technologies asso- optical maser (or laser) [5].
ciated with light waves has imperceptibly crossed the
threshold into the 21st century, and we have simultane- Nowadays, as in the past, crystalline lasers play a spe-
ously entered the fifth decade of the crystallline laser, cial role in modern laser physics, nonlinear optics, and
which, as is well known, originated from the work of quantum electronics [6]. The diverse structures and phys-
Maiman at the Hughes Research Labs, who in 1960 built ical properties of activated lasing crystals in combination
the world’s first working laser based on a synthetic ruby, with powerful and long-lived semiconductor laser diodes
Al2 O3 :Cr3+ [1]. Here we must note three previous impor- (LDs) as pumping sources have led to a veritable revolution
tant landmarks concerning the birth and growth of laser in the progress of solid-state laser (SSL) engineering. At
crystal physics: when Einstein (1916) realized the phys- present, this branch of the research and development of LD-
ical nature of stimulated emission (SE) [2], when Basov pumped crystalline lasers continues to grow very fast (see,
and Prokhorov independently and contemporaneously with e.g. [7–9]). Currently, highly transparent Nd3+ -, Er3+ -, and
Townes and co-workers (1954) developed the ammonia mi- Yb3+ -doped Y3 Al5 O12 , Y2 O3 , Sc2 O3 , and Lu2 O3 laser ce-
* e-mail: kaminalex@mail.ru
© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

94 A. A. Kaminskii: Laser crystals and ceramics: recent advances
ramics represent the rapid progress in quantum electronics and “fibres” (Sect. 9) which are presently already widely
and SSL materials science. New revolutionary technology, used in numerous modern laser technologies and applica-
developed by Japanese scientists (the vacuum sintering and tions are also discussed. All the above mentioned data on
nanotechnology (VSN) method [10]), makes it possible to laser and nonlinear-laser crystals and crystalline lasers are
obtain these laser ceramics with any required size and ac- summarized in tabular form.
tivator ion concentration, which correspondingly has al-
lowed the achievement of multi-kilowatt levels of continu-
ous wave (CW) Y3 Al5 O12 :Nd3+ laser output power with LD 2. Laser host crystals* and their generating
pumping at the one-micron lasing channel (4 F3/2 → 4 I11/2 ) lanthanide and transition metal ions
during the last several years [12,13]. The extremely active
interest in the study of nonlinear optical cascaded effects
(present status)
in χ(3) - and (χ(2) + χ(3) )-active crystalline materials can For the past four years following the publication of the
be accounted for by a number of practical reasons. So, ob- author’s last topical review [11, 18] the arsenal of known
served multiple Stokes and anti-Stokes equidistant lasing laser host crystals increased to about 18 new types and
coherent components covering very wide spectral regions presently there are more than 345 various names. Among
(in most cases more than 5000 cm−1 in the visible and near- them are different structure fluorides, oxides, chlorides,
IR) open up new promising possibilities for synthesis of bromides, and compounds with mixed anion pairs like
femtosecond waveforms (pulses). They are also very attrac- chlorine-oxygen, fluorine-oxygen, or sulphur-oxygen, as
tive for the creation of Raman laser converters with an effi- well as several nanocrystalline ceramics and semiconduc-
ciency of more than 50%, which can significantly enlarge tor hosts. They form, with known generating ions, over
the spectral range of SSLs and can compress their pulses 620 laser crystals and ceramics, which can produce CW or
(see, e.g. [11,14,15]). In the last few years, due to the results pulsed SE generation over a very wide spectral range from
of intensive research and improvements in crystals combin- ∼ 0.172 to ∼ 7.24 µm [11,18,19]. These crystals have been
ing both laser and these nonlinear optical properties, as well demonstrated to have laser application possibilities with
as the development of new methods of fabricating perfect the following lanthanide (Ln), actinide (Ac), and transition
single-crystal light-guiding structures, several promising metal (TM) ions, as well as a defect centre (d-c) (it is quite
ideas have emerged for the creation of new efficient crys- possible that the lasing defect centre in the Ca3 Ga2 Ge3 O12
talline lasers with self-frequency conversion phenomena, garnet crystal discovered in [22] is only an unidentified
namely self-frequency doubling (self-FD), self-stimulated TM activator, e.g. Fe3+ or genuine Cr4+ ion.): Ln3+ –Ce3+ ,
Raman scattering (self-SRS), self-pumped optical paramet- Pr3+ , Nd3+ , Sm3+ , Eu3+ , Tb3+ , Dy3+ , Ho3+ , Er3+ , Tm3+ , and
ric oscillation (self-pumped OPO), etc. Yb3+ ; Ln2+ –Sm2+ , Eu2+ , Dy2+ , and Tm2+ ; TM5+ –Mn5+ ;
The last decade of laser crystal physics development has TM4+ –Cr4+ ; TM3+ –Ti3+ and Cr3+ ; TM2+ –V2+ , Cr2+ , Fe2+ ,
featured a number of promising results and much research Co2+ , and Ni2+ ; Ac3+ –U3+ . As regards practicable crys-
activity. During this period the arsenal of laser host crystals talline lasers their number will be considerably more be-
and their generating activator ions has increased consider- cause the majority of Ln3+ materials can generate SE at the
ably. Over this time special attention also was paid to the wavelengths of several 4fN –4fN intermanifold J–J transi-
generation of Yb3+ and Cr2+ ions in different media, includ- tions. Laser host crystals are divided into two types accord-
ing semiconductor hosts (see, e.g. [16,17]). Efficient SE of ing to their spectroscopic and generating properties [20,21]:
crystals doped with these activator ions (lasants) is very simple ones having an ordered structure, mainly of a single-
attractive both for obtaining high-peak-power ultra-short centred type, and disordered multicentre compounds.
pulses, including femtosecond pulses, and for the creation
of broad-band tunable crystalline lasers emitting in useful
spectral regions. New visible and mid-IR laser channels of 2.1. Fluoride and oxide crystals with ordered
Pr3+ and Dy3+ ions were discovered, which has allowed
a new wide range of uses resulting from the continually and disordered structure
expanding scientific and technological frontiers of crys- In terms of the variety of SE-active activator ions (lasants)
talline lasers. the richest is the class of fluoride laser host crystals featur-
The main intention of this review is to present with max- ing an ordered structure (Tables 1 and 2), while those with
imum completeness published data on laser crystals and the most numerous and variable atomic structures is the
the intermanifold SE channels of their generating activator class of ordered oxide crystals (Tables 3 and 4). According
ions, as well as to present recent advances in the vigorously to Tables 5–7, the number of fluoride and oxide laser host
growing research on laser crystalline ceramics. These gen- crystals with a disordered structure is also large. Based on
eral topics are covered in Sects. 2–6. Another object is to investigations of these crystals, they have significant possi-
give new data on crystals for laser cascaded (SE → χ(2) ) and bilities for SE excitation in various lasing regimes. For in-
(SE → χ(3) ) nonlinear frequency converters, including self- stance, due to their satisfactory laser, thermal, and nonlinear
FD and self-SRS, as well as for self-pumped OPO (Sects. 7
*
and 8). Crystalline materials for a new generation of SSLs, This definition here and further the following is meant – laser
namely with LD pumping, as well as for laser waveguides single crystals and crystalline ceramics.
© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

Laser & Photon. Rev. 1, No. 2 (2007) 95
Table 1 Fluoride laser host crystals with ordered structure and their Ln3+ , Ln2+ , and Ac3+ lasants.
space Ln3+ Ln2+ Ac3+

host crystal group
Ce3+ Pr3+ Nd3+ Sm3+ Tb3+ Dy3+ Ho3+ Er3+ Tm3+ Yb3+ Sm2+ Dy2+ Tm2+ U3+
monoclinic crystals
LiKYF5 a) C2h 5 + +
LiKGdF5 C2h 5 +
β-BaY2 F8 C2h 3 + + + + + + +
β-Ba(Y,Er)2 F8 C2h 3 +
β-Ba(Y,Yb)2 F8 C2h 3 + + +
β-BaEr2 F8 C2h 3 + +
β-BaTm2 F8 C2h 3 +
β-BaYb2 F8 C2h 3 + + + + +
orthorhombic crystals
K2 YF5 C2v 9 +
K5 NdLi2 F10 D2h 16 +
BaMgF4 C2v 12 +
α-BaLu2 F8 D2h 16 + +
YF3 D2h 16 +
TbF3 D2h 16 +
HoF3 D2h 16 +
ErF3 D2h 16 +
tetragonal crystals
LiYF4 C4h 6 + + + + + + + + +
Li(Y,Er)F4 C4h 6 + +
Li(Y,Yb)F4 C4h 6 + +
Li(Y,Lu)F4 C4h 6 +
LiGdF4 C4h 6 + + +
LiTbF4 C4h 6 +
LiErF4 C4h 6 +
LiHoF4 C4h 6 +
LiYbF4 C4h 6 + + + +
LiLuF4 C4h 6 + + + + +
trigonal crystals
LiCaAlF6 D3d 2 +
Li(Ca,Sr)AlF6 D3d 2 +
LiSrAlF6 D3d 2 +
KYF4 D3 4 + + + + +
LaF3 D3d 4 + + + + +
CeF3 D3d 4 +
PrF3 D3d 4 +
hexagonal crystals
NaYF4 C3h 1 +
CsY2 F7 D6 6 +
CsGd2 F7 D6 6 +
cubic crystals
KY3 F10 Oh 5 + +
CaF2 Oh 5 + + + + + + d) + + + +
CaF2 (ceramic) Oh 5 b)
+
CaF2 c) Oh 5 + + + +
SrF2 Oh 5 + + + + + + + +
BaF2 Oh 5 + +
www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 1 (continued)
a)
Two types of LiKYF5 crystals are known, grown by the hydrothermal method [24–26] and by the Czochralski pulling
technique [27]. For Ln3+ lasing ions the former are single-centred crystals and the latter are two-centred fluoride hosts.
b)
Ceramic grains are nano- and (or) micrometre-sized single crystals.
c)
Crystals contained oxygen: in the table they introduced conditionally.
d)
For suppressing the formation of Yb2+ ions in [706] was grown laser crystals CaF2 :Na+ ,Yb3+ .
Table 2 Fluoride laser host crystals with ordered structure and 2.2. Anisotropic chloride, bromide, sulphide,
their TM3+ and TM2+ lasants. oxychloride, oxyfluoride, and oxysulphide, as
space TM3+ TM2+ well as II–VI and III–V semiconductor crystals
host crystal group
Cr3+ V2+ Co2+ Ni2+ Widening of the SE long-wavelength cut-off of Ln3+ crys-
talline lasers to the mid-IR region (now this point is in the
tetragonal crystals
∼ 7.24 µm region [41]) in most known cases bears an in-
MgF2 D4h 14 + + + timate relation to the use of crystals of ultra-low phonon
MnF2 D4h 14 + energy (usually less than 300 cm−1 ). Among these are pri-
ZnF2 D4h 14
+ marily chlorides and bromides (LaCl3 [42], PbCl2 [43],
SrAlF5 C4 5 + KPb2 Cl5 [44], LaBr3 [45], etc. (Table 8)). Taking into
account the fast-growing interest in the mid-IR SE laser
trigonal crystals sources based on Ln3+ ion-doped crystals for remote sens-
LiCaAlF6 D3d 2 + ing, trace gas monitoring, and medical applications, there is
Li(Ca,Sr)AlF6 D3d 2 + reason to believe that current active work in many laser ma-
2 terial science research centres will give rise to new lasing
LiSrAlF6 D3d +
compounds of this type. Table 8 also lists several laser crys-
LiSrCrF6 D3d 2 + tals with mixed anion pairs like chlorine-oxygen, fluorine-
LiSrGaF6 D3d 2 + oxygen, and sulphur-oxygen. Among them are the Yb3+ -
doped apatite structure family of crystals [48], Sr5 (PO4 )3 F,
cubic crystals
with unusually favourable laser gain characteristics that
Na3 Ga2 Li3 F12 Oh 10 + have been applied already in the development of a high-
1
KMgF3 Oh + + peak-power “Mercury” laser system for utilization in iner-
KZnF3 Oh 1 + + tial fusion energy production [49, 50].
CsCaF3 Oh 1 +
It is probable that II–VI semiconductors, namely ZnS,
ZnSe, CdTe, and others, are very suitable host crystals with
tetrahedrally coordinated sites for TM2+ ions (Table 9) that
can lase in the mid-IR region. In particular, these chalco-
genides doped with Cr2+ ions have already been shown to
produce highly efficient and broadly tunable SE in differ-
optical properties, characteristics of a number of disordered
ent lasing modes in the 2–3 µm spectral region [52–54].
cubic fluorides doped with Nd3+ ions, they are considered
As before, activated semiconductor crystals, especially of
as substitutes for neodymium glasses in high-power lasers,
the II–VI family, stimulate the imagination and foster cor-
including laser fusion driver systems (see, e.g. [37, 38]).
responding activity of researchers in the development of
There is good reason to believe that these crystals will be
SSLs with “electrical” pumping (see, e.g. [55]).
further developed, especially to fabricate large-size active
elements for powerful laser amplifiers with LD pumping.
Disordered Ln3+ -doped crystals with inhomogeneous 3. Spectral ranges of lasing activator ions
and very broad luminescence bands are extremely attrac-
tive for producing ultra-short laser pulses. For example, Triply and doubly ionized lanthanide ions, the most numer-
the creation of lasers with a combined active medium [39] ous family of activators for known laser crystals, permit one
(sometimes also termed “hybrid” lasers) based on dissimi- to excite CW and pulsed SE generation over a very wide
lar disordered crystals with the same or different SE-active spectral range from vacuum UV to mid-IR at the wave-
Ln3+ ions (in particular, one-micron generating Nd3+ and length of numerous inter-Stark transitions (already more
Pr3+ or Nd3+ and Yb3+ , as well as Er3+ and Ho3+ activa- than 1000, see also [19]) of 85 4fN –4fN and 4fN −1 5d1 –
tors) makes it possible to obtain super-wide laser gain con- 4fN inter- and intraconfiguration channels. Presently, the
tours [40] (even substantially above 1000 cm−1 ) essential total number of intermanifold and interconfiguration tran-
for the generation of femtosecond pulses. sitions of Ln, Ac, and TM lasing ions is 101 (Table 10).

Table 3 Oxide laser host crystals with

space Ln3+
host crystal ordered structure and their Ln3+ lasants.
group
Pr3+ Nd3+ Eu3+ Dy3+ Ho3+ Er3+ Tm3+ Yb3+
monoclinic crystals
Li6 Y(BO3 )3 C2h 5 + +
LiPrP4 O12 C2h 6 +
LiNdP4 O12 C2h 6 +
LiBiP4 O12 C2h 6 +
NaNdP4 O12 C2h 5 +
α-KY(WO4 )2 C2h 6 + + + + + + +
KNdP4 O12 C2 2 +
KGd(PO3 )4 C2 2 +
α-KGd(WO4 )2 C2h 6 + + + + + + +
α-KEr(WO4 )2 C2h 6 +
α-KYb(WO4 )2 C2h 6 + +
α-KLu(WO4 )2 C2h 6 + + + + + +
CaAl4 O7 C2h 6 + +
Ca3 (VO4 )2 C2h 6 +
Ca4 Y(BO3 )3 O Cs 3 + +
Ca4 Gd(BO3 )3 O Cs 3 + + +
Sc2 SiO5 C2h 6 + +
Sc2 Si2 O7 C2h 3 +
RbNd(WO4 )2 C2h 6 +
SrAl4 O7 C2h 6 +
Y2 SiO5 C2h 6 + + + + +
a)
YP5 O14 C2h 6 + +
j)
BaGd2 (MoO4 )4 C2h 6 + +
La2 Be2 O5 C2h 6 +
LaB3 O6 C2h 6 +
LaP5 O14 C2h 5 + +
La2 CaB10 O19 C2 3 +
b)
LaSc3 (BO3 )4 C2h 6 + + + +
LaGaGe2 O7 C2h 5 +
LaNbO4 C2h 6 + +
La2 (WO4 )3 C2h 6 +
CeP5 O14 C2h 5 +
PrP5 O14 C2h 5 +
a)
NdP5 O14 C2h 5 +
NdGaGe2 O7 C2h 5 +
Gd2 O3 C2h 3 +
Gd2 SiO5 C2h 6 +
GdGaGe2 O7 C2h 5 +
Er2 SiO5 C2h 6 +
Lu2 SiO5 C2h 6 + +
i)
Ta2 O5 C2h 6 +
NaYGeO4 D2h 16 +
NaGdGeO4 D2h 16 +
NaLuGeO4 D2h 16 +
KY(MoO4 )2 D2h 14 + + +
CaSc2 O4 D2h 16 +
Ca3 Ga4 O9 C2v 11 +
Ca(NbO3 )2 D2h 14 + + + + +

Table 3 (continued)
space Ln3+
host crystal group
YAlO3 D2h 16 + + + + +
(Y,Er)AlO3 D2h 16 + + +
CsNd(MoO4 )2 D2h 3 +
GdAlO3 D2h 16 + + + +
GdScO3 D2h 16 (?) +
β -Gd2 (MoO4 )3 C2v 8 +
ErAlO3 D2h 16 + + +
(Er,Lu)AlO3 D2h 16 + +
LuAlO3 D2h 16 + + + + +
tetragonal crystals
CaMoO4 C4h 6 + + +
CaWO4 C4h 6 + + + + +
SrMoO4 C4h 6 + +
SrWO4 C4h 6 +
YVO4 C4h 19 + + + + + +
CsLa(WO4 )2 D2d 4 +
La2 Si2 O7 D4 3 +
GdVO4 C4h 19 + + + +
ErVO4 C4h 19 +
LuPO4 D4h 19 +
LuVO4 D4h 19 + + +
PbMoO4 C4h 6 +
PbWO4 C4h 6 +
trigonal crystals
LiNbO3 C3v 6 + + + + + +
LiNbO3 :MgO c) C3v 6 + +
LiTaO3 C3v 6 +
β-YAl3 (BO3 )4 D3 7 + +
La2 O3 D3d 5 +
β-LaBGeO5 d) C3 2 + +
LaAlO3 D3d 5 +
β-(La,Nd)Sc3 (BO3 )4 D3 7 +
β-CeSc3 (BO3 )4 D3 7 +
β-NdAl3 (BO3 )4 e) D3 7 +
β-NdSc3 (BO3 )4 D3 7 +
β-GdAl3 (BO3 )4 D3 7 + +
Pb5 Ge3 O11 C3 1 +
hexagonal crystals
CaAl12 O19 D6h 4 +
SrAl12 O19 D6h 4 +
SrAl12 O19 :MgO f) D6h 4 + +
cubic crystals
Ca3 Ga2 Ge3 O12 Oh 10 + +
Sc2 O3 Th 7 + + +
Sc2 O3 (ceramic) Th 7 g) +
Y2 O3 Th 7 + + +
Y2 O3 (ceramic) Th 7 g) + +
Y3 Al5 O12 Oh 10 + + + + + +
Y3 Al5 O12 (ceramic) Oh 10 g) + +

Table 3 (continued)
space Ln3+
host crystal group
Y3 Sc2 Al3 O12 Oh 10 + + + +
Y3 Sc2 Al3 O12 (ceramic) Oh 10 g,h) + +
Y3 Fe5 O12 Oh 10 +
Y3 Ga5 O12 Oh 10 + + + +
(Y,Er)3 Al5 O12 Oh 10 + + +
(Y,Er)3 Al5 O12 (ceramic) Oh 10 g) +
(Y,Yb)3 Al5 O12 Oh 10 + +
(Y,Lu)3 Al5 O12 Oh 10 + +
Nd3 Ga5 O12 Oh 10 +
Gd3 Sc2 Al3 O12 Oh 10 + + +
Gd3 Sc2 Ga3 O12 Oh 10 + + + + +
Gd3 Ga5 O12 Oh 10 + + + + +
(Gd,Er)3 Al5 O12 Oh 10 +
Ho3 Al5 O12 Oh 10 +
Ho3 Sc2 Al3 O12 Oh 10 +
Ho3 Ga5 O12 Oh 10 +
Er2 O3 Th 7 + +
Er3 Al5 O12 Oh 10 + + +
Er3 Sc2 Al3 O12 Oh 10 +
(Er,Tm,Yb)3 Al5 O12 Oh 10 +
(Er,Yb)3 Al5 O12 Oh 10 +
(Er,Lu)3 Al5 O12 Oh 10 + +
Tm3 Al5 O12 Oh 10 +
Yb3 Al5 O12 Oh 10 + + +
(Yb,Lu)3 Al5 O12 Oh 10 +
Lu2 O3 Th 7 +
Lu2 O3 (ceramic) Th 7 g) + +
Lu3 Al5 O12 Oh 10 + + + + +
Lu3 Sc2 Al3 O12 Oh 10 + +
Lu3 Sc2 Ga3 O12 Oh 10 +
Lu3 Ga5 O12 Oh 10 + +
Bi4 Si3 O12 Td 6 +
Bi12 SiO20 Td 6 +
Bi4 Ge3 O12 Td 6 + + + + +
a)
Some stable compounds with different structures form in the Yx Nd1−x P5 O14 system [28].
b)
LaSc3 (BO3 )4 crystal can occur in three phases: high-temperature α-phase with space group C5 4 –C2/c, medium-temperature β-phase
(D3 7 –R32), and low-temperature γ-phase (C5 4 –Cc) [29].
c)
Other ‘co-activators’ ZnO, Sc2 O3 , and ZrO2 are also known.
d)
Is also known as a laser glass [23].
e)
According to [30, 31], NdAl3 (BO3 )4 crystal can also have a centrosymmetric α-phase with space group C2h 6 –C2/c or C2 3 –B2 (C2 ).
f)
Laser action in the 4 F3/2 → 4 I11/2 channel of Nd3+ ions has also been excited in the related Sr0.7 Nd0.1 La0.2 Mg0.3 Al11 O19 crystal [32].
g)
Ceramic grains are nano- and (or) micrometre-sized single crystals.
h)
Y3 (Sc,Al)2 Al3 O12 according to [711].
i)
Was grown in the film form, the structure is not carefully determined [703].
j)
To a high probability this crystal has disordered structure.

Table 4 Oxide laser host crystals with ordered

space TM
host crystal structure and their generating TM2+ , TM3+ , TM4+ ,
group
Ni2+ Ti3+ Cr3+ Cr4+ a)
Mn5+ d–c and TM5+ ions and TM defect centres.
monoclinic crystals
ZnWO4 C2h 4 +
Y2 SiO5 C2h 6 +
LiScGeO4 D2h 16 +
LiInGeO4 D2h 16 +
LiNbGeO5 D2h 16 +
BeAl6 O8 C2v 5 +
Mg2 SiO4 b) D2h 16 + +
Al2 (WO4 )3 D2h 14 +
Ca2 GeO4 D2h 16 +
trigonal crystals
α-Al2 O3 D3d 6 + +
ScBO3 D3d 6 +
Sr3 (VO4 )2 D3d 5 +
Ba3 (VO4 )2 D3d 5 +
hexagonal crystals
BeAl2 O4 Dd 6 + +
Be3 Al2 (SiO3 )6 D6h 2 +
BeScAlO4 Dd 6 +
cubic crystals
MgO Oh 5 + +
Ca3 Ga2 Ge3 O12 Oh 10 +
Y3 Al5 O12 Oh 10 +
Y3 Al5 O12 :CaO c) Oh 10 +
Y3 (Al,Sc)2 Al3 O12 :CaO Oh 10 +
Y3 Sc2 Al3 O12 Oh 10 +
Y3 Sc2 Al3 O12 :CaO Oh 10 +
Y3 Sc2 Ga3 O12 Oh 10 +
Y3 Ga5 O12 Oh 10 +
(Y,Lu)3 Al5 O12 :CaO Oh 10 +
Gd3 Sc2 Al3 O12 Oh 10 +
Gd3 Sc2 Ga3 O12 Oh 10 +
Gd3 Ga5 O12 Oh 10 + +
Gd3 (In,Ga)2 Ga3 O12 Oh 10 +
Lu3 Al5 O12 :CaO Oh 10 +
a)
The valency should be refined.
b)
Tunable CW laser action was achieved in Mg2 SiO4 :Li+ crystal [705].
c)
Mg2+ ions (MgO) are also used in the place of the Ca2+ (CaO) charge compensators.
Table 5 Fluoride laser host crystals with disordered

space Ln3+
host crystal structure and their Ln3+ lasants.
group
Nd3+ Ho3+ Er3+ Tm3+
trigonal crystals
Ca2 Y5 F19 D3d 4 +
Sr2 Y5 F19 D3d 4 + +
YF3 –SrF2 D3d 4 (?) +
LaF3 –SrF2 D3d 4 + +
GdF3 –CaF2 D3d 4 +

Table 5 (continued)
space Ln3+
host crystal group
Nd3+ Ho3+ Er3+ Tm3+
hexagonal crystal
CaLu2 F8 D6h 4 (?) +
cubic crystals
5NaF · 9YF3 (Na0.4 Y0.6 F2.2 ) a) Oh 5 + +
α-NaCaYF6 Oh 5 +
α-NaCaCeF6 Oh 5 +
α-NaCaErF6 Oh 5 + +
CaF2 –ScF3 Oh 5 +
CaF2 –SrF2 Oh 5 +
CaF2 –SrF2 –BaF2 –YF3 –LaF3 Oh 5 +
CaF2 –YF3 Oh 5 + + +
CaF2 –YF3 –NdF3 Oh 5 +
CaF2 –LaF3 Oh 5 +
CaF2 –CeO2 b) Oh 5 +
CaF2 –CeF3 Oh 5 +
CaF2 –NdF3 Oh 5 +
CaF2 –GdF3 Oh 5 +
CaF2 –HoF3 Oh 5 +
CaF2 –HoF3 –ErF3 Oh 5 + +
CaF2 –ErF3 Oh 5 + + +
CaF2 –ErF3 –TmF3 Oh 5 + +
CaF2 –ErF3 –TmF3 –YbF3 Oh 5 +
CaF2 –LuF3 Oh 5 +
SrF2 –ScF3 Oh 5 +
SrF2 –YF3 Oh 5 + +
SrF2 –LaF3 Oh 5 +
SrF2 –CeF3 Oh 5 +
SrF2 –CeF3 –GdF3 Oh 5 +
SrF2 –NdF3 Oh 5 +
SrF2 –GdF3 Oh 5 +
SrF2 –ErF3 Oh 5 + +
SrF2 –LuF3 Oh 5 +
CdF2 –ScF3 Oh 5 +
CdF2 –YF3 Oh 5 +
CdF2 –YF3 –LaF3 Oh 5 +
CdF2 –CeF3 Oh 5 +
CdF2 –LaF3 Oh 5 +
CdF2 –NdF3 Oh 5 +
CdF2 –GdF3 Oh 5 +
CdF2 –LuF3 Oh 5 +
BaF2 –YF3 Oh 5 +
BaF2 –LaF3 Oh 5 +
BaF2 –CeF3 Oh 5 +
BaF2 –NdF3 Oh 5 +
BaF2 –GdF3 Oh 5 +
BaF2 –ErF3 Oh 5 +
BaF2 –LuF3 Oh 5 + +
a)
It is probable that Na0.4 Y0.6 F2.2 (2NaF · 3YF3 or 4NaF · 6YF3 ) [33] is the
same as 5NaF · 9YF3 . The phase structure of these crystals requires a more
accurate definition.
b)
Crystal contains oxygen: in the table it is introduced conditionally.

Table 6 Oxide laser host crystals with dis-

space Ln3+
host crystal ordered structure and their Ln3+ lasants.
group
Pr3+ Nd3+ Ho3+ Er3+ Tm3+ Yb3+
monoclinic crystals
Li3 Ba2 Gd3 (MoO4 )8 C2h 6 +
K3 Nd(PO4 )2 C2h 6 +
(Y,Gd)2 SiO5 C2h 6 (?) +
LaSr2 Ga11 O20 C2h 3 +
La0.5 Nd0.5 P5 O14 C2h 5 +
Gd2 (WO4 )3 C2h 6 +
Bi5.8 PO11.2 (?) +
Na3 Nd(PO4 )2 D2h 11 +
Ca0.25 Ba0.75 (NbO3 )2 D2h 14 +
Sr0.4 Ba0.6 (NbO3 )2 a) C2v 4 +
Ba2 NaNb5 O15 C2v 11 +
tetragonal crystals
LiLa(MoO4 )2 C4h 6 +
LiGd(MoO4 )2 C2h 6 + +
NaY(MoO4 )2 C2h 6 +
NaY(WO4 )2 C2h 6 +
NaLa(MoO4 )2 C2h 6 + + +
NaLa(WO4 )2 C2h 6 + +
Na5 Nd(WO4 )4 C2h 6 (?) +
NaGd(MoO4 )2 C2h 6 +
NaGd(WO4 )2 C2h 6 + + +
NaLu(WO4 )2 C2h 6 +
NaBi(MoO4 )2 C2h 6 +
NaBi(WO4 )2 C2h 6 +
KLa(MoO4 )2 C2h 6 (?) + + +
Ca2 Al2 SiO7 D2d 3 + + + +
Ca2 Ga2 SiO7 D2d 3 +
CaYAlO4 D4h 17 + +
CaGdAlO4 D4h 17 +
SrYAlO4 D4h 17 +
SrLaGa3 O7 D2d 3 + +
SrGdGa3 O7 D2d 3 +
(Y,Gd)VO4 C4h 19 + +
Ba2 MgGe2 O7 D2d 3 +
Ba2 ZnGe2 O7 D2d 3 +
BaLaGa3 O7 D2d 3 +
trigonal crystals
β -Na1.67 Mg0.67 Al10.33 O17 D3d 5 +
K5 Nd(MoO4 )4 D3d 5 +
K5 Bi(MoO4 )4 D3d 5 +
Ca3 Ga2 Ge4 O14 D3 2 +
Sr3 Ga2 Ge4 O14 D3 2 +
Ba3 LaNb3 O12 D3d 5 + b)
Ba3 LaTa3 O12 D3d 5 + b)
La3 Ga5 SiO14 D3 2 +
La3 Ga5 GeO14 D3 2 +

Table 6 (continued)
space Ln3+
host crystal group
Pr3+ Nd3+ Ho3+ Er3+ Tm3+ Yb3+
La3 Ga5.5 Nb0.5 O14 D3 2 +

La3 Ga5.5 Ta0.5 O14 D3 2 +
Nd3 Ga5 SiO14 D3 2 +
Pb3 Ga2 Ge4 O14 D3 2 +
hexagonal crystals
CaY4 (SiO4 )3 O C6h 2 + + +
CaLa4 (SiO4 )3 O C6h 2 +
Ca4 La(PO4 )3 O C6h 2 +
CaGd4 (SiO4 )3 O C6h 2 + +
Sr3 Al(BO3 )3 D2d 3 (?) +
SrY4 (SiO4 )3 O C6h 2 + + +
(Sr,La)(Al,Mg)12 O19 D6h 4 +
SrLa4 (SiO4 )3 O C6h 2 + +
LaMgAl11 O19 D6h 4 +
7La2 O3 · 9SiO2 C6h 2 +
cubic crystals
CaMg2 Y2 Ge3 O12 Oh 10 +
Ca3 (Nb,Ca)2 Ga3 O12 Oh 10 + +
YScO3 Th 7 +
YGaO3 (Y3 (Y0.5 Ga0.5 )2 Ga3 O12 ) Oh 10 +
(Y0.5 Gd0.5 )O2 (ceramic) Th 7 +
Ba0.25 Mg2.75 Y2 Ge3 O12 Oh 10 +
(La,Sr)(Al,Ta)O3 c) (?) +
(La,Lu)3 (Lu,Ga)2 Ga3 O12 Oh 10 +
LuScO3 Th 7 +
ZrO2 –Y2 O3 Oh 5 + +
ZrO2 –Er2 O3 Oh 5 + + +
HfO2 –Y2 O3 Oh 5 +
Bi4 (Si,Ge)3 O12 Td 6 +
a)
As well as Sr0.6 Ba0.4 (NbO3 )2 and Sr0.47 Ba0.53 (NbO3 )2 [704].
b)
Results on pulse SE obtained in [34,35] require confirmation: in the table they are introduced conditionally.
c)
The exact formula of the crystal used is (La0.288 Nd0.007 Sr0.704 )(Al0.648 Ta0.352 )O3 [36].
Before considering the intermanifold lasing transitions of will be more perceptible. This could also significantly help
Ln3+ , it should be emphasized here that the above men- in investigating novel pumping technologies.
tioned number of their SE channels is only a small part of
their theoretically possible emitting potential. According
to [65] the number of the 4fN –4fN intermanifold transi- 4. Stimulated emission of intermanifold
tions is 192 177. Due to some limitations stipulated by the
physical characteristics of host crystals and spectroscopic
4fN –4fN and 4fN−1 5d1 –4fN transitions of
properties of Ln3+ ions, as well as other pumping difficul- lanthanides (Ln3+ and Ln2+ ) and the 5f3 –5f3
ties, currently researchers discover an average of one or two channel of the U3+ ion
new laser channels per year. The point is that, in laser crystal
physics, these searches are the most complex ones. How- The Stark levels of 2S + 1 LJ manifolds of 4fN config-
ever, accumulated knowledge and experience in this field uration electrons of Ln3+ generating ions in many host
of investigations (see, e.g. [11, 18, 21, 66, 67]) can give us crystals have been studied and analysed adequately (see,
confidence that in the near future the results of this research e.g. [11, 18, 68, 69]), while for the energy levels of the

Table 7 Oxide laser host crystals with disordered structure and No. SE channel crystal and pumping ref.
their TM2+ , TM3+ , and TM4+ lasants. condition
host crystal space TM 1 5d1 → 2 F7/2 LiYF4 , 300K, las. [70]
group 2 5d1 → 2 F5/2 LaF3 , 300K, las. [71]
Ni2+ Cr3+ Cr4+ a)
trigonal crystals
Ca3 Ga2 Ge4 O14 D3 2 +
2
Sr3 Ga2 Ge4 O14 D3 +
La3 Ga5 SiO14 D3 2 +
2
La3 Ga5 GeO14 D3 +
La3 Ga5.5 Nb0.5 O14 D3 2 +
La3 Ga5.5 Ta0.5 O14 D3 2 +
hexagonal crystals
CaGd4 (SiO4 )3 O C6h 2 +
2
SrGd4 (SiO4 )3 O C6h +
cubic crystals
Figure 1 Known intermanifold 5d1 –4f1 laser
10
CaMg2 Y2 Ga3 O12 Oh + transitions (SE channels) of Ce3+ ions in
(La,Lu)3 (Lu,Ga)2 Ga3 O12 Oh 10 + anisotropic fluoride crystals SE generation of
(Gd,Ca)3 (Ca,Mg,Zr)2 Ga3 O12 Oh 10 + which were excited with laser pumping. Nota-
tions in figure table as in Table 10.
a)
mid-IR SE generation can be excited also at wavelengths

4fN −1 5d1 configurations this is not so complete. For the of inter-Stark transitions in the 2 F7/2 → 2 F5/2 channel by
latter case, many laser crystals cannot be studied, because the cascade generation principle [18, 75] within the possi-
the energy position of the 5d1 levels usually coincides with ble 5d1 → 2 F7/2 → 2 F5/2 laser scheme using UV pumping in
the fundamental absorption band of the host. To study the 4f1 → 5d1 absorption bands.
levels of the 5d1 configuration fluorides having a broad Crystals doped with Pr3+ ions permit one to excite SE at
optical transparency are most suitable. These compounds the wavelengths of their 18 generating intermanifold 4f2 –
were used for the first laser crystals in which SE generation 4f2 transitions (Fig. 2) overlapping the widest spectral range
was excited across 4fN −1 5d1 –4fN transitions of Ce3+ and (from ∼ 0.48 to ∼ 7.24 µm) among all of the known lasing
Nd3+ ions. activators [11, 18, 19]. The longest wavelength intermani-
fold 3 F3 → 3 F2 transition of all known SE channels of gen-
erating Ln, TM, and Ac activators in laser crystals also
4.1. Laser channels of Ce3+ and Pr3+ ions belongs to Pr3+ ions (Table 10). From the end of the 1970s,
interest in the visible SE of crystalline lasers revived, and
Ce3+ ions have two UV laser channels which are connected the anisotropic fluorides doped with Pr3+ ions again ap-
with their 4fN −1 5d1 –4fN (5d1 –4f1 ) electric dipole (ed) al- peared attractive to researchers. During the ensuing years,
lowed transitions in several fluoride crystals (Table 1 and several low-threshold SE generations at room temperature
Fig. 1). To achieve this SE generation the radiation of KrF with Xe-flashlamp pumping have been excited in the or-
and ArF excimer lasers as well as quadrupled pulsed gener- ange, red, deep red, and IR spectral ranges across inter-
ation (λp ≈ 0.266 µm) of Y3 Al5 O12 :Nd3+ lasers were used Stark transitions of the 4f2 –4f2 channels of this advanced
as pumping sources (see, e.g. [70–73]). The result of UV lasing activator. Ytterbium-containing fluorides with Pr3+
lasing excitation in the LuPO4 :Ce3+ crystal is also worth ions have allowed SE generation in two intermanifold tran-
noting [74], which indicates that Ce3+ -doped oxides are sitions which start from the levels of the 1 G4 manifold:
also promising materials for obtaining 5d1 –4f1 UV laser ac- 1
G4 → 3 H5 and 1 G4 → 3 F4 . The first, 1.34 µm, channel has
tion. The high-gain UV band associated with 5d1 → 2 F5/2,7/2 become widely used in praseodymium fibreglass lasers
channels also allows tuning of the laser frequency up to and amplifiers (see, e.g. [121, 668]). The second one, at
4000 cm−1 , which enables several modern important ap- about 3.6 µm, appears to be the longest wavelength avail-
plications ranging from the nanotechnology and medical able from a Xe-flashlamp-pumped crystalline laser. Laser
fields to lidar atmospheric sensing (see, e.g. [157]). It is action can also be achieved at this intermanifold transi-
quite possible that in some crystals with Ce3+ ions fea- tion using the direct cascade 3 P0 → 1 G4 → 3 F4 scheme [18].
turing high transparency in the 4.5–6 µm spectral range, New properties of Pr3+ activator ions have been discovered

Table 8 Anisotropic chloride, bromide, sulphide, oxyfluoride, oxychloride, and oxysulphide laser host crystals and their Ln3+ , Ln2+ ,
and TM5+ lasants.
space Ln3+ Ln2+ TM5+

host crystal group
Pr3+ Nd3+ Dy3+ Ho3+ Er3+ Yb3+ Eu2+ Mn 5+
monoclinic crystal
KPb2 Cl5 C2h 5 + + +
5
KPb2 Br5 C2h +
CaGa2 S4 :(Na+ ) D2h 24 +
24
CaGa2 S4 D2h + +
PbCl2 D2h 16 +
PbGa2 S4 D2h 24 +
tetragonal crystals
RbPb2 Br3 D4h 18 + +
hexagonal crystals
Na2 Nd2 Pb6 (PO4 )6 Cl2 C6h 2 +
a) 2
Ca5 (PO4 )3 F C6h + + + +
(Ca,Sr)5 (PO4 )3 F C6h 2 +
Sr5 (PO4 )3 F a) C6h 2 + +
2
Sr5 (VO4 )3 F C6h + + +
Sr5 (VO4 )3 Cl C6h 2 +
Ba5 (PO4 )3 F a) C6h 2 +
2
Ba5 (PO4 )3 Cl C6h +
BaCaBO3 F D3h 3 +
2
LaCl3 C6h +
LaBr3 C6h 2 +
CeCl3 C6h 2 +
2
PrCl3 C6h +
PrBr3 C6h 2 +
2
Pb5 (PO4 )3 F C6h +
trigonal crystal
La2 O2 S D3d 3 +
a)
Laser action of Yb3+ ions has been excited in several solid solutions in the Sr5−x Bax (PO4 )3 F system (with x = 0.25; 0.5; and 1)
[46]; likewise, Nd3+ ions have been lased in solid solutions of the Ca5−x Srx (PO4 )3 F system (with x = 0−1) [47].
in YAlO3 and α-KY(WO4 )2 type crystals. At 300 K with In accordance with the general notions of the theory
Xe-flashlamp-pumping low-threshold one-micron SE was and practice of colour mixing for the creation of different
excited connected with the long-lived initial laser 1 D2 state. hues, including white, it is necessary to have three primary
With this manifold pulsed generation was also achieved in colours (red, green, and blue) whose additive mixtures pro-
a new 1.5 µm 1 D2 → 1 G4 channel (Table 10 and Fig. 2). duce nearly all other colours. It should be particularly em-
Laser action in this spectral region can have practical im- phasized that the already existing visible praseodymium
portance, especially if it is possible to use direct “red” LD crystalline lasers are capable of generating all the needed
pumping (3 H4 → 1 D2 ). It should be particularly emphasized primary emissions (Fig. 3). This promotes the idea of us-
here that the intermanifold luminescence branching ratios ing these lasers for the development of a new generation
of two SE channels (1 D2 → 1 F3 and 1 D2 → 1 G4 ) are rather of projection colour televisions and other display devices.
high [182, 279]. Over the last few years the average output power in the red

No. SE channel crystal and pumping ref.

condition
1 1
D2 → 3 F4 CaWO4 , 77K, Xe [76]
CaWO4 , 300K, Xe [77]
2 3
P0 → 3 H6 LaF3 , ≈ 76K, Xe [78]
β-BaY2 F8 , 300K, Xe [79]
3 3
P0 → 3 F2 PrCl3 , 300K, las. [80]
LiYF4 , LiLuF4 , 300K, Xe [81, 82]
4 3
P1 → 3 H5 LaCl3 , ≈ 35K, las. [42]
LiGdF4 , 300K, las. [83]
5 3
P0 → 3 H4 LaCl3 , ≈ 14K, las. [42]
LiYF4 , 300K, las. [84]
6 3
P2 → 3 F3 LaBr3 , 300K, las. [85]
7 3
P0 → 3 F4 LaF3 , 300K, Xe [86]
8 3
P0 → 3 F3 YAlO3 , 300K, Xe [87]
9 3
P0 → 3 H5 LiYF4 , ≈ 110K, Xe [81]
LiGdF4 , 300K, las. [83]
10 1
G4 → 3 H5 β-BaYb2 F8 , ≈ 110K, Xe [88]
11 1
G4 → 3 F4 β-BaYb2 F8 , ≈ 110K, Xe [88]
12 3
P0 → 1 G4 LiYF4 , 300K, Xe [89]
13 1
D2 → 3 F3 YAlO3 , 300K, Xe [90]
14 3
F3 → 3 H4 LaCl3 , ≈ 130K, las. [91]
15 3
F3 → 3 H6 LaCl3 , ≈ 200K, las. [91]
16 3
F3 → 3 F2 LaCl3 , ≈ 148K, las. [41]
17 1
D2 → 1 G4 α-KY(WO4 )2 , ≈ 110K, Xe [11]
18 3
F3 → 3 H5 RbPb2 Cl5 , 300K, las. [728]
Figure 2 Known intermanifold 4f2 –4f2 laser transitions of Pr3+ ions in crystals. The channels in which SE was excited with laser
pumping are marked by open circles. Notations in figure table as in Table 10.
of Pr3+ :LiYF4 lasers with the usual Xe-flashlamp pumping where AJJ is the probability of 4fN –4fN intermanifold
has amounted to 2.3 W [122]. J → J transitions which is the sum of the probabilities of
Quite recently in studies of the spectroscopic proper- ed and magnetic dipole (md) transitions
ties of Pr3+ ions in laser crystals significant progress has
also been achieved in refining the calculation method of Aed,md
JJ = Aed md
JJ + AJJ (3)
electric-dipole (ed) intermanifold J → J transition inten-
sity theory of Ln3+ activators in crystalline materials (see, 64π 2 e2 n̄(n̄2 + 2)2 ed
= 3
SJJ + n̄3 SJJ
md
.
e.g. [133] and references therein). This method, based on 3h(2J + 1)λ̄ 9
the well-known Judd-Ofelt approach for weak interconfig-
It is simple to calculate the line strength of md transitions
uration interaction (WICI), has become widely used for md
SJJ if one knows the dispersion of the averaged crystalline
prediction of the SE generation potential of Ln3+ ions in
refractive index n̄(λ̄) (see, e.g. [18]). The n̄(n̄2 + 2)2 /9
crystals – in particular, such important parameters as in-
term in eq. (3) is the local field correction factor, which
termanifold luminescence branching ratios and radiative
strongly depends on the host crystal type (e.g. for fluorides
lifetimes of metastable initial laser states:
and oxides). In the WICI Judd-Ofelt approximation, the
AJJ energy separation of an excited 4fN −1 5d1 configuration to
βJJ = (1) be identical for each manifold included in the intermanifold
AJJ
J J → J transitions. In this case, the line strength of J–J ed
transitions is given by
and ed
SJJ (WICI) (4)
1
τrad (J) = 2
AJJ
(2) = e2 Ωt 4fN [SL] J U (t) 4fN [S L ] J
J t=2,4,6

Figure 3 Example of a simplified chromaticity

diagram [92]. The wavelengths of monochromatic
light are given in µm. Visible room temperature SE
intermanifold 4f2 –4f2 laser transitions for Pr3+ ions
in insulating crystals are indicated by arrows.
Table 9 Ln3+ - and TM2+ -doped II–VI and III–V semiconductor configuration radial integrals, and energy denominators;
host crystals. … ||U (t) || … are the reduced matrix elements of a unit
tensor operator U (t) of rank t; S, L, and J are the total
Ln3+ TM2+ spin, total orbital, and total angular momenta, respectively;
host crystal space group
Nd3+ Er3+ Cr2+ Fe2+ and λ̄ is the averaged wavelength of the J → J channels.
To calculate the Ω t parameters it is necessary to solve the
ZnS C6v 4 a) + set of equations of eq. (4) using the experimentally mea-
ZnS:(Cu,Cl) Td 2 a) + b) sured values:
ZnS0.42 Se0.58 Td 2 (?) +
k(λ) dλ 3ch(2J + 1) 9n̄
ZnSe Td 2 + c) + ed
SJJ = (5)
N0 3 2
8π e λ̄ (n̄ 2 + 2)2
ZnSe (ceramic) Td 2 +
GaInAsP (?) +
where k(λ) dλ is the integral absorption coefficient of the
CdSe C6v 4 + band area associated with the intermanifold J → J transi-
CdTe Td 2 + tion (sometimes ‘overlapping’ transitions). The rest of the
Cd0.85 Mn0.15 Te Td 2 + notations used in eqs. (3), (4), and (5) are standard. In gen-
n-InP Td 2 (?) + eral, the set of Ω t parameters determined using absorption
spectra allows one to calculate the value of Aed JJ across
a)
Some II–VI compounds can crystallize in either zincblende any pair of manifolds of Ln3+ ions, including their expected
(Td 2 ) or wurtzite (C46v ) structure, depending on the specific SE channels.
growth methods. The WICI Judd-Ofelt approximation will be correct
b)
SE generation result which was obtained in [51] requires only if the energy of the excited 4fN −1 5d1 configuration is
confirmation. significantly larger than the manifold energy of the ground
c)
Record tuning (1.880 to 3.4 µm wavelength) was 4fN configuration. Actually, the manifold energies of Ln3+
achieved [707]. ions are of the same order of magnitude as the energy of the
4fN −1 5d1 configuration. Thus, fulfilment of the conditions
for realization of the WICI approximation is improbable,
where Ω t are the intensity parameters which reflect the and use of eq. (4) should lead to contradictions more often
fundamental coupling of the probabilities of ed transitions than is actually the case. Since the energy intervals between
in absorption and luminescence – they contain implicitly the excited 4fN −1 5d1 configuration and the high- and low-
the effect of the odd-symmetry crystal field terms, inter- lying 4fN manifolds differ significantly from one another,

Table 10 Spectral generation ranges and SE

operating conditions intermanifold transitions of Ln, Ac, and TM
spectral range (µm) lasing ion SE channel
T (K) pumping a) ions in laser crystals.
generation in the vacuum UV

0.172 b) Nd3+ [4f2 5d1 ] → 4 I11/2 300 laser
generation in the UV
0.286 to 0.330 Ce3+ 5d1 → 2 F7/2 300 laser
0.306 to 0.315 Ce 3+
5d → F5/2
1 2
300 laser
0.3479 Tm3+ 1
I6 → 3 H 4 300 laser
generation in the visible
0.38006 to 0.38052 Nd3+ 4
D3/2 → 4 I11/2 < 90 laser
0.41296 Nd 3+ 2
P3/2 → 4 I11/2 < 90 laser
0.4526 to 0.456 Tm 3+ 1
D2 → H4 3
300 laser
0.4574 to 0.4581 Tm3+ 1
I6 → 3 F 4 ∼ 77 laser
0.469 to 0.470 Er 3+ 2
P3/2 → I11/2 4
20 to 35 laser
0.479 to 0.489 Pr3+ 3
P0 → 3 H4 300 laser
0.482 to 0.486 Tm3+ 1
G4 → 3 H6 ∼ 300 laser
0.510 to 0.512 Tm 3+ 1
D2 → H5 3
300 laser
0.522 to 0.532 Pr3+ 3
P1 → 3 H5 300 laser
0.539 to 0.578 Pr 3+ 3
P0 → H5 3
300 Xe
0.544 Tb3+ 5
D4 → 7 F 5 300 Xe
0.544 to 0.561 Er3+ 4
S3/2 → 4 I15/2 300 Xe, laser
0.5507 to 0.5515 Ho 3+ 5
S2 → I8 5
77 Xe, laser
0.5555 to 0.5755 Eu2+ [4f6 5d1 ] → 4f7 c)
77 laser
0.561 Er 3+ 2
G(1)9/2 → I13/2 4 d)
49 to 77 Xe, laser
0.572 to 0.5739 Dy3+ 4
F9/2 → 6 H13/2 ≤ 180 Xe
0.5932 to 0.605 Sm3+ 4
G5/2 → 6 H7/2 300 Xe, laser
0.598 to 0.622 Pr3+ 3
P0 → 3 H6 300 Xe
0.611 to 0.619 b)
Eu 3+ 5
D0 → 7 F 2 77 Xe
0.611; 0.66 to 1.18 Ti 3+ 2
E → T2
2
300 Xe, laser
0.616 to 0.6201 Pr3+ 3
P1 → 3 F2 e)
300 laser
0.617 to 0.618 Er3+ 2
P3/2 → 4 F9/2 ≤ 41 laser
0.632 Pr 3+ 3
P2 → F3 3
300 laser
0.637 to 0.6624 Pr3+ 3
P0 → 3 F2 300 Xe
0.649 to 0.65 Tm 3+ 1
G4 → H4 3
300 laser
0.662 to 0.6636 Dy3+ 4
F9/2 → 6 H11/2 ∼ 110 Xe
0.67 to 0.671 Er3+ 4
F9/2 → 4 I15/2 ∼ 100 Xe, laser
0.6703 Pr 3+ 3
P1 → F3 3 e)
300 laser
0.679 to 0.745 Sm2+ [4f5 5d1 ; 5 D0 ] → 7 F1 20 to 310 Xe, laser
0.68 to 0.704 Cr 3+ 2
E → A2
4
300 Xe, Hg
0.694 to 0.7073 Er3+ 2
G(1)9/2 → 4 I11/2 d)
15 to 90 Xe, laser
0.694 to 0.7221 Pr3+ 3
P0 → 3 F3 300 Xe
0.6994 Pr 3+ 3
P1 → F4 3 e)
300 laser
0.7082 Pr3+ 1
I6 → 3 F 4 e)
300 laser
0.717 to 0.7537 Pr 3+ 3
P0 → F4 3
300 Xe, laser
0.7295 Nd3+ 2
P3/2 → [2 H(2)9/2 +2 F5/2 ] < 20 laser
0.74 to 0.89 Cr3+ [2 E, 4 T2 ] → 4 A2 77 to 500 Xe
0.75 to 0.761 Ho3+ 5
S 2 → 5 I7 300 Xe

Table 10 (continued)
operating conditions
T (K) pumping a)
0.7505 b) Dy3+ 4
F9/2 → [6 H9/2 +6 F11/2 ] f) f)
0.792 to 0.799 Tm3+ 1

G4 → 3 H5 300 laser
0.810 Tm3+ 3
F4 → 3 H6 300 laser
generation in the near-IR
0.843 to 0.863 Er3+ 4
S3/2 → 4 I13/2 300 Xe, PCh
0.86 to 1.480 Cr3+ 4
T2 → 4 A2 300 laser
0.879 to 0.947 Nd3+ 4
F3/2 → 4 I9/2 300 Xe, laser, LD
0.901 to 0.9395 Pr3+ 3
P0 → 1 G4 300 Xe
∼ 0.97 Nd3+ [ H(2)9/2 +4 F5/2 ] → 4 I9/2
2
300 OPO
0.979 to 1.018 Ho3+ 5
F5 → 5 I7 300 Xe
0.98 to 1.108 Yb3+ 2
F5/2 → 2 F7/2 300 Xe, LED, laser, LD
0.996 to 1.0223 Pr3+ 1
D2 → 3 F3 300 Xe
1.014 to 1.031 Ho3+ 5
S2 → 5 I6 300 Xe
1.037 to 1.12 Nd3+ 4
F3/2 → 4 I11/2 300 g) Xe, Kr, W, solar, PCh, LED,
laser, LD, e-beam, X-ray,
OPO
1.0465 to 1.0697 Pr3+ 1
D2 → 3 F4 300 Xe
1.05 to 1.33 V2+ 4
T2 → 4 A2 77 to 200 Xe, Kr
1.1160 Tm2+ 2
F5/2 → 2 F7/2 4.2 Xe
1.1664 Er3+ 4
F9/2 → 4 I13/2 ∼ 110 Xe
1.167 to 1.950 Cr4+ 3
T2 → 3 A2 300 Xe, laser, LD
1.168 to 1.181 h) Mn5+ 1
E → 3 A2 300 laser
∼ 1.18 Nd3+ [ H(2)9/2 +4 F5/2 ] → 4 I13/2
2
300 OPO
1.19 to 1.216 Ho3+ 5
I6 → 5 I8 ∼ 110 Xe
1.2195 to 1.26 Er3+ 4
S3/2 → 4 I11/2 300 Xe, laser, LD
1.2805 d-c – 77 to 180 Xe
1.306 to 1.486 Nd3+ 4
F3/2 → 4 I13/2 300 i) Xe, Kr, laser, LD
1.314 to 1.939 Ni2+ 3
T2 → 3 A2 77 to 240 Xe, laser
1.334 to 1.347 Pr3+ 1
G4 → 3 H5 ∼ 110 Xe
1.391 to 1.408 Ho3+ 5
S2 → 5 I5 300 Xe
∼ 1.4 b) Dy3+ [ H9/2 +6 F11/2 ] → 6 H15/2
6
300 laser
1.462 to ∼ 1.505 Tm3+ 3
F4 → 3 H4 300 Xe, laser, LD, FL
1.4862 to 1.4912 Ho3+ 5
F5 → 5 I6 ≤ 190 Xe
1.5235 Pr3+ 1
D2 → 1 G4 ∼ 110 Xe
1.529 to 1.664 Er3+ 4
I13/2 → 4 I15/2 77 to 300 Xe, laser, LD
1.568 to 1.5808 Tm3+ 1
G4 → 3 F3 300 Xe, laser
1.611 to 1.644 Pr3+ 3
F3 → 3 H4 ∼ 130 laser
1.62 to ∼ 2.5 j) Co2+ 4
T2 → 4 T1 77 to 300 Xe, laser
1.645 to 1.777 Er3+ 4
S3/2 → 4 I9/2 300 Xe
1.673 Ho3+ 5
I5 → 5 I7 77 Xe
∼ 1.68 b) Er3+ 4
I9/2 → 4 I13/2 300 Xe
1.833 Nd3+ 4
F3/2 → 4 I15/2 ∼ 300 Xe
1.85 to ∼ 2.18 Tm3+ 3
H4 → 3 H6 77 to 300 Xe, Hg, W, laser, LD
1.880 to ∼ 3.100 Cr2+ 5
E → 5 T2 300 laser, OPO
1.965 to 2.0025 Er3+ 4
F9/2 → 4 I11/2 300 Xe
1.933 to 2.171 Ho3+ 5
I7 → 5 I8 77 to 300 Xe, Kr, W, PCh, solar, laser,
LD

Table 10 (continued)
operating conditions
T (K) pumping a)
2.234 to 2.827 k) U3+ 4

I11/2 → 4 I9/2 77 to 300 Xe, Hg, laser
2.274 to ∼ 2.46 Tm 3+ 3
F4 → H53
300 Xe, laser
2.31 to 2.59 Pr3+ 3
F3 → 3 H5 300 laser
2.35 to 2.377 Ho3+ 5
F 5 → 5 I5 ∼ 100 Xe
2.359 to 2.366 Dy 2+ 5
I7 → I8
5
4.2 to 120 Xe, solar, PCh, LED, laser
2.432 Dy3+ [6 H9/2 +6 F11/2 ] → 6 H13/2 300 laser
2.660 to ∼ 3.01 Er3+ 4
I11/2 → 4 I13/2 77 to 400 Xe, laser, LD
2.83 to ∼ 3.05 Ho 3+ 5
I6 → 5 I7 77 to 350 Xe
generation in the mid-IR
2.972 to 3.040 Dy3+ 6
H13/2 → 6 H15/2 77 to 300 Xe, laser
3.369 Ho 3+ 5
S2 → 5 F5 300 laser
∼ 3.41 Er3+ 4
F9/2 → 4 I9/2 77 laser
3.53 to 5.05 l)
Fe 2+ 5
T2 → 5 E 300 laser, Raman laser
3.605 Pr 3+ 1
G4 → F4 3
∼ 110 Xe
3.893 to 3.914 Ho3+ 5
I5 → 5 I6 300 laser, cascade
4.31 to ∼ 4.38 Dy3+ 6
H11/2 → 6 H13/2 300 laser
∼ 4.75 Er 3+ 4
I9/2 → I11/2
4
∼ 110 Xe, cascade
∼ 5.15 Nd3+ 4
I13/2 → 4 I11/2 300 Xe, cascade
5.117 to 5.242 Pr3+ 3
F 3 → 3 H6 ∼ 200 laser
∼ 7.24 b)
Pr 3+ 3
F3 → 3 F2 ∼ 148 laser
a)
e-beam, electron beam; LED, light-emitting diode; PCh, pyrochemical pumping; FL, fiber laser; OPO, optical parametric oscillator;
Xe, W, Hg, Kr, xenon, tungsten-iodine, mercury, krypton lamps, respectively.
b)
Data should be corroborated or refined.
c)
Laser transition not identified precisely.
d)
Notation of the initial laser state changed in accordance with the recent calculation of the reduced-matrix elements (see, e.g. [58,
59]).
e)
This SE channel is included in the table conditionally because in [60] no scientific explanation for its identification was given.
f)
Pumping condition in [61] was not given.
g)
Laser action in the pulse regime was excited up to ∼ 1100 K [21].
h)
The valency of “Cr4+ ”-ion lasing centers in most published crystals should be refined.
i)
Laser action in the pulse regime was excited up to ∼ 700 K [21].
j)
Short-wave border of SE tuning range in [62] indicated as ∼ 1.52 µm. According to [63], MgF2 :Co2+ crystals can generate with
tuning of the SE wavelength from 1.8 to ∼ 2.5 µm with laser pumping at 300K.
k)
According to [64], laser action at a wavelength of 2.234 µm can belong to the U4+ ions in tetragonal centres of the CaF2 host.
l)
Tunable SE range (∼ 3.95 to ∼ 5.05 µm wavelength) was achieved with ZnSe:Cr2+ laser [708].
the excited configuration will influence different manifolds crystal field Hamiltonian was obtained, which in addition
to a substantially different extent. Among the Ln3+ activa- to the usual terms contains energy-dependent operators. In
tors this situation appears to a large extent for Pr3+ ions. addition, a convenient expression was obtained for the ef-
It is well known that intensity analysis using eq. (4) for a fective ed line strength operator:
number of Pr3+ -doped crystals, including lasing anisotropic
fluorides LiYF4 :Pr3+ , leads to meaningless negative values ed
of the Ω t parameters. As noted above, in [133] an impor- SJJ (IICI) (6)
tant step was made in the solution of this problem. In an

approximation of the intermediate interconfiguration inter- = e2 Ωt 1 + 2Rt EJ + EJ − 2Ef0
action (IICI) taking into account the effect of the differ- t=2,4,6 2

ent influence of the 4fN −1 5d1 configuration on Ln3+ (Pr3+ ) × 4fN [SL]JU (t) 4fN [S L ]J
manifolds in the ground 4fN configuration a corresponding
Ω̃t


condition
1 4
F3/2 → 4 I11/2 CaWO4 , 300K, Xe [93]
2 4
F3/2 → 4 I9/2 CaWO4 , 77K, Xe [104]
Y3 Al5 O12 , 300K, Xe [105]
3 4
F3/2 → I13/2
4
CaWO4 , 300K, Xe [104]
4 4
F3/2 → 4 I15/2 Y3 Al5 O12 , ≈ 300K, Xe [105]
5 4
I13/2 → I11/2
4
BaF2 -LaF3 , 300K, cascade [107]
6 4f2 5d1 → 4 I11/2 LaF3 , 300K, las. [108]
7 4
D3/2 → 4 I11/2 LaF3 , <90K, las. [109]
8 3
P3/2 → I11/2
4
LiYF4 , <90K, las. [110,111]
9 3
P3/2 → [2 H(2)9/2 +4 F5/2 ] LiYF4 , <20K, las. [110,111]
10 [ H(2)9/2 + F5/2 ] → I11/2
2 4 4
RbPb2 Cl5 , 300K, OPO [702]
11 [2 H(2)9/2 +4 F5/2 ] → 4 I13/2 RbPb2 Cl5 , 300K, OPO [702]
12 4
F3/2 → I9/2
4
GdVO4 , 300K, LD [710]
Figure 4 Known intermanifold 4f3 –4f3 and 4f2 5d1 –4f3 laser transitions of Nd3+ ions in crystals. Notations as in Fig. 2.
where Ω̃t are the intensity parameters that depend linearly eration properties for more than 240 crystals with or-
on manifold energy EJ and EJ , E f 0 is the barycentre of dered and disordered structures (Tables 1, 3, 5, 6, 8, and
the 4fN configuration, and Rt are the additional parameters 9). Among the most extensively used SSLs are lasers
with t = 2, 4, and 6. The use of eq. (6) removes the problem based on Nd3+ -doped crystals (Y3 Al5 O12 [94], YAlO3 [95],
of the negative Ω 2 parameter and allows one to get more YVO4 [96], Gd3 Ga5 O12 [94], LiYF4 [97], LiLuF4 [98],
realistic calculated spectroscopic intensity characteristics α-KGd(WO4 )2 [99], GdVO4 [100], LiNbO3 :MgO [101],
βJJ and τrad that adequately correlate with corresponding and some others [102]). Nd3+ ions in crystals can lase at
experimental values. It should be noted here also that the wavelengths of eleven 4f3 –4f3 and one 4f2 5d1 –4f3 channels
evaluation of 4fN –4fN intermanifold J → J ed transition (Fig. 4). The many pumping methods used for obtaining
probabilities of certain Ln3+ ions (e.g. Nd3+ and Er3+ ) in CW and pulsed SE generation in Nd3+ -doped crystals [103]
crystalline materials could be expanded into the vacuum in particular include different types of Xe, Kr, Hg, and W
UV region because the corresponding required reduced lamp pumping sources [93, 112, 113], solar [114] and py-
matrix elements …||U (t) ||… have been calculated (see, rochemical [115] excitation without electric energy con-
e.g. [18, 57, 59]). sumption, LED [116], OPO [702], and LD [117] pumping,
as well as by using electron beam [118] and X-ray [119]
sources. As is shown in Sect. 9 the majority of crystalline
4.2. Laser channels of Nd3+ ions lasers of the new generation, namely with LD pumping
as well as “fibre”-like and waveguide types, also use Nd3+ -
The Nd3+ ion as an activator was the first Ln3+ lasant doped crystals. It should be noted here also that neodymium
in crystals (CaWO4 ) [93]. Because of extremely suit- crystalline lasers (on the base of Y3 Al5 O12 :Nd3+ ceramic)
able spectroscopic properties for SE excitation by differ- offer currently the multi-kilowatt level (up to 100 kW) of
ent pumping techniques Nd3+ lasants have provided gen- CW output power.


condition
Sm3+
1 4
G5/2 → 6 H7/2 TbF3 , ≈ 110K, Xe [123]
LiTbF4 , 300K, las. [124]
3+
Eu
1 5
D0 → 7 F2 Y2 O3 , ≈ 220K, Xe [125]
Tb3+
1 5
D4 → 7 F5 LiYF4 :Gd3+ , 300K, Xe [126]
Figure 5 Known intermanifold 4fN –4fN laser transitions of Sm3+ , Eu3+ , and Tb3+ ions in crystals. Notations as in Fig. 2.
4.3. Visible laser channels of Sm3+ , Eu3+ , and 4.5. Laser channels of Ho3+ ions
Tb3+ ions
Fourteen SE channels have been discovered for Ho3+ acti-
vators (Fig. 7). Presently, the list of laser crystals with Ho3+
At present, each of these ions has only one known lasing ions consists of slightly more than 70 entries (Tables 1, 3,
channel with a single inter-Stark SE transition (Fig. 5). For 5, 6, and 8), which is second only to that of Nd3+ ions in the
visible generation Sm3+ and Tb3+ activators in anisotropic number of generating compounds. The first laser 4f10 –4f10
fluorides use the sensitizing operating laser scheme (see, intermanifold transition of Ho3+ activators in crystals was
e.g. [18,21,66]). The Tb3+ ions, in the case of Sm3+ lasants the 2 µm 5 I7 → 5 I8 channel (CaWO4 :Ho3+ [139]) and the
(Fig. 5), form the structure of their host crystals TbF3 and second one was the ‘green’ 5 S2 → 5 I8 (CaF2 :Ho3+ [141]).
LiTbF4 , and also act as the sensitizers. The majority of articles on the 5 I7 → 5 I8 channel have been
devoted to optimization of pumping conditions, because
Ho3+ lasing at ∼ 2.1 µm is suitable for several important
modern applications due to its eye-safe laser wavelengths
4.4. Laser channels of Dy3+ ions
in the window of high atmospheric transmission. Tunable
holmium 2- µm SE generation shows great potential for re-
The electronic 4f9 configuration of Dy3+ ions gives rise to mote sensing and monitoring of atmospheric CO2 and H2 O
a large number of closely located 2S+1 LJ manifolds re- laser spectroscopic technologies (see, e.g. [154,155]). The
sulting in a very tangled picture of their crystal field split- CO2 gas and water vapour molecules play important roles
ting. Over the past few years the SE generation of Dy3+ in global climate change, including the greenhouse effect
ions as opposed to other Ln3+ lasing activators in different (global warming) [156]. A large number of Ln3+ and TM3+
types of crystals has been studied most productively (see, ion sensitizers (Er3+ , Tm3+ , Yb3+ , Cr3+ , and Fe3+ ) can im-
e.g. [127–132]). It is now possible to excite SE on inter- prove this SE excitation by Xe-flashlamp and LD-pumping
Stark transitions of the seven 4f9 –4f9 channels (Fig. 6) in a techniques [18,21,102,103]. The second 5 S2 → 5 I8 channel
relatively wide spectral range from ∼ 0.57 to ∼ 4.35 µm. It was the first ‘visible’ laser 4fN –4fN intermanifold transi-
is beyond doubt that other new SE channels will soon be tion of Ln3+ lasants in crystals. Spectroscopic investiga-
discovered in Dy3+ -doped compounds, including the low- tions show that SE generation can also be excited on other
energy-phonon crystals. channels in Ho3+ -doped crystals.


condition
1 6
H13/2 → 6 H15/2 β-Ba(Y,Er)2 F8 , 77K, Xe [135]
β-BaYb2 F8 , [127,136]
LaF3 , 300K, las.
2 6
H11/2 → 6 H13/2 LiYF4 , 300K, las. [137]
3 4
F(3)9/2 → [ H9/2 + F11/2 ]
6 6
LiNbO3 a)
[138]
4 [6 H9/2 +6 F11/2 ] → 6 H15/2 CaGa2 S4 :Na+ , 300K, las. [128]
5 [ H9/2 + F11/2 ] → H13/2
6 6 6
CaGa2 S4 :Na , +
[128,129,131]
KPb2 Cl5 , 300K, las.
6 4
F(3)9/2 → 6 H13/2 α-KGd(WO4 )2 , ≈ 180K, Xe [130]
7 4
F(3)9/2 → 6 H11/2 α-KY(WO4 )2 , ≈ 110K, Xe [130]
a)
In the absence of details of pumping conditions used to obtain SE results
in [138], it is desirable to confirm these.
Figure 6 Known intermanifold 4f9 –4f9 laser transitions of Dy3+ ions in crystals. Notations as in Fig. 2.
4.6. Laser channels of Er3+ ions At room temperature this CW 2- µm thulium lasing was
later achieved with W-lamp pumping using a sensitized
The relatively large energy gap between 2S+1 LJ manifolds Y3 Al5 O12 :Cr3+ garnet [140]. Tm3+ ions in crystals are now
of Er3+ ions creates very favourable conditions for SE ex- known to lase over a relatively wide wavelength range
citation at different laser channels. Thus far, generation has (from ∼ 0.348 to ∼ 2.46 µm; Table 10) in their 12 inter-
been achieved at 16 4f12 –4f12 intermanifold transitions in manifold transitions (Fig. 9). The disposition of the energy
numerous fluoride and oxide crystals and spans the spec- levels and luminescence intensity properties of known gen-
tral range from 0.469 to ∼ 4.75 µm (Table 10 and Fig. 8). erating Tm3+ -doped crystals (Tables 1, 3, 5, and 6) allow the
The principal reason for the large number of discovered creation of cascade and cross-cascade [75,202,203] as well
Er3+ laser channels, as in the case of Pr3+ and Ho3+ ions as cross-relaxation [195] laser schemes. It is also known
(see Sects. 4.1 and 4.5), is the relatively small nonradia- that tunable SE in the vacuum UV region can be excited
tive transition probabilities between the low-lying initial at the interconfiguration 4f11 5d1 –4f12 ed-allowed transition
and terminated manifolds involved in SE generation (see of Tm3+ ions in several anisotropic fluoride crystals [204].
Chap. 4 in [18]). The Er3+ ions in fluoride and oxide crys- Yb3+ ions have only one 4f13 –4f13 intermanifold transi-
tals, just as for Ho3+ ions, have spectroscopic properties that tion (2 F5/2 → 2 F7/2 ). Ytterbium SE generation was demon-
are favourable for cascade SE excitation [18, 170]. This strated in the mid-1960s up to 120 K using Xe-flashlamp
very attractive principle of laser action in activated crys- pumping [140, 197]. In double-sensitized garnet crystal
tals was first realized in Er3+ ions by the direct cascade (Y3 Al5 O12 :Cr3+ ,Nd3+ ) the lasing temperature of Yb3+ gen-
scheme 4 S3/2 → 4 I13/2 → 4 I15/2 (CaF2 –YF3 :Er3+ [75, 178]). eration was raised to 210 K [198]. It should be particularly
The overwhelming majority of cascade laser schemes have emphasized here that this articles put start of the detailed
been performed with Er3+ - and Ho3+ -doped crystals (see spectroscopic and SE investigations of Yb3+ -doped crys-
also [149, 173, 179–181, 183, 184]). tals. In the last decade using a pumping technique based on
InGaAs quantum well LDs, which emit in the 0.9–0.98 µm
range, one-micron ytterbium laser action was obtained at
4.7. Laser channels of Tm3+ and Yb3+ ions room temperature. Many scientists believe that Yb3+ las-
ants, due to their small ‘quantum defect’ (the energy differ-
The first laser 4f12 –4f12 intermanifold transition of Tm3+ ence between their generation and excitation transitions),
ions was the 3 H4 → 3 H6 channel (CaWO4 :Tm3+ [186]). which means that little pump power is lost as heat, will


condition
1 5
I7 → 5 I8 CaWO4 , 77K, Xe [139]
3+
(Y,Er)3 Al5 O12 :Tm , 300K, Xe [140]
2 5
S2 → 5 I8 CaF2 , 77K, Xe [141]
3 5
F5 → I5
5
β-BaYb2 F8 , 77K, Xe [142]
4 5
I7 → 5 I8 β-BaYb2 F8 :Er3+ ,Tm3+ , 295K, Xe [142]
5 5
F5 → 5 I6 LiHoF4 , ∼
= 90K, Xe [143]
LiYF4 , ∼
= 190K, Xe [144]
6 5
F5 → 5 I7 ∼ 90K, Xe
LiHoF4 , = [143]
∼
LiYF4 , = 300K, Xe [144]
7 5
S2 → 5 I7 LiYF4 , ∼
= 90K, Xe [145]
YAlO3 , 300K, Xe [146]
8 5
S2 → 5 I6 LiYF4 , ∼
= 90K, Xe [145]
YAlO3 , 300K, Xe [146]
9 5
S2 → 5 I5 LiYF4 , 300K, Xe [145]
10 5
I6 → 5 I7 YAlO3 , Y3 Al5 O12 , Lu3 Al5 O12 , 300K, Xe [147]
11 5
I5 → 5 I7 LiYF4 , ∼
= 116K, Xe [148]
LiYF4 , 300K, las., cascade [149]
12 5
I6 → 5 I8 Gd3 Ga5 O12 , ∼
= 110K, Xe [150]
β-BaYb2 F8 , 300K, las. [151]
13 5
I5 → 5 I6 LiYF4 , 300K, las., cascade [149]
β-BaY2 F8 , 300K, las. [152]
14 5
S2 → 5 I5 LiYF4 , 300K, las., cascade [153]
Figure 7 Known intermanifold 4f10 –4f10 laser transitions of Ho3+ ions in crystals. The dashed line shows the level that is the terminal
for electron–vibration SE transition (channel 4). Notations as in Fig. 2.
be an increasingly attractive alternative to Nd3+ activators 4.8. Laser channels of Sm2+ , Eu2+ , Dy2+ , Tm2+ ,
in crystals for high-power lasers. Currently there are 55 and U3+ ions
known Yb3+ -doped laser crystals (Tables 1, 3, 6, and 8)
and about half of them can very efficiently generate in the
CW and pulsed mode, including femtosecond pulses, as In the early 1960s researchers looking for new crystals con-
well as with LD pumping (see Sect. 9.1). An excellent re- sidered the broad 4fN –4fN −1 5d1 absorption bands and nar-
view on the spectroscopic and SE laser properties of Yb3+ - row 4fN –4fN luminescence lines of Ln2+ ions in fluorite.
containing crystals and their possible applications has been At the same time all potentially attractive activated crystals
published [16]. Recently CW and femtosecond laser action for SE generation were compared with ruby. CaF2 :Ln2+ and
of Yb3+ ions was excited in VSN ceramics based on cu- α-Al2 O3 :Cr3+ have many spectroscopic similarities. Origi-
bic Y2 O3 , Sc2 O3 , and Lu2 O3 sesquioxides, and Y3 Al5 O12 nated luminescent states of Ln2+ ions have long decay times
garnet (see, e.g. [205, 291, 301, 627, 701]; Sect. 6). In last (because the crystallographic sites occupied by Ln2+ ions
years the great interest was newly aroused in developments in CaF2 have an inversion centre of symmetry, these lumi-
of high-power (hundreds watts) CW cryogenically cooled nescence transitions are of the magnetic dipole type). Iron-
ytterbium crystalline lasers (see, e.g. [731–733]). ically, the allowed 4f5 5d1 → 7 F1 transition of Sm2+ ions
in CaF2 crystals was the first laser channel of Ln2+ acti-
vators (Fig. 10) [206]. In the case of SrF2 :Sm2+ crystals


condition
1 4
I13/2 → 4 I15/2 CaWO4 , 77K, Xe [158]
Y3 Al5 O12 :Yb3+ , 300K, Xe [159]
2 4
S3/2 → I11/2
4 *
CaF2 , 77K, Xe [160]
LiYF4 , 300K, Xe [161]
3 4
S3/2 → 4 I9/2 CaF2 * , 77K, Xe [160]
YAlO3 , 300K, Xe [162]
4 4
I11/2 → 4 I13/2 CaF2 -ErF3 -TmF3 , 300K, Xe [163]
5 4
S3/2 → 4 I13/2 CaF2 , 77K, Xe [164]
LiYF4 , 300K, Xe [165]
6 4
F9/2 → I15/2
4
β-Ba(Y,Yb)2 F8 , 77K, Xe [166]
β-BaYb2 F8 , 300K, las. [167]
7 4
S3/2 → I15/2
4
β-BaY2 F8 , 77K, Xe [168]
LiYF4 , 300K, Xe [169]
8 2
G(1)9/2 → 4 I13/2 β-BaY2 F8 , 77K, Xe [168]
9 2
G(1)9/2 → 4 I11/2 β-BaY2 F8 , 77K, Xe [168]
10 4
I9/2 → 4 I11/2 ∼ 110K, Xe, cascade
YAlO3 , = [170]
KPb2 Cl5 , 300K, las. [171]
11 4
F9/2 → 4 I11/2 β-BaYb2 F8 , 300K, Xe [170, 172]
12 4
I9/2 → 4 I13/2 LiYF4 , 300K, las. [173]
13 4
F9/2 → I13/2
4
β-BaYb2 F8 , ∼
= 110K, Xe [174]
14 2
P3/2 → 4 I11/2 LiYF4 , ∼
= 35K, las. [175]
15 2
P3/2 → 4 F9/2 LiYF4 , ∼
= 41K, las. [176]
16 4
F9/2 → 4 I9/2 LiYF4 , 77K, las. [177]
Figure 8 Known intermanifold 4f11 –4f11 laser transitions of Er3+ ions in crystals. Notations as in Fig. 2.
the spectroscopic situation is different, because the absorp- Pulsed mid-IR laser action of U3+ ions in cubic CaF2
tion (4f6 –4f5 5d1 ) and luminescence (4f6 –4f6 ) bands are not crystals (4 I11/2 → 4 I9/2 channel) was achieved under Xe-
overlapped, and the authors of [207] could excite “red” SE flashlamp pumping in 1960 soon after the SE generation
generation in the 5 D0 → 7 F1 md transition at cryogenic tem- in the visible in ruby [214]. Two years later the same U3+
peratures. Laser action of Sm2+ ions was obtained in CaF2 ion generation was discovered in two other fluorite-type
(type II, containing oxygen) fluorite [218] and BaMgF4 crystals, SrF2 and BaF2 [221, 222]. A difficulty of using
crystals [219]. CaF2 , SrF2 , and BaF2 is that the substitution of divalent al-
Eu2+ ions exhibit SE (4f6 5d1 –4f7 channel) only in the kaline earth cations by U3+ activators requires charge com-
thiogallate crystal CaGa2 S4 at 77 K under laser pumping pensation. U3+ ion room temperature SE can be excited in
(Fig. 10) [209]. Unfortunately, this paper contains no addi- tetragonal LiYF4 fluoride at a wavelength of 2.83 µm with
tional explanatory spectroscopic information. laser pumping (α-Al2 O3:Ti3+ ) [216]. In LiYF4 :U3+ crystals
no charge compensation should take place. It is interesting
The generation of SE in CaF2 crystals doped with
to note here that the first crystalline laser with LD-pumping
Dy2+ (5 I7 → 5 I8 channel) and Tm2+ (2 F5/2 → 2 F7/2 ) ions was
was the laser based on the CaF2 :U3+ crystal [223].
achieved in the early 1960s at cryogenic temperatures ac-
cording to [210–212] and [213], respectively. Dy2+ ions
can lase under similar pumping conditions in SrF2 crys-
tals [220]. Unfortunately, crystalline lasers with these two 5. Laser spectroscopic potential
Ln2+ activators did not find wide application due to the ne- of transition metal ions
cessity of cryogenic temperatures and also an undesirable
Ln2+ → Ln3+ degradation process which proceeds under the As mentioned in Sect. 1, historically the first lasant in insu-
action of heat and light. lating crystals was the TM3+ (3d3 ) ion Cr3+ in trigonal leu-


condition
Tm3+
1 3
H4 → 3 H6 CaWO4 , 77K, Xe [186]
3+ 3+
Y3 Al5 O12 :Cr ,Nd , 300K, Xe [140]
2 3
F4 → 3 H5 YAlO3 :Cr3+ , 300K, Xe [187]
3 1
D2 → 3 H4 LiYF4 , 300K, las. [188]
4 3
F4 → 3 H4 β-BaYb2 F8 , LiYbF4 , 300K, las. [189]
β-BaYb2 F8 , 300K, Xe [190]
5 1
G4 → 3 H4 β-BaYb2 F8 , 300K, las. [191]
6 1
G4 → 3 F 3 β-BaYb2 F8 , 300K, las. [191]
7 1
G4 → H6 3
LiYF4 , ∼
= 150K, las. [192]
β-Ba(Y,Yb)2 F8 , 300K, las. [193]
8 1
D2 → H5 3
β-Ba(Y,Yb)2 F8 , 300K, las. [194]
9 1
G4 → 3 H5 β-Ba(Y,Yb)2 F8 , 300K, las. [194]
10 1
I6 → 3 H 4 β-Ba(Y,Yb)2 F8 , 300K, las. [195]
11 1
I6 → F 4
3
β-Ba(Y,Yb)2 F8 , ∼
= 77K, las. [193]
12 3
F4 → 3 H6 LiYF4 F8 :Yb3+ , 300K, las. [196]
Yb3+
1 2
F5/2 → 2 F7/2 CaF2 :Nd3+ , ∼
= 120K, Xe [140]
Y3 Al5 O12 , 77K, Xe and 80K, LED [197,805]
Y3 Al5 O12 :Cr3+ ,Nd3+ , ∼
= 210K, Xe [198]
Y3 Al5 O12 , 300K, Xe, las., LD [199, 200, 729, 730]
2 2
F5/2 → F7/2 2
Sr5 (PO4 )3 F, 300K, las., LD [201, 709]
Figure 9 Known intermanifold 4fN –4fN laser transitions of Tm3+ and Yb3+ ions in crystals. Notations as in Fig. 2.
cosapphire (corundum), α-Al2 O3 , single crystal. The sec- ions [17,67,236]. Laser action of this activator ion has been
ond and third laser-active TM activators were the two TM2+ achieved using the vibronic transitions of the 4 T2 → 4 A2
ions Ni2+ (3d8 ) and Co2+ (3d7 ) in tetragonal MgF2 fluorides. channel in two fluoride crystals (Table 2 and Fig. 11).
There are now six other known 3dN lasing dopants in nu- The Cr2+ ion is the latest TM lasant activator to be used
merous insulating crystals as well as in a few II–IV and III– in crystals [227]. Among several known laser crystals con-
V semiconductor host crystals: TM2+ –V2+ (3d3 ), Cr2+ (3d4 ), taining these 3d4 ions (Table 9) the most promising for ob-
and Fe2+ (3d6 ); TM3+ –Ti3+ (3d1 ); TM4+ –Cr4+ (3d2 )* ; and taining broadly tunable and ultra-short-pulsed generation in
TM5+ –Mn5+ (3d2 ) (Tables 2, 4, 7–9). A comprehensive the mid-IR with LD pumping is ZnSe:Cr2+ [53, 234, 235].
analysis of the spectroscopic background of TM-doped Fe2+ ions can generate in the very important mid-IR
crystalline lasers with many examples and some of their spectral region ranging from ∼ 3.53 to ∼ 4.54 µm (Table 10)
applications has been published recently [17, 67]. for many applications, especially in remote sensing. This
3d6 activator was the first lasant to be used in a semicon-
ductor host crystal (n-type InP:Fe2+ [229]). Its SE gener-
5.1. Lasing transitions of V2+ , Cr2+ , Fe2+ , Co2+ , ation was excited both in electronic (n-InP:Fe2+ ) and vi-
and Ni2+ ions bronic (ZnSe:Fe2+ , with very wide tuning) transitions of
the 5 T2 → 2 E channel (Fig. 11).
V2+ ions are isostructural with Cr3+ ions, and therefore The 3d7 electronic configuration of Co2+ ions can be
their spectroscopic properties and the structure of their en- considered as 3d10 − 3 , i.e. three electrons are required to
ergy levels are similar. The difference is included in the fill the 3d shell. Therefore, due to this electron–hole sym-
crystal-field parameter Dq – it is always less for divalent 3d3 metry the structure of the terms of 3d7 and 3d3 ions is
identical, but the sequence of energy levels is reversed. A
*
This chromium valency should be refined. similar situation is also observed for 4fN electronic con-


condition
Sm2+
1 4d5 5d1 → 7 F1 CaF2 , ∼
= 45K, Xe [206]
2 5
D0 → F17
SrF2 , 4.2K, Xe [207]
3 4d5 5d1 → 7 F1 CaF2 , 65–210K, las. [208]
Eu2+
1 4f6 5d1 → 4f7 CaGa2 S4 , 77K, las. [209]
Dy2+
1 5
I7 → 5 I8 CaF2 , 77K, Xe [210–212]
2+
Tm
1 2
F5/2 → 2 F7/2 CaF2 , 4.2K, Xe [213]
3+
U
1 4
I11/2 → 4 I9/2 CaF2 , 77K, Hg, Xe [214]
CaF2 , 300K, Xe [215]
LiYF4 , 300K, las. [216]
Figure 10 Known SE channels of Sm2+ , Eu2+ , Dy2+ , Tm2+ , and U3+
2 4
I11/2 → 4 I9/2 CaF2 , 77K, Xe [217]
ions in crystals. Notations as in Fig. 2.
figurations, as, for example, in Ce3+ (4f1 ) and Yb3+ (4f13 ), Fig. 11 shows simplified energy level schemes for Ni2+
Nd3+ (4f3 ) and Er3+ (4f11 ), and others. As for Fe2+ consid- ions in two laser crystals. In tetragonal MgF2 the Dq pa-
ered above, Co2+ ions also lase on both electronic and vi- rameter is less than that in cubic MgO. As is shown, the SE
bronic transitions (Fig. 11). The tuning range of SE gen- generation of these 3d8 activator ions proceeds between
eration for the MgF2 :Co2+ crystal is large enough to be levels of the 3 T2 and 3 A2 states. The energy disposition of
interesting for practical applications [62]. laser levels depends on the strength of the octahedral crystal


condition
V2+
1 4
T 2 → 4 A2 MgF2 , 77K, Xe [225, 226]
2+
Cr
1 5
E → 5 T2 ZnS, ZnSe, 300K, las. [227, 228]
2+
Fe
1 5
T2 → 5 E n-InP, ≈ 2K, las. [229]
2 5
T2 → E5
ZnSe, ≈ 180K, las. [230]
2+
Co
1 4
T2 → 4 T1 MgF2 , 77K, Xe [225, 231]
2 4
T2 → 4 T1 MgF2 , 77K, Xe [225, 231]
MgF2 , 300K, las. [232]
2+
Ni
1 3
T 2 → 3 A2 MgF2 , 77–240K, Xe [233]
Figure 11 Known SE channels of TM2+ ions in insulating and semicon-
2 3
T 2 → A2
3
MgO, 77K, Xe [225]
ductor laser crystals. Notations as in Fig. 2.
field of these compounds [236]. In both cases, cooling of the Cr3+ ions, which were the first lasing activators in crys-
generating crystals is required. The low-temperature laser tals, usually enter octahedral sites, and the 4 T2 and 4 T1
action of Ni2+ ions has also been achieved in four other crys- states of the 4 F term undergo a strong interaction [236].
tals: MnF2 [225], Ca2 Y2 Mg2 Ge3 O12 [237], KMgF3 [238], Due to the strong octahedral crystal field in ruby the 4 T2
and Gd3 Ga5 O12 [17] (Tables 2, 4, and 7). manifold of its Cr3+ ions is located ∼ 2300 cm−1 above
the 2 E state [254]. Therefore, in the case of α-Al2 O3 :Cr3+
only the 2 E → 4 A2 channel is luminescent and lasing. Be-
5.2. Lasing transitions of Ti3+ , Cr3+ , Cr4+ , and sides ruby, three other Cr3+ -doped crystals are known
Mn5+ ions that can generate on the R-lines of this doubly forbid-
den (by both parity and spin) transition (Y3 Al5 O12 [255],
The single 2 D term of Ti3+ ions in an octahedral crystal BeAl2 O4 [256], and Be3 Al2 Si6 O18 [257]). The majority of
field is split into two states, 2 E and 2 T2 (Fig. 12), which are known Cr3+ -doped laser oxides and fluorides (Tables 2, 4,
connected by intense vibronic transitions. The first laser ac- and 7) can generate in the 4 T2 → 4 A2 intermanifold transi-
tion of these activator ions was achieved in α-Al2 O3 [239]. tion (Fig. 12). Because this lasing channel is not spin for-
α-Al2 O3 :Ti3+ crystals are now widely used for obtaining bidden it has extensive vibronic transitions which give rise
broad tunable SE generation (∼ 0.66 to ∼ 1.18 µm) and in to tunable SE generation (see, e.g. [244,258,259]). Another
pico- and femtosecond lasers (see, e.g. [251]). The second case is known where SE occurs from two thermally popu-
crystal to be used for tunable lasing with these 3d1 ions was lated initial states 2 E and 4 T2 (BeAl2 O4 :Cr3+ [244]). Cr3+
hexagonal chrysoberyl BeAl2 O4 :Ti3+ [252, 253].


condition
Ti3+
1 2
E → 2 T2 α-Al2 O3 , 300K, las. [239]
α-Al2 O3 , 300K, Xe [240–242]
3+
Cr
1 2
E → 4 A2 α-Al2 O3 , 300K, Xe [1]
2 2
E → 4 A2 α-Al2 O3 , 300K, las. [243]
3 2
E, T2 → A2
4 4
BeAl2 O4 , 300K, las. [244]
4 4
T2 → 4 A2 KZnF3 , 260K, las. [245]
(La,Lu)3 (Lu,Ga)2 Ga3 O12 , 300K, las. [246]
Cr4+
1 3
T2 → 3 A2 Mg2 SiO4 , 300K, las. [247, 248]
Mg2 SiO4 , 300K, Xe [249]
5+
Mn
Figure 12 Known SE channels of Ti3+ , Cr3+ , Cr4+ , and
1 1
E → 3 A2 Ba3 (VO4 )2 , 300K, las. [250]
Mn5+ ions in crystals. Notations as in Fig. 2.
ions possess very similar laser properties in a large family is a topic of extensive discussion (see, e.g. [17, 67, 247,
of disordered compounds having the Ca-gallogermanate 248, 264–267]). Many investigators have suggested that in
structure [259–261], which have in the 4 T2 → 4 A2 channel crystals of Mg2 SiO4 :Cr grown under oxidizing conditions
the greatest tuning width of the SE wavelength of about this broadband generation is due to Cr4+ ions in tetrahedral
3300 cm−1 in the near-IR region. Some fluorides with the sites and connects with the 3 T2 → 3 A2 channel (Fig. 12).
colquiriite structure (e.g. LiSrAlF6 and LiSrGaF6 ) doped Actually, the situation is very complex, as the Mg2 SiO4
with Cr3+ ions are very attractive active media for the cre- structure permits the formation of several types of centres
ation of LD-pumped all-solid-state pico- and femtosecond both with Cr3+ and Cr4+ . An analogously complex situa-
laser oscillator and amplifier systems [262, 263]. tion also exists in the laser Cr-doped Y3 Al5 O12 garnet with
The nature of the broadband tunable laser action of Cr- co-doping ions. The phototropic colour centres that form in
containing crystals, particularly Mg2 SiO4 and Y3 Al5 O12 , this crystal complicate the understanding of the nature of

Figure 13 Progress in the development of LD-pumped Y3 Al5 O12 :Nd3+ ceramic CW lasers emitting at wavelengths of two 4 F3/2 → 4 I11/2
and 4 F3/2 → 4 I13/2 generation channels at 300K with end (longitudinal, open circles and triangles) and side (transverse, filled circles and
triangle) pumping geometries. The CW laser output power is given in mW, W, kW. In understanding some date see also Table 11.
the broadband tunable laser operation (1.35–1.55 µm). SE 6. Laser potential

generation in this spectral range of LiNbGeO5 , Y2 SiO5 , of oxide crystalline ceramics
Ca2 GeO4 , and LiScGeO4 crystals doped with chromium
ions has also been the subject of detailed studies [268–271]. Laser gain materials based on Ln3+ -ion doped (in partic-
It is possible that lasing chromium has only a four-valence ular, Nd3+ and Yb3+ ) highly transparent cubic Y3 Al5 O12
state in these compounds [270–275]. The first assured at- and RE2 O3 ceramics (RE = Sc, Y, and Ln) are the focus of
tempt of the theoretical calculation of the manifold energies many research groups (see, e.g. [280, 282, 298, 299, 447]).
and the transition probabilities of tetrahedrally coordinated It is enough to note here the results that were achieved
Cr4+ ions in the two silicate laser crystals Mg2 SiO4 and concerning the creation of high-power Nd3+ :Y3 Al5 O12 ce-
Y2 SiO5 by the electronic structure calculation method was ramic lasers with LD pumping. Because of novel ce-
done in [120], independently of ligand field theory (see, ramic technology, only in the last two years has the one-
e.g. [67]). It is important to note here that Y3 Al5 O12 :CaO micron neodymium lasing channel (4 F3/2 → 4 I11/2 ) CW out-
garnet crystals doped with chromium ions are widely used put power been increased from a few hundreds milli-
as saturable absorbers for Q-switched SSLs [276, 277]. watts to the 100 kW range. This remarkable progress is
The first laser crystals with 3d2 ions were the Mn5+ - summarized in Fig. 13. A new generation of laser crys-
doped vanadates Ba3 (VO4 )2 and Sr3 (VO4 )2 [278], the talline ceramics was fabricated by the recently developed
SE of which involved generation in the 1 E → 3 A2 chan- revolutionary VSN method without a high-pressure pro-
nel (Fig. 12). cess, where the raw materials were prepared by nanocrys-

4 5 2
R ~ 99.5% 6 6 R~~ 93%

1.06 µm 1.06 µm Figure 14 Schematic drawing of quasi-CW
Nd3+ :Y3 Al5 O12 ceramic laser: 1 – hermetic metal-
lic chamber; 2 – quartz tube; 3 – cartridge with non-
pressed explosive pyrotechnical KClO4 +Zr pow-
der; 4 – Nd3+ :Y3 Al5 O12 laser ceramic rod; 5 – tung-
7
sten wire fuse; 6 – electrical contacts; 7 – metal
8 plate; 8 – condensing rubber collar; 9 – resonator
mirror with high reflectivity on lasing wavelength;
9 3 1 10 10 – output coupler (mirror).
talline technology [10]. Investigations have shown that 1 nm [292]. Characterization showed that the main optical,
the Y3 Al5 O12 :Nd3+ ceramic lasers demonstrate practically laser, nonlinear, and spectroscopic properties as well as the
identical efficiency and output power as lasers based on thermal conductivity and microhardness of Y3 Al5 O12 and
single crystals of the same material (see, e.g. [12,13,289]). RE2 O3 ceramics are almost identical to or better than those
However, this new generation of laser ceramics has signifi- of single crystals of the same materials [287, 546].
cant advantages over laser Y3 Al5 O12 :Nd3+ single crystals. Prior to a consideration of some of their specific
They can be obtained in large sizes and at low cost and properties, it should be emphasized here that the re-
with the required high Ln3+ ion concentration, as well as search history of laser ceramics began in 1966 with hot-
in the form of very large multilayer plates for multifunc- pressed CaF2 :Dy2+ polycrystals [296]. The second ce-
tional lasers [12, 546]. These ceramics provide clear evi- ramic laser was demonstrated only ten years later (Y2 O3 –
dence that new VSN technology is not limited to Y3 Al5 O12 ThO2 :Nd3+ [297]).
doped with Nd3+ , Er3+ , and Yb3+ lasants, but that it is a Due to the promising practical value of Nd3+ -doped
really universal method for fabricating other new ceramic Y3 Al5 O12 and RE2 O3 (in particular, Y2 O3 ) laser ceramics
SSL materials. Quite recently efficient CW generation from it is worth briefly discussing their general distinctive spec-
Nd3+ - and Yb3+ -ceramic lasers based on refractory Ia3 cu- troscopic characteristics. Fig. 14 shows the three-band lu-
bic Sc2 O3 , Y2 O3 , (Gd0.5 Y0.5 )2 O3 (or YGdO3 ), and Lu2 O3 minescence spectra of Nd3+ activator ions (4 F3/2 → 4 I9/2–13/2
sesquioxides was obtained (see Table 11). It should be noted channels) in Y3 Al5 O12 and Y2 O3 ceramics with an indica-
here that due to very high melting temperatures (2400– tion of their intermanifold luminescence branching ratios
2500 ◦C) and structural phase transitions (at ∼ 2280 ◦C βJJ . Due to the essential difference in the crystal fields
for Y2 O3 [295]) obtaining single crystals of some cubic (oxygen coordination, hypersensitive absorption interman-
sesquioxides with perfect optical quality and large sizes by ifold transitions, etc. [18, 21]) of these ceramic materials,
existing melt-growth methods is impracticable at present. the βJJ ratios of their lasing channels are quite differ-
The preparation by VSN-process of practically fully ent. As seen from Fig. 15, for Y3 Al5 O12 :Nd3+ ceramics the
transparent undoped and Ln3+ -doped Y3 Al5 O12 and RE2 O3 branching ratio β J,11/2 of the 4 F3/2 → 4 I11/2 channel is about
ceramics contains several important steps [10, 12, 546, 1.6 times larger than the β J,9/2 ratio of the 4 F3/2 → 4 I9/2
727]. Aqueous solutions of Al, Y, and Ln chlorides are channel. However, for Y2 O3 :Nd3+ ceramics the spectro-
added dropwise and then mixed with an aqueous solution scopic picture is quite the opposite. The branching ratio
of ammonium hydrogen carbonate or urea (NH4 HCO3 , β J,11/2 of the 4 F3/2 → 4 I11/2 channel is about 1.2 times less
NH4 SO4 ). Steps of filtration and washing with water are than β J,9/2 of the 4 F3/2 → 4 I9/2 channel.
then repeated several times, followed by drying for 2 days Analysis has shown also that the probability of sponta-
at about 100 ◦C. The precursor thus obtained, containing neous transitions for the various 4 F3/2 → 4 I(J =9/2−15/2)
particles of 10 nm in size, is calcined at 1000–1200 ◦C to channels of Nd3+ ions in different crystalline hosts de-
produce the raw oxide powder with a particle size of about pends primarily on the well-known intensity parameters Ω t
100 nm. This powder is milled with solvent, binder, and of the fourth and sixth rank, because the matrix elements
dispersion medium for 24h. The milled slurry is put in a 4 F3/2 U (2) 4 IJ for ed transitions between the 4 F3/2 and
4
gypsum mould and dried, and the desired form is obtained. IJ manifolds are equal to zero (see Table 3.2 in [18]). It
After removing the organic components by calcining, this should be particularly emphasized here that Ω t parameters
material is vacuum sintered at ∼ 1750 ◦C for several hours. describe the efficiency of the interaction between the Nd3+
It should be noted here that the sintering temperature for ions and their surrounding crystal field. Therefore, the in-
RE2 O3 is about 700 degrees lower than the melting temper- termanifold luminescence branching ratios (see eq. (1)) can
ature, so it is much easier to fabricate large-size RE2 O3 , par- be represented as dependent on only one parameter – the
ticularly Y2 O3 ceramics, compared to single-crystal melt- spectroscopic quality parameter X Nd [18,21,300] – which
growth methods. The porosity of the highly transparent is defined as
Y3 Al5 O12 and RE2 O3 ceramics obtained is only of the Ω4
1 ppm level and their grain boundary width is less than XNd = . (7)
Ω6

Table 11 Some data on the latest research achievements of laser crystalline ceramics fabricated by the VSN method [10] a) .
ceramic space laser and nonlinear-laser characteristics c)

group
b) Ln3+ lasants and their SE channels Yb3+ ωSRS d)
fs-lasing cm−1
Nd3+ Er3+ Yb3+
Y2 O3 Th7 4
F3/2 → 4 I11/2 [290] e) 2
F5/2 → 2 F7/2 [291] e) 188 fs ∼ 378 [351]
0.16 W f) 9.2 W [712] f) [714, 715,
717–719]
Y3 Al5 O12 Oh 10 4
F3/2 → 4 I9/2 [713] e) 2
F5/2 → 2 F7/2 ∼ 370 [352, 353]
0.64 W f) [701] e)
0.35 W [712] f)
4
F3/2 → 4 I11/2
[12,283] e)
1470 W [13] f)
∼ 45 kW g)
∼ 67 kW h)
(Xe [723] i) ,
Pth [722] j)
4
F3/2 → 4 I13/2 [286] e)
36 W [288] f)
(Y0.5 Er0.5 )3 Al5 O12 k)

Oh 10 4
I11/2 → 4 I13/2 [688] e)
∼ 22 W
(Xe [724]) e,f)
4
S3/2 → 4 I9/2
(Xe [726]) m)
Sc2 O3 Th7 2
F5/2 → 2 F7/2 [205] e) ∼ 419 [688]
0.42 W f)
(Gd0.5 Y0.5 )2 O3 l)
Th7 4
F3/2 → 4 I11/2 [294] e)
0.005 W f)
Lu2 O3 Th7 4
F3/2 → 4 I11/2 [293] e) 2
F5/2 → 2 F7/2 357 fs [714] ∼ 392 [716]
0.01 W f) [715] e)
∼ 2 W [714] f)
a)
It is known also several laser crystalline ceramics which were fabricated by the solid-state reaction (SSR) method (see, e.g.
Japanese patents JP3463941 and JPS3243278, as well as [724]: Y3 (Al,Sc)2 Al3 O12 :Nd3+ [725] and Y3 (Al,Sc)2 Al3 O12 :Yb3+ [711]
for CW and femtosecond lasers. Quite recently, to these modern routes (SSR and VSN) for laser oxide ceramics fabrication, a new
attractive HPCSC method was reported (at March 29 on 241. Session of All-Moscow Seminar on physics and spectroscopy of laser
crystals, see also [804]). The method is based on the high-pressure colloidal slip-casting process via which lasing Nd3+ :Y3 Al5 O12
ceramics was obtained.
b)
Grains of the ceramics are randomly oriented nano- or micro-size single crystals.
c)
Majority laser data were achieved with LD-pumping in CW-mode generation.
d)
Promoting vibration mode of the observed the picosecond high-order Stokes and anti-Stokes generation.
e)
Pioneer publication.
f)
Best published output power.
g)
Was presented by T.F. Soules, M.D. Rotter, S.N. Fochs, R.M.Yamamoto, C. Parks, B. Bhachu, J. Otto, T. Shigeta, S. Yuminani,T.
Yanagitani, and H. Yagi in: The 9-th Annual Direct Energy Symposium of the Directed Energy Professional Society (August 2006,
Kauai, Hawaii, USA).
h)
Information from H.Yagi presentation in: 2-nd Laser Ceramic Symposium (November 2006, Tokyo, Japan).
i)
Pulsed laser action with Xe-flashlamp pumping.
j)
Quasi-CW generation with pyrotechnical (Pth) lamp pumping (Fig. 14).
k)
Solid solution of Y3 Al5 O12 and Er3 Al5 O12 in the ratio 1:1, can be written also as (Y,Er)3 Al5 O12 .
l)
Solid solution of Gd2 O3 and Y2 O3 in the ratio 1:1, can be written also as GdYO3 .
m)
Pulsed SE was achieved at ∼ 110K with Xe-flashlamp pumping.

Figure 15 Room temperature three-band lumi-

nescence spectra of Nd3+ ions (4 F3/2 → 4 I11/2 and
4
F3/2 → 4 I13/2 channels) in laser Y3 Al5 O12 and Y2 O3
ceramics with an indication of their intermani-
fold luminescence branching ratios βJJ . The in-
set shows the dependence of βJJ on X Nd and a
simplified scheme of the intermanifold 4 F3/2 → 4 IJ
luminescence transitions for Nd3+ -doped materi-
als [18,21]. For β J,15/2 (X Nd ) the scale has been
increased ten times. The dashed lines indicate the
spectroscopic quality parameter X Nd for Nd3+ las-
ant in Y3 Al5 O12 and Y2 O3 ceramics.
Because for the 4 F3/2 → 4 I9/2–15/2 transitions the Amd

JJ prob- using the fitting with measured βJJ values in [290], the
abilities are equal to zero, the AedJJ probabilities for lumi-
spectroscopic quality parameters for the first neodymium
nescence channels originate from the initial laser 4 F3/2 state laser ceramics fabricated by VSN method [10] were esti-
mated: X Nd = 0.43± 0.07 for Y3 Al5 O12 and X Nd = 1.6±
64π 4 e2 n̄(n̄2 + 2)2 0.2 for Y2 O3 . It should be noted here also that the known
Aed
JJ = values of βJJ (X Nd ) for Nd3+ -doped Y3 Al5 O12 and Y2 O3
3h(2J + 1)λ̄3 9
4 t 4 2 single crystals are 0.43 ± 0.06 [18] and 1.8 ± 0.5 [302],
× Ωt F 3/2 U IJJ . (8) respectively. Comparison once again emphasizes that the
t=4,6 spectroscopic and laser properties of these ceramics and
single crystals of the same materials are very similar.
By substituting eq. (8) into eq. (1), the analytical depen-
dences can be obtained as
6.1. Stimulated and spontaneous
(aJ XNd + bJ )λ̄3JJ
βJJ = (9) Raman scattering
(aJ XNd + bJ )λ̄3JJ
J The high optical quality of the new generation of undoped
and Ln3+ -doped Y3 Al5 O12 , Sc2 O3 , Y2 O3 , and Lu2 O3 laser
where the constants aJ and bJ are equal to the squared
host ceramics is convincingly evidenced by recent exper-
matrix elements:
iments on the excitation in these materials of high-order
2
Stokes and anti-Stokes Raman lasing in the visible and
aJ = 4 F3/2 U (4) 4 IJ near-IR regions with picosecond pumping [351–353, 688,
2 (10) 716]. For illustration, several selected spectra of stimu-
4 (6) 4
and bJ = F3/2 U IJ . lated (SRS) and spontaneous Stokes Raman scattering of
Y3 Al5 O12 and Y2 O3 ceramics and single crystals are shown
The inset of Fig. 15 shows a plot of the analytical depen- in Figs. 16–19. It should be noted that Stokes and anti-
dences (eq. (9)). These dependences are universal in char- Stokes generation spectra were obtained under steady-state
acter and, in particular, they can be used for the analysis of (ss) excitation conditions:
Nd3+ -doped nanocrystalline ceramics. Based on these fun- 1
damental properties of the βJJ (X Nd ) dependences and by τp T 2 = (11)
π∆νR

Figure 16 Steady-state SRS spectra of undoped Y3 Al5 O12 ceramics (l = 40 mm) and Nd3+ -doped Y3 Al5 O12 single crystals (C Nd ≈
1 at.%, l = 50 mm) recorded at 300 K with picosecond pumping in the near-IR (λf1 = 1.06415 µm) and visible (λf2 = 0.53207 µm)
regions [353]. Wavelengths of all lines are given in µm and their intensity is shown without correction for spectral sensitivity of recording
system of used set-up (see inset). The pump lines are marked by asterisks. Stokes and anti-Stokes lasing lines related to SRS-active
vibration modes ωSRS ≈ 370 cm−1 are indicated by horizontal scale lines.

Figure 17 Room temperature spontaneous

Stokes Raman scattering (A1g , Eg , F2g ) spec-
tra of undoped Y3 Al5 O12 ceramics and sin-
gle crystals [353]. The Raman shifts of the
most intense lines are given in cm−1 .
where τ p is the pumping pulse duration (Fig. 18) and T 2 The C-modification of the yttrium sesquioxide Y2 O3
and ∆νR are the dephasing time (∼ 5.7 ps for Y3 Al5 O12 and with bixbyite mineral (Fe,Mn)2 O3 structure crystallizes in
∼ 8 ps for Y2 O3 ) and the linewidth of the strongest spon- the Ia3 cubic system with 16 formulae per unit cell [687],
taneous Raman scattering lines determined by a mecha- where 24 Y occupy the C2 sites and the other 8 Y are located
nism of vibronic phase relaxation and connected with SRS- in centrosymmetric C3i crystallographic positions. As the
active vibration modes of the Y3 Al5 O12 and Y2 O3 materials Y2 O3 structure is body-centred, its primitive cell contains
(Figs. 17 and 19). 40 atoms and hence 3N = 120 degrees of vibration freedom.
The 80 atoms of the Ia3d primitive cell of the Y3 Al5 O12 The irreducible representations for its optical and acoustical
garnet crystals have 3N = 240 degrees of freedom, which, modes at k = 0 are
according to factor group analysis and symmetry degener-
acy [303], give rise to 98 vibration modes belonging to the ΓN = 4Ag + 4Eg + 14Fg + 5A2u + 5Eu + 17Fu . (13)
following irreducible representations at k = 0 (centre of
the Brillouin zone): Factor group analysis predicts 22 Raman active modes (4Ag
+ 4Eg + 14Fg ), 17 Fu modes should appear in IR spec-
ΓN = 3A1g + 8Eg + 14F2g + 5A1u + 5A2u + 5A2g tra (among them one Fu is the acoustic mode), and (A2u ,
Eu ) species are both Raman and IR inactive. For the Ia3
+ 10Eu + 14F1g + 16F2u + 18F1u . (12) structure, spontaneous Raman and IR spectra are mutually
exclusive since there are no vibration modes that are both
Of these, 25 (A1g , Eg , F2g ) modes and 17 (F1u ) modes Raman and IR active. The vibration modes (Au + Eu +
should appear in the spontaneous Stokes Raman scatter- 3Fu ) of C3i octahedra (YO6 9− ) are Raman inactive [439].
ing and IR spectra, respectively, as well as the acoustic, In much the same manner as for the Y3 Al5 O12 crystalline
triply degenerated F1u mode. As can be seen from Fig. 17 compounds, in the case of Y2 O3 single crystals and ceram-
the spontaneous Stokes Raman spectra of Y3 Al5 O12 single ics the spontaneous Stokes Raman spectra are practically
crystals and VSN crystalline ceramics are practically iden- indiscernible (Fig. 19).
tical and possess the strongest lines at ∼ 370 cm−1 . These Sc2 O3 has the Ia3 cubic structure in perfect analogy
lines may be attributed to the internal A1g and F2g vibra- to the C-modification of the Y2 O3 sesquioxide. Compari-
tion modes whose frequencies coincide for the S4 tetrahe- son confirms that the spectral composition of spontaneous
dral AlO4 5− and C3i octahedral AlO6 9− groups. The lasing Stokes Raman scattering spectra of Sc2 O3 and Y2 O3 ce-
components of high-order Stokes and anti-Stokes steady- ramics is very similar (see Figs. 19 and 20).
state generation in Y3 Al5 O12 single crystals and ceram- Comparative SRS experiments on first-order Stokes
ics were identified by these SRS-active optical phonons threshold generation measurements for Y3 Al5 O12 , Y2 O3 ,
ωSRS ≈ 370 cm−1 (Fig. 16) [352, 353]. Sc2 O3 , and Lu2 O3 ceramics under the same steady-state

Figure 18 Steady-state SRS spectra of undoped Y2 O3 ceramics (l = 40 mm) recorded at 300K with pumping in a) the near-IR and b)
the visible regions [351]. The inset shows a schematic of the picosecond laser pumping set-up used. Stokes and anti-Stokes lasing lines
related to SRS-active vibration mode ωSRS ≈ 378 cm−1 are indicated by the horizontal scale lines. Other notations as in Fig. 16.

Figure 19 Room temperature spontaneous Stokes Raman scattering (Ag , Fg ) spectra of undoped Y2 O3 ceramics and single crys-
tals [351]. Zero corresponds to Ar ion laser excitation radiation at a wavelength of 0.5145 µm. Other notations as in Fig. 17.

Figure 20 Room temperature spontaneous Stokes Raman scattering (Ag , Fg ) spectra of undoped Sc2 O3 ceramics [688]. Notations as
in Fig. 17.
pumping conditions at a wavelength of λf1 = 1.06415 µm ferent ceramic sample lengths. The SRS data obtained for
give rise to the following Raman gain coefficients [351– Y3 Al5 O12 , Y2 O3 , Sc2 O3 , Lu2 O3 ceramics correlate rea-
St1
353, 688, 716]: gssR = 0.1 ± 0.02 cm/GW at λSt1 = sonably well with the linewidth of their strongest Raman
1.1078 µm for Y3 Al5 O12 , gssR
St1
= 0.6 ± 0.08 cm/GW at shifted lines (see, e.g. ∆νR values in Figs. 17, 19, and 20).
λSt1 = 1.1088 µm for Y2 O3 , gssR St1
= 0.75 ± 0.12 cm/GW
at λSt1 = 1.1138 µm for Sc2 O3 , and gssR St1
= 0.3 ±
0.05 cm/GW at λSt1 = 1.1684 µm wavelength for Lu2 O3 6.2. Some physical properties
St1
(see Fig. 21). Considering that Sc2 O3 has the biggest gssR and possible applications
value, its SRS spectra obtained for the same pumping power
density and sample length contain many more Stokes and As stated above, Y3 Al5 O12 :Nd3+ garnet VSN ceramics are
anti-Stokes lines. It should be noted here that the spec- practical advanced active materials for LD-pumped multi-
tra shown in Figs. 16, 18, and 21 were recorded for dif- kilowatt industrial lasers, and nowadays these ceramics are

Figure 21 Steady-state SRS spectra of undoped Sc2 O3 ceramics (l ≈ 20 mm) recorded at 300 K with picosecond laser pumping
in a) the near-IR and b) the visible regions [688]. The inset shows a schematic of the picosecond laser pumping set-up used. Stokes
and anti-Stokes lasing lines related to SRS-active vibration mode ωSRS ≈ 419 cm−1 are indicated by the horizontal scale lines. Other
notations as in Fig. 16.

Figure 22 Imprint images of a dia-

mond indenter on a) the {100} surface of
Y3 Al5 O12 single crystal and b) on a surface
of Y3 Al5 O12 ceramic; c) shows the scheme
of the imprint analysis. The 10 µm scale bar
refers to both images. Other notations as in
Table 12.
Table 12 Microhardness and brittleness (brit-

characteristic ceramic Y3 Al5 O12 single crystal tle failure) for Y3 Al5 O12 and Y3 Al5 O12 :Nd3+
Y3 Al5 O12 Y3 Al5 O12 :Nd3+ ceramics as compared with Y3 Al5 O12 single
crystals [287].
H (GPa) a) 16.0 c) 15.5 d) 15.5 c) 14.5 c) 14 d)
1/2 b) c) d) c) c)
K 1C (MPa m ) 8.7 8.8 8.8 1.8 1.86 d)
a)
H = 185P/d2 is the microhardness, where P is the load on the diamond indentor and d is the diagonal of the indentor im-
print (Fig. 22).p p
b)
K1C = 0.016 E/H 3 P/C is the brittleness, where E is Young’s modulus and C is the crack length (Fig. 22).
c)
With mechanical polishing.
d)
With chemical polishing.
used as commercial SSL materials [690]. Some of the im- here λ is in µm and coefficients A = 2.282, B =
portant physical properties of this material have been mea- (0.108858)2 , C = 3.27644, and D = (16.8147)2 for
sured. Comparative experiments [289] using the steady Y3 Al5 O12 [694], and A = 2.5503, B = (0.12626)2 ,
heat flow method [691] have shown that the room tem- C = 1.5839, and D = (16.031)2 for Y2 O3 [695].
perature thermal conductivities of Nd3+ -doped (C Nd ≈ There is no doubt that Ln3+ -doped Y3 Al5 O12 and
1 at.%) Y3 Al5 O12 ceramics and single crystals are prac- RE2 O3 novel laser ceramics will challenge the correspond-
tically the same: ∼ 0.107 and ∼ 0.105 W/K · cm, respec- ing single crystals for many practical applications in the
tively. This means that in high-power laser applications very near future. Apart from ‘bulk’ ceramics, multilayer
Y3 Al5 O12 :Nd3+ ceramics can have the same thermal per- structures in particular also look very promising. Accord-
formance as Y3 Al5 O12 :Nd3+ single crystals. ing to the manufacturing process of ceramics, multilayer
Quite recently mechanical characteristics such as mi- laser components can be fabricated together, whereas this
crohardness (H) and brittleness (K 1C ) of Y3 Al5 O12 and is impossible with the existing crystal growth methods.
Y3 Al5 O12 :Nd3+ garnet ceramics were measured [287] us- Concerning RE2 O3 :Nd3+ ceramics, one can expect that
ing the traditional indentation and scratching methods (see, these novel laser materials with their unique physical prop-
e.g. [692,693]). The main results obtained in [287] are given erties and technological capabilities, together with Nd
in Table 12 and shown in Fig. 22. As is evident from Ta- HAP-4 glass and disordered cubic fluorides, as well as
ble 12, mechanically and chemically polished Y3 Al5 O12 YSr5 (PO4 )3 F:Yb3+ crystals, would be rather attractive for
and Y3 Al5 O12 :Nd3+ ceramics exhibit a small (10–15%) in- experiments on the realization of the laser fusion concept
crease of the microhardness. At the same time these garnet (see, e.g. [37,38,49,50]). To illustrate this expectation more
ceramics feature a brittleness K 1C about five times greater clearly, the corresponding spectroscopic and thermal pa-
than that of Y3 Al5 O12 :Nd3+ single crystals. This is an indis- rameters of Y2 O3 :Nd3+ ceramics as possible candidates for
putable practical advantage of novel crystalline ceramics. LD-pumped high-energy SSL systems for laser fusion reac-
The refractive indexes over a wide spectral range (from tor drivers have been plotted for comparison (Fig. 23). This
∼ 0.4 to ∼ 5 µm) of undoped Y3 Al5 O12 and Y2 O3 ceram- plot was produced from data as applied to the “KOYO”
ics have been measured by the prism and interferometric inertial fusion energy reactor (see, e.g. [38, 56]). Experts
methods [694, 695]. A fit to the Sellmeier equation from the Institute of Laser Engineering of Osaka Univer-
sity [38, 56] prefer the Nd HAP-4 glass for LD-pumped
Aλ2 Cλ2 laser drivers, while Sr5 (PO4 )3 F:Yb3+ single crystals have
n2 − 1 = + (14) been the focus of attention at the Lawrence Livermore Na-
λ2 − B λ2 − D

Figure 23 Comparative plot of certain

spectroscopic and physical properties of se-
lected Nd3+ - and Yb3+ -doped SSL materials
(Nd HAP-4 glass [56], Sr5 (PO4 )3 F:Yb3+ for
two lasing polarizations [49, 50], and Yb3+ -
and Nd3+ -doped Y3 Al5 O12 single crystals)
which are undergoing experiments with the
aim of producing LD-pumped slab ampli-
fiers for laser fusion reactor drivers. The
positions in the plot of Nd3+ -doped laser
SiO2 glass, disordered fluoride crystals, and
Y2 O3 ceramics are subject to refinement af-
ter full characterization of their properties.
The dashed lines indicate some very impor-
tant limits for the design concepts in the
“KOYO” project (for details, see [38, 56]).
tional Laboratory [49,50]. It is obvious that the most prefer- 7. Nonlinear crystalline materials
able area of Fig. 23 is the top of its central region. Of course, for laser Raman converters
a more detailed characterization of laser and physical prop-
erties of Y2 O3 :Nd3+ ceramics is essential for the refinement
Stimulated Raman scattering in crystalline materials has
of their actual position in this plot. There are some un-
been of topical interest for many years in SSL physics. SRS
certainties concerning the nonlinear refractive index n2 of
is an inelastic phenomenon in which a laser pump (funda-
Y2 O3 (Sc2 O3 , Lu2 O3 ) ceramics. The very high value of this
mental) wavelength can be converted into laser emission
parameter could be a very serious obstacle for the use these
at other specific wavelengths accompanied by the excita-
ceramics in laser drivers, while crystalline materials with
tion (in the case of down conversion by Stokes generation)
large n2 are efficient for the Kerr lens mode locking genera-
or absorption (in the case of up conversion by anti-Stokes
tion regime and could be attractive for femtosecond lasers.
generation) of SRS-active optical vibrational (including po-
At the end of the 1960s the author of this review lariton) modes of crystalline materials. Stokes SRS can also
suggested the use of disordered fluoride crystals (non- improve the spatial quality of laser beams as well as the con-
stoichiometric phases) with the cubic fluorite structure trast between peak and background intensities of ultra-short
doped with Ln3+ (Nd3+ ) ions for high-power (energy) lasers laser pulses, etc. [14, 15, 66, 103, 383–385]. The investiga-
and laser amplifiers for the creation of a new generation tion of SRS in crystalline solids (it is likely that natural
of laser drivers for the problem of inertial confinement fu- diamond and calcite were used) dates from 1963 [304].
sion experiments (see, e.g. [696]). This is also evident from The first known SRS-active synthetic crystals were or-
the advantageous positioning of these neodymium laser thorhombic α-sulphur [304], polar niobates LiNbO3 and
crystalline materials in Fig. 23. Compared to neodymium Ba2 NaNb5 O15 [308], α-LiIO3 [312], and centrosymmet-
glasses (e.g. HAP-4), disordered fluorides possess much ric nitrates Ba(NO3 )2 , NaNO3 , and Pb(NO3 )2 [357]. The
better thermal properties, whereas the laser and spectro- discovery of SRS potential in several widely used insu-
scopic characteristics of both of these materials are essen- lating laser host crystals (e.g. monoclinic α-KGd(WO4 )2
tially similar. In this respect, it would be very desirable and α-KY(WO4 )2 [329, 335, 338], tetragonal YVO4 and
to have new types of ceramics based on Nd3+ -doped dis- GdVO4 [354, 355], trigonal LiCaAlF6 [307], and the γ-
ordered fluorides with sufficiently large sizes and of laser ray scintillator PbWO4 [327, 369]), as well as novel very
quality. This problem is rather difficult, but with regard to promising SRS materials with unique physical properties
the already accumulated ceramic technological experience – polycrystalline [720] and single crystal [721] CVD (SC-
its solution is possible. CVD) diamonds has led to a renewed interest in crystalline

Raman laser converters. Experimentally measured Raman of SRS-generating centres, nSt1 is the refractive index of
laser frequency shifts for numerous known SRS-active in- the crystalline sample at wavelength λSt1 , and ∆Ω is the
organic and organic crystalline materials range from ∼ 60 solid angle of the SRS generation. As can be seen from
to ∼ 3200 cm−1 (Table 13). eq. (17) the Raman gain coefficient is linearly proportional
Raman laser effects can be described phenomenolog- to the scattering cross-section and inversely proportional to
ically in terms of the nonlinear susceptibility tensor of the linewidth of the spontaneous Raman line. The product
a crystalline medium by expressing the polarization as a (1/∆ν R )( dσ/ dΩ) may be considered as the spectroscopic
power series in the electric field strength of the laser pump parameter providing a measure of the peak intensity of the
beam as (see, e.g. [383–388]) corresponding spontaneous Raman transition. This figure
of merit can be used in a comparative selection for suitable
P ≡ χ(1) E + χ(2) E 2 + χ(3) E 3 + . . . (15) SRS-active crystalline media [532]. In consequence, high-
where χ(1) is the linear optical susceptibility tensor describ- gain materials should have a small ∆νR value of intense
ing, for example, refraction and reflection processes, and Raman shifted lines. Integration of eq. (16) yields [384,385]
χ(2) , χ(3) , etc., are the second- and third-order, etc., non-
St1
linear optical susceptibilities responsible for a large variety ISt1 (lR ) = ISt1 (lR = 0) exp gssR Ip lR . (18)
of nonlinear optical phenomena (see Table 1 in [445]). The
most important nonlinear effects arise from the second and Extensive SRS investigations carried out in the 1960s and
third terms on the right-hand side of eq. (15). The second 1970s mainly with liquids and gases showed that the las-
term χ(2) E 2 is connected with second harmonic genera- ing at the first Stokes wavelengths becomes reliably de-
tion (SHG) in crystals with no centre of symmetry, whereas tectable when the exponent in eq. (18) reaches a value of
the tensor χ(3) of the third term is not subject to symme- 25–30, which corresponds to a conversion efficiency of
try restrictions. Therefore, in χ(3) media several nonlinear about 1% (see, e.g. [384,385]). A laser pump intensity pro-
processes, such as SRS, third harmonic generation (THG), viding such a 1% efficiency value is customarily consid-
p
and others, can occur in optically anisotropic and isotropic ered as a steady-state SRS threshold, ISt1 /Ithr ≈ 0.01. As
crystalline materials (Table 13). evidenced by SRS experiments conducted during the last
In a nonlinear χ(3) lasing process, spontaneous Stokes decade with different non-centrosymmetric crystals (see
Raman scattering photons provide the major contribution, Table 13 and its references), this conventional determina-
because the frequency-shifted emission of the intense lines tion of the SRS threshold pump intensity is not reasonable
acts as a seed for SRS amplification [383–385]. This sit- in all instances. In many crystals under a 1% efficiency
uation is analogous to the case of luminescence photons laser pump intensity other competitive χ(2) or χ(3) non-
(spontaneous emission) in the laser action of activated crys- linear lasing processes occur (SHG, many-phonon SRS,
tals [18, 21]. Depending on the pump pulse duration τp , filamentation, etc.). Therefore, in some comparative mea-
two temporal SRS regimes, steady state and transient, can surements, e.g. in the estimation of the Raman gain coef-
be considered (see, e.g. [536]). The first is more interest- ficient, it is more appropriate to use a level slightly below
ing for many practical cases, the main condition of which that of the laser pump intensity when the first Stokes las-
is described by eq. (11). It should be pointed out here that ing becomes perceptible. Examples of single- and many-
practically all the SRS data given in Table 13 were obtained phonon Stokes and anti-Stokes generation spectra of two
under this pumping condition. If in this lasing regime the widely used inorganic laser host crystals GdVO4 [354,
intensity Ip of the plane wave laser pump is much greater 355] and α-KY(WO4 )2 [337], two organic crystals with
than the intensity of the first Stokes generation Ip ISt1 predominantly ionic [C(NH2 )3 ]Zr{N(CH2 COO)3 ]2 · H2 O
the SRS amplification can be written [324, 446] as (GuZN-III) [379]) and van der Waals C12 H22 O11 (α-d-
glucopyranosido-β-d-fructofuranoside (sucrose), a crys-
dISt1 St1 dσ talline food sugar) [443]) structural units, three fluorides
= gssR Ip (lR )ISt1 + Ip (lR ) NSRS ∆Ω
dlR dΩ with the fluorite structure (CaF2 [742], SrF2 [801], and
St1 BaF2 ), as well as two novel promising SRS-active crys-
= gssR Ip (lR )[ISt1 (lR ) + ISt1 (lR = 0)] (16) tals with high Raman gain coefficients (SC-CVD dia-
where lR is the SRS-active length of a crystal, ISt1 (lR = mond [720] and Na3 Li(SeO4 )3 · 6H2 O [734]) and are given
0) is the intensity of spontaneous Raman scattering at the in Figs. 24–30.
wavelength λSt1 of the first Stokes seed emission (from As can be seen from these spectra the organic crys-
zero-point fluctuations in the front end (lR = 0) of the tals show significantly larger Stokes and anti-Stokes shifts.
St1
amplifying crystalline sample) and gssR is the steady-state The multi-atom unit cells of many investigated SRS-active
Raman gain coefficient given by crystals (see Table 13) provide them (e.g. GuZN-III, Fig. 28
and Na3 Li(SeO4 )3 ·6H2 O, Fig. 31) several hundred optical
St1 2λ2St1 NSRS 1 dσ vibration modes. Among them the strong stretching vibra-
gssR = . (17) tions of their (e.g. CH2 or OH) bond systems with a Raman
πn2St1 hνp ∆νR dΩ
frequency shift more than 3000 cm−1 are modes promoting
In eqs. (16) and (17) dσ/ dΩ is the peak spontaneous Ra- the efficient SRS observed. It is obvious that in the case of
St1
man scattering cross-section, NSRS is the number density many-phonon SRS crystals the determination of the gssR

Table 13 Known χ(3) and (χ(2) + χ(3) )-active inorganic and organic crystals for the steady-state SRS generation and Raman laser
converters. Most of them are also the laser host materials (see Tables 1–4 and 6–8).
crystal space Ln and TM nonlinearity SRS-active vibration observed nonlinear ref.

group lasants mode at room tem- laser effects
perature (cm−1 )
inorganic crystalline materials
α-HIO3 D4 2 – χ(2) + χ(3) ∼ 1280 SRS, SHG, OPO, [305]
self-SRS (SHG) a)
Li2 B4 O7 C4v 12 – χ(2) + χ(3) ∼ 716, ∼ 160 SRS, SHG p) , self-THG y) , [734]
self-SRS (SHG) a) ,
self-FD q) , self-SFM b)
Li2 SO4 · H2 O C2 2 – χ(2) + χ(3) ∼ 1009 SRS, SHG, self-SRS [735]
(SHG) a)
LiBGeO4 S4 2 – χ(2) + χ(3) ∼ 532 SRS, SHG, self-SFM [134]
(SRS) b)
LiCaAlF6 D3d 2 Ce3+ , Cr3+ χ(3) ∼ 560 SRS [307]
LiNbO3 x) C3v 6 Nd3+ , Dy3+ , χ(2) + χ(3) 491–628, SRS, SHG, OPO, [308–310]
Ho3+ , Er3+ , 212–248, self-FD (Nd3+ ,Yb3+ ) d) ,
Tm3+ , Yb3+ ∼ 152 c) self-pump OPO (Nd3+ ) e) ,
self-SFM (Nd3+ ) f)
LiNbGeO5 D2h 16 Cr4+ χ(3) ∼ 786, ∼ 754, ∼ 699 SRS [311]
α-LiIO3 C6 6 – χ(2) + χ(3) ∼ 818, ∼ 792, ∼ 760 SRS, SHG, OPO [224, 305,
312, 313]
Li3 Ba2 Gd3 (MoO4 )8 C2v 6 Nd3+ χ(3) ∼ 768 SRS [314]
C (diamond) g) Oh 7 – χ(3) ∼ 1332 SRS [304]
C (CVD diamond) u) Oh 7 – χ(3) 1332.5 SRS [720, 721]
α-NH4 Al(SO4 )2 ·12H2 O Th 6 – χ(3) ∼ 992 SRS [736]
Na3 Li(SO4 )2 ·6H2 O C3v 6 – χ(2) + χ(3) ∼ 815 SRS [734]
NaNO3 D3d 6 – χ(3) ∼ 1066 SRS [325, 357]
NaClO3 T4 – χ(2) + χ(3) 936, ∼ 482 SRS, SHG, [316–319]
self-SFM (SRS) b)
Na2 SO4 (I) D6h 4 – χ(3) ∼ 987 SRS [15]
Na2 SO4 (V) D2h 24 – χ(3) ∼ 992 SRS [315]
Na2 S2 O6 · 2H2 O D2h 16 χ(3) ∼ 1098, ∼ 290 SRS [738]
NaBrO3 T4 – χ(2) + χ(3) ∼ 798 SRS [315, 320,
321]
NaY(WO4 )2 C4h 6 Nd3+ χ(3) ∼ 914, ∼ 328 SRS [326, 327]
NaLa(MoO4 )2 C4h 6 Nd3+ , Ho3+ χ(3) ∼ 888, ∼ 320 SRS, self-SRS (Nd3+ ) h) [328, 329]
NaBi(MoO4 )2 C4h 6 Nd3+ χ(3) ∼ 877 SRS [330]
NaBi(WO4 )2 C4h 6 Nd3+ χ(3) ∼ 910 SRS [330]
α-Al2 O3 D3d 6 Cr3+ , Ti3+ χ(3) ∼ 419 SRS [322–324]
α-SiO2 D3 6 – χ(2) + χ(3) ∼ 465, ∼ 128 SRS, SHG [308]
α-S8 (α-sulphur) D2h 24 – χ(3) ∼ 216, ∼ 468 SRS [304]
KH2 PO4 (KDP) D2d 12 – χ(2) + χ(3) ∼ 915, ∼ 93 SRS, SHG, OPO, OR i) , [331–333]
self-TSRS (THG) j)
KD2 PO4 (DKDP ) k) D2d 12 – χ(2) + χ(3) ∼ 887 SRS, SHG, OPO, OR i) , [334]
self-TSRS (THG) j)
KB5 O8 · 4H2 O C2v (?) – χ(2) + χ(3) ∼ 551 l) SRS, SHG [428]
α-KAl(SO4 )2 · 12 H2 O Th 6 – χ(3) ∼ 990 SRS [185, 736]
KTiOPO4 (KTP) y) C2v 9 – χ(2) + χ(3) ∼ 695, ∼ 270 SRS, self-FD (SRS) q) , [739, 740]
self-THG ab) , self-SFM b)
KY(MoO4 )2 D2h 14 Nd3+ , Er3+ , χ(3) 947, 868 SRS, self-SRS (Nd3+ ) h) [305]
Yb3+

Table 13 (continued).

perature (cm−1 )
α-KY(WO4 )2 C2h 6 Pr3+ , Nd3+ , χ(3) 905, 765, 87 SRS, [329, 335–
Dy3+ , Ho3+ , self-SRS (Nd3+ ,Yb3+ ) h) 337, 389]
Er3+ , Tm3+ ,
Yb3+
K3 Nb3 O6 (BO3 )2 C2v 2
– χ(2) + χ(3) ∼ 648, ∼ 324 SRS [737]
γ-KIO3 C1 1 – χ(2) + χ(3) ∼ 781, ∼ 733 SRS, SHG [313]
KLa(MoO4 )2 C2h (?) Nd3+ , Ho3+ ,
6
χ(3) ∼ 898, ∼ 319 SRS [305]
Er3+
α-KGd(WO4 )2 C2h 6 Pr3+ , Nd3+ , χ(3) ∼ 901, ∼ 768, ∼ 84 SRS, self-SRS (Pr3+ , [329, 335,
Dy3+ , Ho3+ , Nd3+ ,Yb3+ ) h) 338]
Er3+ , Tm3+ ,
Yb3+
α-KDy(WO4 )2 C2h 6
– χ(3) ∼ 899, ∼ 760 SRS [339]
α-KYb(WO4 )2 C2h 6 Tm3+ , Yb3+ χ(3) ∼ 907, ∼ 757, ∼ 87 SRS
α-KLu(WO4 )2 C2h 6 Pr3+ , Nd3+ , χ(3) ∼ 907, ∼ 757 SRS, self-SRS (Nd3+ ) h) [339]
Ho3+ , Er3+ ,
Tm3+ , Yb3+
CaCO3 D3d 6
– χ(3) ∼ 1086 SRS, THG m) [304, 340,
341]
CaF2 Oh 5 Nd3+ , Dy3+ , χ(3) 322.5 SRS, THG [742, 803]
Ho3+ , Er3+ ,
Tm3+ , Yb3+ ,
Sm2+ , Dy2+ ,
Tm2+ , U3+
Ca3 Ga2 Ge3 O12 Oh 10 Nd3+ , Er3+ , χ(3) ∼ 807 SRS [342]
d-c
Ca(NbO3 )2 D2h 14 Pr3+ , Nd3+ , χ(3) ∼ 901 SRS, self-SRS (Nd3+ ) h) [305]
Ho3+ , Er3+ ,
Tm3+
Ca3 (Nb,Ga)2 Ga3 O12 Oh 10 Nd3+ , Er3+ χ(3) ∼ 500 SRS [345]
CaMoO4 C4h 6 Nd3+ , Ho3+ , χ(3) ∼ 880 SRS, self-SRS (Nd3+ ) h) [343]
Tm3+
Ca4 Y(BO3 )3 O Cs 3 Nd3+ , Yb3+ χ(2) + χ(3) ∼930 SRS, SHG
Ca4 Gd(BO3 )3 O Cs 3 Nd3+ , Yb3+ χ(2) + χ(3) ∼ 933 SHG, SRS, [346–348]
self-FD (Nd3+ , Yb3+ ) d) ,
self-SRS (SHG) a)
CaWO4 C4h 6 Pr3+ , Nd3+ , χ(3) ∼ 908 SRS [327, 344]
Ho3+ , Er3+ ,
Tm3+
Sc2 O3 (ceramic) n) Th 7 Yb3+ χ(3) ∼ 419 SRS [688]
ZnWO4 C2h 4 Cr3+ χ(3) ∼ 907 SRS [327]
α-RbAl(SO4 )2 ·12H2 O Th 6 – χ(3) ∼ 991 SRS [736]
Sr(NO3 )2 Th 6 – χ(3) ∼ 1057 SRS [349]
SrF2 Oh 5 Nd3+ , Ho3+ , χ(3) ∼ 282 SRS, THG [801, 803]
Er3+ , Tm3+
Sr5 (PO4 )3 F C6h 2 Nd3+ , Yb3+ χ(3) ∼ 950 SRS [350]
SrMoO4 C4h 6 Pr3+ , Nd3+ χ(3) ∼ 885 SRS, self-SRS (Nd3+ ) h) [343]
SrWO4 C4h 6 Nd3+ χ(3) ∼ 922 SRS, self-SRS (Nd3+ ) h) [343, 802]
Y2 O3 (ceramic) n) Th 7 Nd3+ , Yb3+ χ(3) ∼ 378 SRS [351]


perature (cm−1 )
Y3 Al5 O12 Oh 10 Pr3+ , Nd3+ , χ(3) ∼ 370 SRS [352, 353]
Ho3+ , Er3+ ,
Tm3+ , Yb3+ ,
Cr3+
Y3 Al5 O12 (ceramic) n) Oh 10 Nd3+ , Yb3+ χ(3) ∼ 370 SRS [353]
YVO4 D4h 19 Nd3+ , Eu3+ , χ(3) ∼ 890, ∼ 815 SRS, self-SRS (Nd3+ ) h) , [354, 355,
Ho3+ , Er3+ , self-SRS (Yb3+ ) b) 744]
Tm3+ , Yb3+
CdWO4 C2h 4 – χ(3) ∼ 890 SRS [327]
α-TeO2 D4 4 – χ(2) + χ(3) ∼ 648, ∼ 148, ∼ 62 SRS, SHG [305]
CsLiMoO4 Td 2 – χ(2) + χ(3) ∼ 925, ∼ 310 SRS, SHG [741]
CsLiMoO4 · 1/3H2 O Td 2 – χ(2) + χ(3) ∼ 925, ∼ 310 SRS, SHG, self-SFM [741]
(SRS) b)
Cs(NO3 )2 (II) C2 3 – χ(2) + χ(3) ∼ 1051 SHG, SRS [349]
Cs2 S2 O6 C6v 4 – χ(2) + χ(3) ∼ 1091 SRS [745]
β-BaB2 O4 C3v 6 – χ(2) + χ(3) ∼ 636 SRS, SHG, OPO, THG m) , [356, 684]
self-SRS (SHG) a) ,
self-SFM (OPO) o)
Ba(NO3 )2 Th 6 – χ(3) ∼ 1049 SRS [357, 358]

BaF2 Oh 5 Nd3+ , U3+ χ(3) ∼ 238 SRS
Ba2 NaNb5 O15 C2v 11
Nd3+ χ(2) + χ(3) ∼ 650 SRS, SHG, self-FD [308, 405,
(Nd3+ ) d) 746]
BaWO4 C4h 6 – χ(3) ∼ 925, ∼ 332 SRS [359, 360]
β-LaBGeO5 C2 3 Pr3+ , Nd3+ χ(2) + χ(3) 803, ∼ 790 SRS, SHG p) , self-FD [347, 361,
(Nd3+ ) d) , 362]
self-SRS (Nd3+ ) h) ,
self-SRS (SHG) a) , self-FD
(SRS) q) ,
self-DFG r)
La2 (WO4 )3 C2h 6 χ(3) ∼ 940 SRS [363]
Gd3 Sc2 Ga3 O12 Oh 10 3+
Nd , Ho , 3+
χ(3) ∼ 351 SRS [345]
Er3+ , Tm3+ ,
Yb3+ , Cr3+
GdVO4 D4h 19 Nd3+ , Ho3+ , χ(3) 882, ∼ 807, ∼ 256 SRS, self-SRS (Nd3+ ) h) [354, 355]
Tm3+ , Yb3+
Gd3 Ga5 O12 Oh 10 Pr3+ , Nd3+ , χ(3) ∼ 354 SRS [345]
Ho3+ , Er3+ ,
Yb3+ , Cr3+ ,
Ni2+
β -Gd2 (MoO4 )3 C2v 8 Nd3+ χ(2) + χ(3) ∼ 960, ∼ 943, ∼ 857, SRS, SHG, DSHG [364–367]
∼ 100 (Nd3+ ) s) ,
self-FD (Nd3+ ) d) , self-SRS
(SHG) a)
Tb3 Ga5 O12 Oh 10 – χ(3) ∼ 360 SRS [747]
Lu2 O3 (ceramic) n) Th 7 Nd3+ , Yb3+ χ(3) ∼ 392 SRS [716]
YbVO4 D4h 19 – χ(3) ∼ 897 SRS [748]
LuVO4 D4h 19 – χ(3) ∼ 900 SRS [742]
α-TlAl(SO4 )2 ·12H2 O Th 6 – χ(3) ∼ 991 SRS [736]
Pb(NO3 )2 Th 6 – χ(3) ∼ 1060 (?) SRS [357]
PbCl2 D2h 16 Nd3+ χ(3) ∼ 143 SRS [43]


group lasants mode at room temper- laser effects
ature (cm−1 )
PbMoO4 C4h 6 Nd3+ χ(3) ∼ 869 SRS, self-SRS (Nd3+ ) h) [368–370]

PbWO4 C4h 6 Nd3+ χ(3) ∼ 901, ∼ 328 SRS, self-SRS (Nd3+ ) h) [327, 369–
372]
BiB3 O6 C2 3 – χ(2) + χ(3) ∼ 604, 583, ∼ 542, SRS, SHG, OPO, [373]
374, ∼ 215, ∼ 168 self-SFM (SRS) b)
Bi4 Si3 O12 Td 6 Nd3+ χ(2) + χ(3) ∼ 97 SRS [374]
Bi12 SiO20 T3 Nd3+ χ(2) + χ(3) ∼ 277 SRS [375]
Bi4 Ge3 O12 Td 6 Nd , Ho , χ(2) + χ(3) 91
3+ 3+
SRS, SHG, [318, 374]
Er3+ , Tm3+ , self-SFM (SRS) b)
Yb3+
heterodesmic organic crystals with predominantly ionic bonds between structural units
LiHCOO · H2 O C2v 9 – χ(2) + χ(3) ∼ 1372, (∼ 163, SRS, SHG [306]
∼ 113, ∼ 104, ∼ 82,
∼ 79, ∼ 76) aa)
LiNH2 C6 H4 SO3 · H2 O C2h 5 – χ(3) ∼ 3075, ∼ 1128, SRS [750]
∼ 111
C6 H4 (COOH)[COO(NH4 )] D2 4 – χ(2) + χ(3) ∼ 3120, ∼ 1055 SRS
C6 H4 (COOH)(COOK) D2 4
– χ(2) + χ(3) ∼ 3110, ∼ 1045, SRS
∼ 795, ∼ 78
[C(NH2 )3 ]2 Zr[N(CH2 COO)3 ]2 D2 5
– (2)
χ +χ (3)
∼ 2940, ∼ 1008 SRS, SHG [379, 751]
· H2 O
(GuZN-III)
N(CH2 CH2 NH3 )3 Br3 T4 – χ(2) + χ(3) ∼ 2965 SRS [749]
(“tren” · 3Br)
α-Ca(HCOO)2 D2h 15 – χ(3) ∼ 2892, ∼ 1387, SRS [750]
∼ 1352, ∼ 67
Y(HCOO)3 · 2H2 O D2 4 – χ(2) + χ(3) ∼ 2895, ∼ 1395, SRS, SHG, self-FD [743, 756,
∼ 1377 (SRS) q) , self-SFM b) , 806]
self-SRS (SFM) v)
heterodesmic organic crystals with predominantly van der Waals bonds between structural units
C12 H22 O11 C2 2 – χ(2) + χ(3) ∼ 2960 SRS, SHG [443]
t)
(sucrose)
C13 H10 O D2 4 – χ(2) + χ(3) ∼ 3070, ∼ 1650, SRS, SHG [378, 752]
(benzophenone) ∼ 998, ∼ 103
C13 H10 O3 D2h 16 – χ(3) ∼ 3150 SRS [378, 754]
(salol)
C14 H10 O2 D3 4 (D3 6 ) – χ(2) + χ(3) ∼ 1000 SRS [378, 757]
(benzil)
α-C14 H12 O C2h 5 – χ(3) ∼ 3065 SRS [378]
(α-4-methylbenzophenone)
C15 H19 N3 O2 C2v 9 – χ(2) + χ(3) ∼ 1280 SRS, SHG, [377, 753]
(AANP) self-SFM (SRS) b)
C16 H15 N3 O4 Cs 4
– (2)
χ +χ (3)
∼ 1587 SRS, SHG, [376]
(MNBA) self-FD (SRS) q) , self-
SFM (SRS) b)
(NH3 CH2 CH2 NH3 )((+)– C2 2
– (2)
χ +χ (3)
∼ 3015, ∼ 2975, SRS, SHG [758]
C4 H4 O6 ) ∼ 2945, ∼ 995, ∼ 785,
(EDT) ∼ 470, ∼ 95, ∼ 80

a)
Self-SRS (SHG), i.e. SRS from the SHG arising from the pumping (fundamental) radiation.
b)
Self-SFM (SRS), i.e. self-sum-frequency mixing of the arising SRS lasing components and pumping radiation.
c)
Including polariton modes.
d)
Self-FD, i.e. SHG of the arising SE generation of lasing Nd3+ or Yb3+ activator ions.
e)
Self-pump OPO, i.e. the optical parametric oscillator pumped by the arising SE generation of lasing activator ions.
f)
Self-SFM (SE), i.e. self-sum-frequency mixing of the arising SE generation of Nd3+ lasing activator ions and pumping radiation.
g)
IIA-type natural diamond was used.
h)
Self-SRS (SE), i.e. SRS from the arising SE of lasing Pr3+ or Nd3+ , or Yb3+ activator ions.
i)
OR is the optical rectification [380].
j)
Self-TSRS (THG), i.e. the self-transverse SRS from the arising third harmonic generation.
k)
∼ 80% deuterated KH2 PO4 , i.e. K(H0.2 D0.8 )2 PO4 [334].
l)
Several other SRS-active vibration modes were also observed. Their identification requires more accurate analysis.
m)
THG, third harmonic generation [381, 382].
n)
Ceramic grains are nano- and (or) micrometer-sized single crystals.
o)
Self-SFM (OPO), i.e. the self-sum-frequency mixing of the arising idler generation and pumping radiation.
p)
As well as “Cherenkov”-type SHG.
q)
Self-FD(SRS), i.e. SHG from the arising SRS lasing components.
r)
Self-DFG, i.e. self-difference frequency generation of the pumping (in the visible) and the first Stokes generation by the arising
one-micron SE generation of Nd3+ lasing activator ions.
s)
DSHG, diffuse SHG from the arising SE generation of lasing Nd3+ activator ions.
t)
Picosecond high-order SRS (ωSRS ≈ 2915 cm−1 ) was also observed in food sugar caramel. Both sugar materials are easily
available and are very cheap, e.g. sugar single crystals “Weißer kandis” and glassy caramel “Concorde citron” were purchased in
Berlin “Ulrich” supermarket and in Charles de Gaulle airport duty free, respectively.
u)
Polycristalline CVD [720] and single crystal CVD (SC-CVD) [721] diamonds.
v)
Self-SRS (SFM), i.e. SRS from the SFM arising from pumping radiation and its Stokes generation.
w)
In periodically poled KTiOPO4 was observed cascaded self-SRS (OPO) nonlinear lasing χ(2) → χ(3) processes where SRS
components arose from OPO signal at ∼ 1.572 µm wavelength [758].
x)
In periodically poled LiNbO3 :Mg2+ was observed cascaded self SRS (OPO) nonlinear lasing χ(2) → χ(3) processes where SRS
components connected with SRS-active vibration modes (∼ 46, 103, ∼ 252, 525, and 631 cm−1 ) arose from OPO signal at
∼ 1.593 µm wavelength [759].
y)
Cascaded conical (“Cherenkov”-type) THG ωSHG + ωp = ωTHG in a Li2 B4 O7 single crystal [734].
aa)
Recorded at cryogenic temperatures.
ab)
Cascaded THG (ω THG = ω SHG + ω p ) in a cerium doped single crystal KTiOPO4 [760].
Additional note: Quite recently in our SRS experiments rather efficient Stokes and anti-Stokes generation with nano- and picosecond
laser pumping was also observed in several new χ(3) -active crystals which were grown by my scientific partners P. Becker, L. Bohatý,
V. Dolbinina, E. Haussühl, S. Haussühl, A. Voloshin and others. In particular, among these crystals are: Na2 S2 O6 · 2 H2 O, Ca2 S2 O6 · 4 H2 O,
Ca2 Zn2 SiO7 , Ca2 Mg2 SiO7 , PbH2 PO4 , Cs5 H3 (SO4 )4 · H2 O, CsH2 PO4 , Ca3 Ga2 Ge4 O14 , Sr3 Ga2 Ge4 O14 , (CH3 )2 NH2 Al(SO4 )3 · 6 H2 O,
(NH4 )3 H(SO4 )2 , (NH2 CH2 COOH)3 · H2 SO4 , (NH3 CH2 COOH)2 · NHO3 . The results of an analysis of nonlinear lasing in these materials
will be the subject of a future publication.
coefficient for the first Stokes lasing wavelengths is a rather different generation and conversion processes can occur
complex experimental task. simultaneously, simplifying the design of lasers based on
these materials (Fig. 32). Among these, the self-FD, self-
SRS, and self-pumped OPO lasers based on Ln3+ -doped
8. Crystalline lasers crystals exhibit the most attractive practical potential.
with self-frequency conversion
Various nonlinear self-frequency conversion effects appear 8.1. Self-frequency doubling crystalline lasers
in Ln- and TM-doped inorganic laser crystals and in un-
doped inorganic and organic crystals subject to their own The physical principles of the phenomenon of self-FD in
powerful SE, SHG, and SRS generation. The investiga- non-centrosymmetric laser crystals have been considered
tion and characterization of new and known χ(3) - and completely in [18, 21, 386]. Due to the symmetry of cen-
(χ(2) + χ(3) )-active crystals, as well as their development trosymmetric crystals, the coefficients of the χ(2) tensor
as the basis of novel frequency conversion laser sources are equal to zero [390], and therefore these crystals cannot
generating specific wavelengths, have received much at- be used for SHG and self-FD lasers. The real possibility
tention in recent years. The distinctive features of these of using Ln3+ -doped insulating crystals for self-FD lasers
types of frequency converters are that in the active crystals was shown in [391], where for the first time the neces-

Figure 24 Steady-state SRS spectra of GdVO4 single crystal recorded at 300 K in c(aa)c (here and so forth: the first letter denotes
excitation direction c-axis, the second the excitation light electric vector direction a-axis (polarization), the third the polarization of
scattering light, and the fourth the scattering light direction) pumping geometry with picosecond laser pumping in a) the visible and
b) the near-IR regions [354, 355]. Stokes and anti-Stokes lasing lines related to SRS-active vibration mode ωSRS = 882 cm−1 of this
tetragonal vanadate are indicated by horizontal scale lines. Other notations as in Fig. 16.

Figure 25 Steady-state SRS spectra of undoped α-KY(WO4 )2 single crystal recorded at 300 K with picosecond laser pumping at
a wavelength of 1.06415 µm with excitation geometry a) a(cc)a and b) b(cc)b [337]. Stokes and anti-Stokes lasing lines related to
SRS-active vibration modes ωSRS1 = 905 cm−1 , ωSRS2 = 765 cm−1 , and ωSRS3 = 87 cm−1 of this monoclinic tungstate are indicated
by horizontal scale lines. Other notations as in Fig. 16.

Figure 26 Steady-state SRS spectra of

metal-organic GuZN-III single crystal
recorded at 300 K with pumping geome-
try a) a(bb)a and b) c(aa)c with picosec-
ond laser pumping at a wavelength of
0.53207 µm [379]. Stokes and anti-Stokes
lasing components related to SRS-active
vibration modes ωSRS1 ≈ 1008 cm−1
and ωSRS2 ≈ 2940 cm−1 are indicated
by horizontal scale lines. Other notations
as in Fig. 16.

Figure 27 Steady-state SRS spectra of randomly oriented C12 H22 O11 (sucrose) single crystal recorded at 300 K with picosecond
laser pumping at a wavelength of 0.53207 µm [443]. Stokes and anti-Stokes lasing components related to SRS-active vibration mode
ωSRS ≈ 2960 cm−1 are indicated by the horizontal scale line. Other notations as in Fig. 16.
[C(NH2)3]2Zr[N(CH2COO)3]2 · H2O
2[C(NH2)3] +
H2O
[Zr(NTA )2] 2-
Figure 28 Projection of the unit cell of the

[C(NH2 )3 ]2 Zr[N(CH2 COO)3 ]2 · H2 O (GuZN-III)
single crystal along the [001] direction and its
three structure fragments 2[C(NH2 )3 ]+ · H2 O, and
b
[Zr(NTA)2 ]2 [379]. The hydrogen bonding system
is plotted by dashed lines for one selected quan-
O N C Zr H
a dinium and water molecule.

Figure 29 Steady-state SRS spectra of

cubic fluoride CaF2 , SrF2 , and BaF2 sin-
gle crystals (l ≈ 100 mm) with fluorite
Oh 5 -structure recorded at 300K with pi-
cosecond pumping in the visible. Stokes
and anti-Stokes lasing lines related to
SRS-active vibration modes (ωSRS =
322.5 cm−1 for CaF2 , ωSRS ≈ 282 cm−1
for SrF2 , and ωSRS ≈ 238 cm−1 for BaF2 )
are indicated by the horizontal scale lines.
Other notation as in Fig. 16.

[111]
SC-CVD
diamond
0.53207*
0.6200
5
0.5727
F2g
1.06415*
4
a0
1.2400
SRS intensity, arb. units
0.6758
0.4968
1.4854
0.4660
0.7427
0.4388
2
(a)
0.9320
ωSRS = 1332.5 cm-1

1
0.8290
0.7466
(c)
(b)
0
ωSRS = 1332.5 cm-1
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.3 1.4 1.5
Wavelength, µm
Figure 30 High-order Stokes and anti-Stokes generation spectra of ≈670- µm SC-CCVD diamond with picosecond laser pumping:
(a) in the visible and (b,c) in the near-IR regions [721]. The tetrahedral bonding of carbon atoms with their nearest neighbors and the
relative displacement along [111] axis (see open circles) of two face-centered cubic sublattices with respect to each other in the triply
degenerated F2g optical vibration mode are shown in the inset. The spacing of χ(3) -lasing components is a multiple of SRS-promoting
vibration mode (ωSRS = 1332.5 cm−1 ) of diamond are indicated by the horizontal scale lines. Other notation as in Fig. 16.
sary σ-polarized SE at a wavelength of 1.0933 µm in an

optical negative nonlinear LiNbO3 :Nd3+ crystal was ob-
tained. For several reasons, the first realization of a “green”
self-FD laser based on the niobate LiNbO3 :Nd3+ (SE gen-
eration of the 4 F3/2 → 4 I11/2 channel converted in SHG)
was not achieved until 10 years later [392]. Soon after,
a “red” self-FD laser was developed based on Nd3+ -doped
non-centrosymmetric β-YAl3 (BO3 )4 crystals (∼ 1.318 µm
SE wavelength of the 4 F3/2 → 4 I13/2 channel converted in
SHG) [393].
Essential progress in the realization of self-FD
lasers was provided by the development of new non-
centrosymmetric laser crystals and modern LD pump-
ing techniques. All known self-FD crystalline lasers with
birefringent phase matching are listed in Table 14. Self-
FD effects have also been observed in several Cr3+ - and
Nd3+ -doped non-centrosymmetric laser crystals with the
Ca-gallogermante structure possessing a relatively small
birefringence that is insufficient for providing the re-
Figure 31 Section of the crystal structure of Na3 Li(SeO4 )2 quired phase-matching condition in the visible and near-IR
· 6 H2 O, representing one sheet of [Na3 O7 (H2 O)6 ] groups to- (Table 13). Recently [362] in (χ(2) +χ(3) )-active mono-
gether with the linking tetrahedral groups [SeO4 ] and the dou- clinic β-LaBGeO5 :Nd3+ and undoped β-LaBGeO5 crys-
ble tetrahedra [O3 SeOLi(H2 O)3 ], that are formed by [SeO4 ] and tals new manifestations of self-frequency conversion were
[LiO(H2 O)3 ] [734]. Hydrogen atoms are marked with spheres. observed. In particular, in non-centrosymmetric lasing
β-LaBGeO5 :Nd3+ crystals the self-FD effect arose at a

Figure 32 Schematic arrangements of crys-

talline lasers: a) single-cavity self-FD or self-
SRS laser; b) two-cavity χ(3) -Raman coverter;
c) intercavity frequency doubled laser. HR MSE
and HR MSRS are highly reflecting mirrors at the
SE and SRS wavelengths, respectively; OCSE is
an output coupler at the SE wavelength; HR MSE –
OCSHG and HR MSE –OCSRS are highly reflecting
mirrors at the SE wavelength and at the same
time output couplers at the SHG and SRS wave-
lengths, respectively; and Q-sw is a Q-switcher.
wavelength of 0.5723 µm (2ωSt1 = 2(ωSE − ωSRS ) = are an extensively growing area in SSL physics. Numerous
17473 cm−1 ) from strong first Stokes emission at examples are shown in Table 15. Quite recently [372] a
1.1446 µm of SE generation at a wavelength of 1.0482 µm high-efficiency (about 60%) and compact (cavity length
(Fig. 33a). In undoped β-LaBGeO5 this effect arose at a 24 mm) LD-pumped self-SRS first-Stokes PbWO4 :Nd3+
wavelength of 0.5818 µm (Fig. 33b) from strong first Stokes laser was reported. As shown by SRS experiments with
generation at 1.1636 µm of the fundamental 1.06415 µm several χ(3) -active laser host crystals of a few millimetres
pumping radiation (2ωSt1 =2(ωf1 − ωSRS )). Due to very in length (α-KY(WO4 )2 , α-KGd(WO4 )2 , α-KLu(WO4 )2 ,
strong (χ(2) +χ(3) ) nonlinearities in these crystals other YVO4 , GdVO4 , and β-LaBGeO5 ), further miniaturization
self-frequency conversion effects such as self-SFG and self- of self-SRS crystalline lasers is possible, down to the real-
DFG, as well as self-SRS, have been observed. Analogous ization of the concept of chip lasers.
self-sum-frequency lasing processes have been evidenced It should be particularly emphasized here that self-SRS
in several other (χ(2) +χ(3) )-active inorganic and organic effects in lasing Ln3+ -doped crystals can be very serious
crystals (Table 13). In particular, multi-wavelength self- channels of nonlinear optical losses. In particular, they can
SFG effects were observed in non-centrosymmetric cubic be manifested in high-power and high-energy ultra-short-
NaClO3 (Fig. 34 [318]) and Bi3 Ge4 O12 (Fig. 35 [318,374]), pulse lasers and amplifiers. Recently [350] such precau-
and in the novel organic orthorhombic C15 H19 N3 O2 tion was detailed in an analysis of SE- and SRS-active
(AANP) crystal (Fig. 36 [377]). Sr5 (PO4 )3 F:Yb3+ crystals which were suggested for a mul-
tistage amplifier for an advanced laser fusion driver sys-
tem [50].
8.2. Self-stimulating Raman scattering lasers
based on Ln3+ -doped crystals
8.3. Self-pumped optical parametric oscillations
Self-SRS lasers are an attractive alternative to conventional in laser crystals (LiNbO3 :MgO doped with Nd3+
intracavity Raman lasers with a separate SE-active Ln3+ -
doped crystal and χ(3) -active frequency converter. Self- and Yb3+ ions)
SRS lasers exhibit much lower reflection and scattering
losses, as well as having a simpler and more robust cav- There are two known realizations of self-pumped OPO
ity design (Fig. 32a). Nowadays crystalline self-SRS lasers based on Nd3+ - and Yb3+ -doped non-centrosymmetric

Figure 33 Room temperature self-frequency conversion spectra of lasing a) β-LaBGeO5 :Nd3+ and b) undoped β-LaBGeO5 non-
centrosymmetric crystals obtained with nanosecond “green” and picosecond one-micron pumping [362]. The wavelengths of all lasing
components are given in µm with their identification. Stokes and anti-Stokes lasing lines related to SRS-active vibration mode ωSRS =
803 cm−1 of this trigonal non-centrosymmetric crystal are indicated by horizontal scale lines. Other notation as in Fig. 16.

Table 14 Self-frequency doubled lasers based on non-centrosymmetric Ln3+ -doped crystals with birefringent phase matching.
crystal stimulated emission SHG phase-matching |deff | ref.

type angles (pm V−1 )
SE channel λSE (µm) polari-
zation
doped with Nd3+ ions
LiNbO3 a) 4
F3/2 → 4 I11/2 1.0933 σ oo–e Θpm ≈ 90◦ ∼6 [392]
LiNbO3 :MgO b) 4
F3/2 → 4 I11/2 ∼ 1.094 σ oo–e c) Θpm ≈ 90◦ ∼6 [394]
LiNbO3 :ZnO 4
F3/2 → 4 I11/2 ∼ 1.084 π – ∼6 [686]
∼ 1.093 σ oo–e Θpm ≈ 79◦
4
F3/2 → I13/2
4
∼ 1.386 σ oo–e Θpm ≈ 90◦ – [689]
LiNbO3 :Sc2 O3 4
F3/2 → 4 I11/2 ∼ 1.092 σ oo–e Θpm ≈ 90◦ ∼6 [395]
LiTaO3 4
F3/2 → 4 I11/2 ∼ 1.082 π – b)
– [396]
Ca4 Y(BO3 )3 O 4
F3/2 → 4 I11/2 ∼ 1.060 σ oo–e Θ ≈ 90◦ , ϕ ≈ 45◦ ∼ 1.1 [397–399]
4
F3/2 → 4 I13/2 ∼ 1.332 σ Θ ≈ 90◦ , ϕ ≈ 28◦ [400]
Ca4 Gd(BO3 )3 O 4
F3/2 → 4 I9/2 ∼ 0.936 σ oo–e Θ ≈ 90◦ , ϕ ≈ 59◦ ∼ 1.3 [401]
4
F3/2 → 4 I11/2 1.0610 σ Θ ≈ 90◦ , ϕ ≈ 46◦ [402]
Θ ≈ 67◦ , ϕ ≈ 134◦ [403]
β-YAl3 (BO3 )4 d) 4
F3/2 → 4 I11/2 ∼ 1.064 σ oo–e Θpm ≈ 30◦ , ϕr ≈ 0◦ ∼ 1.9 [404]
4
F3/2 → 4 I13/2 ∼ 1.318 σ oo–e Θpm ≈ 27◦ , ϕr ≈ 0◦ ∼2 [393]
∼ 1.338 σ/π – [444]
Ba2 NaNb5 O15 e) 4
F3/2 → 4 I11/2 1.0630 σ oo–e Θpm ≈ 90◦ ∼ 11 [405]
1.0710
β-LaBGeO5 4
F3/2 → 4 I11/2 1.0482 π ee–o Θpm ≈ 54◦ , ϕr ≈ 39◦ ∼ 0.3 [361, 406,
4
F3/2 → 4 I13/2 1.3141 π ee–o Θpm ≈ 40◦ , ϕr ≈ 39◦ ∼ 0.5 407]
La2 CaB10 O19 4
F3/2 → 4 I11/2 ∼ 1.051 f) π ee–o Θpm ≈ 36.3◦ , ϕr ≈ 0 – [761]
∼ 1.067 f) π ee–o Θpm ≈ 36.3◦ , ϕr ≈ 0
β-(La,Nd)Sc3 (BO3 )4 4
F3/2 → 4 I11/2 1.0642 σ oo–e Θpm ≈ 33◦ ∼2 [408]
β-CeSc3 (BO3 )4 4
F3/2 → 4 I11/2 ∼ 1.064 σ oo–e Θpm ≈ 33◦ ∼2 [408]
β-GdAl3 (BO3 )4 g) 4
F3/2 → 4 I11/2 1.0619 σ oo–e Θpm ≈ 30◦ – [409, 410]
4
F3/2 → 4 I13/2 ∼ 1.338 σ oo–e Θpm ≈ 24.4◦ – [411]
β -Gd2 (MoO4 )3 4
F3/2 → 4 I11/2 1.0606 π ee–o Θpm ≈ 65◦ , ϕr ≈ 45◦ ∼ 1.9 [412]
doped with Yb3+ ions
LiNbO3 :MgO 2
F5/2 → 2 F7/2 1.0634 σ oo–e Θpm ≈ 82◦ , ϕr ≈ 0◦ ∼ 5.6 [413, 414]
Ca4 Y(BO3 )3 O 2
F5/2 → 2 F7/2 ∼ 1.09 σ oo–e Θ ≈ 90◦ , ϕ ≈ 36.2◦ ∼ 1.1 [415]
Ca4 Gd(BO3 )3 O 2
F5/2 → 2 F7/2 ∼ 1.043 σ oo–e Θ ≈ 90◦ , ϕ ≈ 43◦ ∼ 0.5 [416]
β-YAl3 (BO3 )4 2
F5/2 → 2 F7/2 ∼ 1.040 σ oo–e Θpm ≈ 35◦ , ϕr ≈ 0◦ ∼ 1.4 [417]
1.026–1.092 Θpm ≈ 31◦ , ϕr ≈ 0◦ [418, 419]
a)
Self-FD in Nd3+ -diffused LiNbO3 waveguide was obtained with a domain-inverted grating for the achievement of
quasi-phase-matched SHG [440], and for Nd3+ -doped aperiodically poled LiNbO3 crystal (grown by the off-centre Czochralski
method) the quasi-phase-matched SHG was achieved for two SE channels (4 F3/2 → 4 I11/2 and 4 F3/2 → 4 I13/2 ) [685].
b)
Self-FD under quasi-phase-matched condition was also observed in the LiNbO3 :MgO:Yb3+ crystal with the periodically
domain-inverted structure [420], as well as in LiTaO3 :Nd3+ (λSE ≈ 1.082 µm) crystals [396].
c)
“Cherenkov”-type: in waveguide laser [427].
d)
In [421] blue radiation was observed from β-YAl3 (BO3 )4 :Nd 3+ crystal (cut at ∼ 38◦ ) at three closed wavelengths around
0.4549 µm which was explained as self-FD of laser emission at ∼ 0.91 µm wavelengths of the 4 F3/2 → 4 I9/2 channel. Unfortunately,
these data do not agree with Stark levels of Nd3+ ions in this non-centrosymmetric crystal given in [422, 423].
e)
Diffuse self-FD phenomenon was observed in this crystal with randomly distributed quasi-cylindrical ferroelectric domains. The
same frequency doubling was registered in another laser ferroelectric, Sr0.6 Ba0.4 (NbO3 )2 :Nd3+ (λSE ≈ 1.0626 and 1.0820 µm)
[424, 425]. The theory of this phenomenon was discussed in [426].
f)
Belong to two inequivalent lasing centers.
g)
In a single non-centrosymmetric crystal β-GdAl3 (BO3 )4 :Nd3+ was observed THG at λTHG = 0.3543 µm wavelength by cascaded
χ(2) -processes: self-FD (oo-o type interaction) of SE at λSE = 1.0628 µm wavelength and self-SFM (oo-e) of SE and SHG
lasing [762].

Figure 34 Steady-state Raman-induced generation spectra of NaClO3 single crystal recorded at 300 K with picosecond laser pumping
at wavelengths of a) λf2 = 0.53207 µm and b) λf1 = 1.06415 µm [318]. The identification of self-SFG components in the spectral region
of SHG is shown in the inset. Stokes and anti-Stokes lines related to SRS-active vibration A-mode ωSRS = 936 cm−1 are indicated by
horizontal scale lines. Other notations as in Fig. 16.

Table 15 Self-stimulated Raman scattering effects in laser crystals doped with Ln3+ ions at room temperature
crystal lasing room temperature pulsed stimulated Raman scattering ref. a)

Ln3+ stimulated emission
ion
SE channel λSE mode λSRS (µm) line ωSRS
(µm) (cm−1 )
α-KY(WO4 )2 Nd3+ 4
F3/2 → 4 I11/2 1.0688 ps ∼ 0.975 ASt1 ∼ 905 [335]
∼ 1.183 St1
∼ 1.325 St2
Yb3+ 2
F5/2 → 2 F7/2 1.029– ns b) 1.136–1.139 St1 [389]
1.032
Tm3+ 3
H4 → 3 H6 ∼ 1.950 ns ∼ 2.365 St1 [683]
α-KGd(WO4 )2 Pr3+ 1
D2 → 3 F4 1.0657 µs c) ∼ 1.179 St1 ∼ 901 [362]
Nd 3+ 4
F3/2 → I11/2
4
1.0672 ps, ns ∼ 0.974 ASt1 ∼ 901 [335, 429–431, 763]
1.0672 ∼ 1.181 St1
∼ 1.321 St2
ns ∼ 1.162 St1 ∼ 768 [430, 432]
∼ 1.276 St2
∼ 1.067 CW ∼ 1.181 St1 901 [764]
4
F3/2 → I13/2
4
∼ 1.351 ns ∼ 1.538 St1 ∼ 901 [430, 433]
Yb3+ 2
F5/2 → 2 F7/2 ∼ 1.033 ns ∼ 1.139 St1 ∼ 901 [434]
α-KLu(WO4 )2 Nd 3+ 4
F3/2 → I11/2
4
1.0702 ns 1.1852 St1 ∼ 907 [362]
Yb3+ 2
F5/2 → 2 F7/2 1.0306 ns, ∼ 1.1376 St1 ∼ 907 [765]
CW
KY(MoO4 )2 Nd3+ 4
F3/2 → 4 I11/2 1.0669 ns 1.1758 d) St1 ∼ 868
NaLa(MoO4 )2 Nd 3+ 4
F3/2 → I11/2
4
1.0653 ns ∼ 1.177 St1 ∼ 888 [435]
Ca(NbO3 )2 Nd3+ 4
F3/2 → 4 I11/2 1.0615 ns 1.1737 St1 ∼ 901
CaMoO4 Nd3+ 4
F3/2 → 4 I11/2 1.0573 ns 1.1656 St1 ∼ 880 [343]
SrMoO4 Nd 3+ 4
F3/2 → I11/2
4
1.0577 ns 1.1671 St1 ∼ 880 [343]
SrWO4 Nd3+ 4
F3/2 → 4 I11/2 1.0699 ns 1.1561 St1 ∼ 922 [343, 802]
4
F3/2 → 4 I13/2 ∼ 1.331 ns ∼ 1.517 St1 ∼ 922 [766]
YVO4 Nd 3+ 4
F3/2 → 4 I11/2 1.0641 ns 1.1754 St1 ∼ 890 [355, 755]
4
F3/2 → I13/2
4
∼ 1.342 ns ∼ 1.525 St1 ∼ 890 [767]
Yb3+ 2
F5/2 → 2 F7/2 ∼ 1.014 ns ∼ 1.115 St1 ∼ 892 [744]
∼ 1.018 ns ∼ 1.1195 St1 ∼ 892
β-LaBGeO5 Nd3+ 4
F3/2 → 4 I11/2 1.0482 ns 0.8972 ASt2 ∼ 803 [362]
0.9668 ASt1
1.1446 e) St1
GdVO4 Nd3+ 4
F3/2 → 4 I11/2 1.0633 ns 1.1733 St1 ∼ 882 [355, 770]
4
F3/2 → 4 I13/2 ∼ 1.341 ns,ps ∼ 1.521 St1 ∼ 890 [769]
PbMoO4 Nd 3+ 4
F3/2 → I11/2
4
1.0594 ns 1.1668 St1 ∼ 869 [368]
PbWO4 Nd3+ 4
F3/2 → 4 I11/2 1.0580 ns 1.1695 St1 ∼ 901 [368, 372, 436]
a)
In [437, 438] under 14–20 fs pulse generation in LiSrAlF6 and LiSrGaF6 crystals doped with Cr3+ ions self-frequency red-shifted
effects were observed which were preliminarily identified as induced Raman scattering. The point to note here is that in the
colquirite-type crystal (LiCaAlF6 ) under picosecond excitation there was steady-state high-order SRS generation [307].
b)
Tunable nanosecond self-SRS lasing in the α-KY(WO4 )2 :Yb3+ (C Yb = 10 at.% and ωSRS ≈ 908 cm−1 ) crystal was achieved.
c)
20 ns spikes with pumping of ∼ 15 ms train pulses.
d)
Self-SRS lasing was also observed at a wavelength of 1.1868 µm which is related to ωSRS ≈ 947 cm−1 .
e)
Apart from these self-SRS generations, other self-frequency conversion phenomena were also observed (Fig. 33a). Among these
are self-SFG at a wavelength of 0.5471 µm which results from ωSE + ωSt1 (where ωSE = 9540 cm−1 and ωSt1 = 8737 cm−1 )
and self-DFG at wavelengths of 0.9943 and 1.0806 µm which are connected with two other nonlinear processes ωf2 –ωSE and
ωf2 –ωSt1 , respectively (where ωf2 = 18 794 cm−1 ).

Figure 35 Steady-state Raman-induced generation spectrum of Bi4 Ge3 O12 single crystal recorded at 300 K with picosecond laser
pumping at a wavelength of 1.06415 µm [318]. The wavelengths of lines are given in µm (for the anti-Stokes wings only for a few lines).
The identification of self-SFG components in the spectral region of SHG is shown in the inset. Stokes and anti-Stokes lines related to
SRS-active vibration mode ωSRS = 91 cm−1 are indicated by horizontal scale lines. Other notations as in Fig. 16.
Table 16 Self-pumping OPO based on Ln3+ -doped LiNbO3 :MgO single crystals.
lasing stimulated emission optical parametric oscillation ref.

Ln3+ ion
λSE (µm) polarization interaction type phase-matching angle λsignal (µm) λidler (µm)
Nd3+ ∼ 1.084 σ oo-e Θpm ≈ 46.5◦ ∼ 3.6 ∼ 1.6 [441]

Yb 3+
∼ 1.063 π – a)
∼ 1.360 ∼5 [442]
a)
Periodically poled LiNbO3 :MgO bulk single crystal.
LiNbO3 :MgO crystals (Table 16). As in the case of self- 9. Novel technologies in the physics and
FD and self-SRS, self-pumped OPO active laser crystals techniques of crystalline lasers
also play a double role. They yield SE of the activator ions
and parametrically convert the wavelengths of this inter-
In view of the limited scope of this review paper, we shall
cavity generation to the signal and idler wavelengths pre-
consider here only three fast-growing areas in the physics of
serving the energy conservation law ωSE = ωsignal + ωidler
laser crystals connected with novel scientific technologies.
and satisfying the momentum matching condition kSE =
These areas will affect the future of many new applications
ksignal + kidler . It should be noted that for self-pumped
of crystalline lasers. First, of course, we briefly consider ac-
OPO lasers there is no need for an external good-quality
tivated crystals which have been advantageously tested and
pumping beam contrary to the case for conventional OPO
used in LD-pumped crystalline lasers. Although the study
lasers (see, e.g. [103, 386]). Undoubtedly the concepts of
of LD pumping technology is some 40 years old [223],
self-pumped OPO lasers deserve further development.
it is only fairly recent progress in the development and

Figure 36 Steady-state Raman-induced generation spectrum of C15 H19 N3 O2 (AANP) single crystal recorded at 300 K with picosecond
laser pumping at a wavelength of 1.06415 µm with excitation geometry b(aa)b [377]. Anti-Stokes lines and undetectable Stokes lines
(shown by arrows) related to SRS-active vibration mode ωSRS ≈ 1280 cm−1 are indicated by the horizontal scale line. The identification
of self-SFG components are given in parentheses. The dashed line is a fragment of the nonpolarized transmission spectra of an 0.4-mm
thick AANP sample. Other notations as in Fig. 16.
mass production of high-power LD emitters generating mode. To match this axially symmetric cavity mode volume
near wavelengths of 0.8 and 0.95 µm (see, e.g. [448, 613]) with the asymmetric LD emission diagram, it is necessary
that has begun to revolutionize the field of crystalline lasers to use an anamorphic optical system for coupling of both
and rapidly extend their uses. The modern technological lasers (Fig. 37a). The transverse-pumped (or side-pumped)
level of different light-guiding laser structures with a high scheme with monolithic LD arrays is widely used to in-
density of travelling pumping, namely crystalline waveg- crease the energy parameters of LD-pumped crystalline
uides and fibres, is very promising for numerous optoelec- rod lasers (Fig. 37b). Other forms of lasing crystals (bars,
tronic devices. These researches and developments also discs, etc.) will require different system architectures. A
started rather a long time ago, from the beginning of the large body of data for numerous types of LD-pumped crys-
1970s (see, e.g. [620, 623, 626, 656, 675]), but their recent talline laser designs can be found in the relevant detailed
fast progress is inextricably linked with the advances in LD reviews (see, e.g. [9, 103, 615, 616]).
pumping techniques. The efficiency of Xe-flashlamp-pumped crystalline
lasers is a few percent. With LD excitation, this level has
already been reached when the LD efficiency is about 20%
9.1. Laser action of activated crystals and the efficiency of the absorption of the pumping radia-
under LD pumping tion in the majority of known lasing crystals is only 15%.
There are reasons to believe that in the near future the effi-
The longitudinal and transverse schemes are the most usual ciency of high-power LD arrays or other emitting semicon-
for LD pumping of crystalline lasers. The choice of scheme ductor laser structures will increase to 50%. Ultimately, the
is determined, first of all, by the output power of a compos- efficiency of LD-pumped crystalline lasers will amount to
ite laser and, to a lesser extent, by the spectral characteristics tens of percent. LD performance of practically zero inertia
of the pump line of the activator generating ions. Experi- makes it possible to implement a fast-response feedback
ence shows that the longitudinal-pumped (or end-pumped) between crystal laser output and LD and, hence, to atten-
scheme is preferable for crystalline lasers operating in the uate considerably the noise of all LD-pumped crystalline
TEM00 mode at moderate output power. Such a configu- lasers. The Stokes shift, i.e. energy losses of pump photons
ration makes it possible to match a pumping volume of on their conversion to lasing photons, is constant over the
the generating crystals with a volume of the TEM00 cavity pumped volume of a lasing crystal. Moreover, it is fixed

Figure 37 Schematic arrangement of

the most common set-ups for LD-pumped
crystalline lasers: a) one-side transverse
pumping; b) one-end longitudinal pump-
ing; c) thin-disc design [570]. LC, lasing
crystal; L, lens; CL, cylindrical lens; AR,
anti-reflection coating; TS, thermal stabi-
lizer; HS, heat sink; DM, dichroic mir-
ror; FCPPD, fibre-coupled pump diodes;
HR
MP , highly reflecting mirror for LD
pumping wavelength. Other notations as
in Fig. 32.

at a level of 10–50%, depending on the closeness of the 9.3. Crystalline waveguide lasers
wavelengths of the LD pumping and the SE of the crys-
talline lasers, with the exception of ytterbium crystalline
The first crystalline waveguide laser based on a Ho3+ -doped
lasers (see, e.g. [16]). This means that the thermal load of
multicomposite (Y,Er,Tm,Yb)3 Al5 O12 garnet film was re-
the generating active crystal region is less than 50% of the
ported in [675]. For the fabrication of this waveguiding ac-
LD output power.
tive element the liquid-phase epitaxy growth method was
Over the years a new scalable thin-disc laser design used [626]. The 2 µm laser action (5 I7 → 5 I8 channel) of this
(see, e.g. [570, 572]) has been extensively used for ytter- laser has been excited at 77 K using Xe flashlamp pumping.
bium lasers with LD pumping. The basic idea is to use a Over the last few years in several new crystalline waveg-
very thin crystalline plate (some 10 µm thick), one face of uide lasers modern LD pumping has been used (Table 19). It
which is mounted onto a heat sink (Fig. 33c). The small should be noted here that besides the fabrication method of
distance between the heat source and the heat sink results waveguide lasing crystalline layers mentioned above, there
in minor heating of the generating crystal even at kilowatt are several other possible methods, namely slow-culling
pump power densities. This pump scheme provides min- flux, ion implantation, proton exchange, and others (see,
imized thermal optical distortions in lasing crystals and e.g. [676, 677]). These are being continuously improved,
keeps its relatively high beam quality. which has a positive effect on the optical perfection of crys-
By using cascade and cross-cascade laser schemes [18, talline laser waveguiding layers.
21], thermal loading can also be reduced perceptibly. Ul-
timately, this allows one to raise the pulse repetition rate
of high-power crystalline lasers and at the same time is a
technique that allows for crystal cooling. 10. Concluding remarks
There are good grounds to believe that progress in the
field of LD-pumped crystalline lasers will lead not only to The almost 50-year history of the physics of laser crystals
the reinforcement of the role of crystalline lasers but will testifies to the fact that basic research rather than studies
also stimulate the realization of novel laser technologies. connected with the improvements of SE parameters on one
The forefront of research in the direction of the search for or another transitions of an activator lasant or the charac-
new materials for LD-pumped crystalline lasers is summa- teristics of host crystals is most important for further de-
rized in Table 17. velopments. A wide search for new laser crystalline mate-
rials and generating ions, the discovery of new SE channels
(laser wavelengths) and nonlinear potential for frequency
conversion, as well as the development of new operating
9.2. Crystalline “fibre” lasers schemes and pumping methods are all required for further
progress, and thus for the further engineering development
of novel crystalline lasers. It can be stated with confidence
The first crystalline “fibre” laser was demonstrated, as men- that such impetuses to progress are the recent advances out-
tioned above, at the beginning of the 1970s [620]. This lined in this review, namely the discovery of highly trans-
consisted of unclad Y3 Al5 O12 :Nd3+ fibres of 5–10 mm in parent nanocrystalline laser ceramics and numerous χ(3) -
length and 50–125 mm in diameter placed in an exter- and χ(2) -active nonlinear laser crystals (including organ-
nal flat-mirror cavity and end pumped by a Kr ion laser. ics), as well as the development of several new types of
Its room temperature CW generation (4 F3/2 → 4 I11/2 chan- laser self-frequency converters. Crystalline waveguide and
nel) had a threshold as low as 1 mW. This was shortly “fibre” lasers operating under very high laser excitation
followed by the report of a CW “fibre” laser based on density (including LDs) are also of particular interest.
Nd0.5 La0.5 P5 O14 :Nd3+ [623]. It is probable that the first clad Unfortunately, within the space constraints of this re-
crystalline “fibre” laser was based on Y3 Al5 O12 :Nd3+ gar- view article it has been impossible to consider all the inter-
net [628]. This showed a factor of ten improvement over esting trends of modern laser crystal physics. Among these
the unclad ones. All the crystalline “fibre” lasers reported are the results of active investigations of solar-pumped and
thus far have been based on oxide compounds. A relatively “powder” (see, e.g [697, 799, 800]) lasers, as well as some
full list is given in Table 10.3 of [18]. All the crystalline promising outcomes of investigations of crystallized laser
“fibre” lasers reported to date are not real fibre lasers, as are glasses and crystalline lasers pumped by recently devel-
the genuine widely used glass fibre lasers (see, e.g. [668]), oped LDs emitting in the visible and UV regions. The focus
because the majority of them have SE-active elements of of several research teams still remains on the problem of
more than 100 µm in diameter. However, several of them radiation-balanced lasers (see, e.g. [698, 699]). There are
have a diameter much less than 100 µm and are very close good reasons to believe that progress in the basic research
to real guiding laser structures. It is hoped that among these and developments considered and briefly mentioned above
are the “fibre” lasers listed in Table 18. It would seem that will lead not only to improvements in the understanding of
crystalline “fibre” lasers are well on the way to further de- crystalline lasers but will also stimulate research into novel
velopment. laser technologies.

Table 17 Laser-diode-pumped crystalline lasers.
lasing SE channel crystal pumping condition ref.

Ln3+ ion
T (K) LD type a)
Nd3+ 4
F3/2 → 4 I9/2 Y3 Al5 O12 300 ∼ 0.808 [448, 449, 713]
∼ 0.885 [450]
YVO4 300 ∼ 0.807 [451]
GdVO4 300 ∼ 0.808 [452, 710]
LuVO4 300 ∼ 0.806 [771]
SrGdGaO3 ≤ 70 ∼ 0.808 [453]
Sr5 (PO4 )3 F 300 ∼ 0.81 [454]
4
F3/2 → 4 I11/2 LiKYF5 300 ∼ 0.8 [455]
LiYF4 300 ∼ 0.798 [456]
∼ 0.806 [457]
LiYF4 + Y3 Al5 O12 b)
300 ∼ 0.8 [458]
LiGdF4 300 ∼ 0.8 [459]
LiLuF4 300 ∼ 0.798 [460]
∼ 0.805 [461]
KYF4 300 ∼ 0.8 [462]
K2 YF5 300 ∼ 0.804 [462]
CsY2 F7 300 ∼ 0.8 [455]
CsGd2 F7 300 ∼ 0.81 [464]
β-BaY2 F8 300 ∼ 0.8 [465]
α-BaLu2 F8 300 ∼ 0.798 [466]
LaF3 300 ∼ 0.798 [467]
CeF3 300 ∼ 0.81 [468]
α-NaCaYF6 300 ∼ 0.798 [460]
CaF2 –YF3 300 ∼ 0.795 [469]
SrF2 –GdF3 300 ∼ 0.795 [469]
BaF2 –YF3 300 ∼ 0.8 [469]
BaF2 –LaF3 300 ∼ 0.8 [469]
LiNbO3 :MgO 300 ∼ 0.81 [470]
LiNdP4 O12 300 ∼ 0.805 [471]
∼ 0.87 [472]
LiTaO3 300 ∼ 0.806 [396]
NaGdGeO4 300 ∼ 0.81 [467]
NaLuGeO4 300 ∼ 0.81 [467]
KY(MoO4 )2 300 ∼ 0.81 [474]
α-KY(WO4 )2 300 ∼ 0.807 [475]
α-KGd(WO4 )2 300 ∼ 0.806 [475]
α-KLu(WO4 )2 300 ∼ 0.808 [475]
Ca4 Y(BO3 )3 O 300 ∼ 0.812 [397, 398]
Ca4 Gd(BO3 )3 O 300 ∼ 0.81 [476]
∼ 0.887 [473]
CaWO4 300 ∼ 0.81 [477]
SrAl11 O19 :MgO 300 ∼ 0.81 [478]
Y2 O3 (ceramic) 300 ∼ 0.807 [290]
β-YAl3 (BO3 )4 300 ∼ 0.808 [421, 479, 480]


Ln3+ ion
T (K) LD type a)
YAlO3 300 ∼ 0.803 [482]

Y3 Al5 O12 300 ∼ 0.808 [483]
0.8675 [484, 485]
∼ 0.885 [486]
Y3 Al5 O12 (ceramic) 300 ∼ 0.808 [280, 282]
Y2 SiO5 300 ∼ 0.810 [487]
Y3 (Sc,Al)2 Al3 O12 300 ∼ 808 [725]
YVO4 300 ∼ 0.809 [489, 490]
∼ 0.879 [481]
300 ∼ 0.888 [772]
YGdO3 or (Y0.5 Gd0.5 )2 O3 (ceramic) 300 ∼ 0.81 [294]
(Y,Lu)3 Al5 O12 300 ∼ 0.808 [491]
La2 Be2 O5 300 ∼ 0.811 [492]
β-LaBGeO5 300 ∼ 0.8 [493]
LaSc3 (BO3 )4 300 ∼ 0.808 [494]
β-NdAl3 (BO3 )4 300 ∼ 0.807 [495]
NdP5 O14 300 ∼ 0.80 [496]
β-GdAl3 (BO3 )4 300 0.80–0.81 [497]
Gd3 Sc2 Ga3 O12 300 ∼ 0.808 [498, 499]
Gd3 Sc2 Ga3 O12 :Cr3+ 300 ∼ 0.670 [500]
GdVO4 300 ∼ 0.807 [501]
Gd3 Ga5 O12 300 ∼ 0.808 [478, 502]
β -Gd2 (MoO4 )3 300 ∼ 0.81 [503]
Lu2 O3 (ceramics) 300 ∼ 0.81 [293]
LuPO4 300 ∼ 0.81 [488]
PbMoO4 300 ∼ 0.8 [773]
PbWO4 300 ∼ 0.802 [504]
Bi4 Ge3 O12 300 ∼ 0.81 [505, 529]
NaY(WO4 )2 300 ∼ 0.81 [506]
NaLa(MoO4 )2 300 0.794 - 0.811 [774]
NaGd(WO4 )2 300 ∼ 0.81 [477]
KLa(MoO4 )2 300 ∼ 0.805 [507]
Ca3 Sc2 Ge3 O12 300 ∼ 0.805 [508]
Ca2 Ga2 SiO7 300 ∼ 0.808 [509]
Ca3 Ga2 Ge3 O12 300 ∼ 0.8 [679]
Ca3 Ga2 Ge4 O14 300 ∼ 0.81 [510]
CaYAlO4 300 ∼ 0.807 [511]
CaGdAlO4 300 ∼ 0.807 [512]
Ca3 (Nb,Ga)2 Ga3 O12 300 ∼ 0.808 [507]
Sr3 Ga2 Ge4 O14 300 ∼ 0.81 [510]
SrGaGe3 O7 300 ∼ 0.81 [513]
BaLaGa3 O7 300 ∼ 0.809 [514]
Sr0.6 Ba 0.4 (NbO3 )2 300 ∼ 803 [704]
(Y,Gd)VO4 300 ∼ 0.808 [775]


Ln3+ ion
T (K) LD type a)
LaMgAl11 O19 300 0.797 + 0.801 [515, 516]

La3 Ga5 SiO14 300 ∼ 0.81 [510]
La3 Ga5 GeO14 300 ∼ 0.81 [510]
La3 Ga5.5 Nb0.5 O14 300 ∼ 0.81 [510]
La3 Ga5.5 Ta0.5 O14 300 ∼ 0.81 [510]
LaSr2 Ga11 O20 300 ∼ 0.804 [509]
(La,Lu)3 (Lu,Ga)2 Ga3 O12 300 ∼ 0.81 [517]
(Gd,Ca)3 (Mg,Ga,Zr)2 Ga3 O12 300 ∼ 0.81 [478]
Pb3 Ga2 Ge4 O14 300 ∼ 0.808 [776]
Sr5 (PO4 )3 F 300 ∼ 0.805 [518]
Sr5 (VO4 )3 F 300 ∼ 0.809 [519]
Sr5 (VO4 )3 F + YVO4 300 ∼ 0.809 [520]
4
F3/2 → 4 I13/2 LiKYF5 300 ∼ 0.8 [26]
LiYF4 300 ∼ 0.797 [521]
∼ 0.808 [522]
β-BaY2 F8 300 ∼ 0.798 [463]
LiNdP4 O12 300 ∼ 0.805 [523]
α-KGd(WO4 )2 300 0.8085 [524]
Ca4 Y(BO3 )3 O 300 ∼ 0.812 [400]
YAlO3 300 ∼ 0.803 [525]
Y3 Al5 O12 300 ∼ 0.81 [499]
Y3 Al5 O12 (ceramic) 300 ∼ 0.81 [286, 288]
YVO4 300 ∼ 0.808 [526]
β-LaSc3 (BO3 )4 300 ∼ 0.81 [527]
NdP5 O15 300 ∼ 0.801 [528]
GdVO4 300 ∼ 0.808 [527]
Bi3 Ge4 O12 300 ∼ 0.81 [374, 527]
4
F3/2 → 4 I15/2 Y3 Al5 O12 300 ∼ 0.79 [530]
Dy2+ 5
I7 → 5 I8 CaF2 c)
∼ 1.9 ∼ 0.72 [531]
Ho 3+ 5
I6 → I7
5
β-Ba(Y,Yb)2 F8 300 ∼ 0.96 [468]
β-BaYb2 F8 300 ∼ 0.96 [468]
Y3 Sc2 Ga3 O12 :Yb3+ 300 ∼ 0.975 [451]
5
I7 → 5 I8 LiYF4 ≤ 124 ∼ 0.790 [533]
∼ 210 ∼ 0.792 [534]
LiYF4 :Tm3+ 300 ∼ 0.792 [535]
LiYF4 :Er3+ , Tm3+ 300 ∼ 0.79 [533]
LiLuF4 :Tm3+ 300 ∼ 0.793 [537, 538]
KYF4 :Tm3+ 300 ∼ 0.78 [777]
β-BaY2 F8 :Tm3+ 300 0.7895 [539]
YAlO3 :Tm3+ 300 ∼ 0.795 [540, 541]
Y3 Al5 O12 77 0.7855 [542]
Y3 Al5 O12 :Tm3+ 300 ∼ 0.782 [543, 544]
Y3 Al5 O12 :Yb3+ 300 ∼ 0.970 [545]


Ln3+ ion
T (K) LD type a)
GdVO4 :Tm3+ 300 ∼ 0.808 [778]

Lu3 Al5 O12 :Tm 3+
300 ∼ 0.782 [547]
Er 3+ 4
S3/2 → I15/2
4
LiKYF5 d, e)
300 ∼ 0.651 [548]
∼ 0.808
LiYF4 d)
< 90 ∼ 0.802 [549]
LiLuF4 d)
300 ∼ 0.968 [682]
4
S3/2 → I11/2
4
LiYF4 :Yb 3+
300 ∼ 0.968 [550]
4
I9/2 → 4 I11/2 KPb2 Cl5 300 ∼ 0.8 [551]
4
I11/2 → I13/2
4
LiYF4 300 ∼ 0.795 [552, 553]
LiYF4 :Pr3+ f)
300 ∼ 0.97 [554]
β-BaY2 F8 300 ∼ 0.79 [555, 556]
∼ 0.967 [554, 557]
β-Ba(Y,Er)2 F8 300 ∼ 0.969 [558]
α-BaLu2 F8 300 ∼ 0.97 [559, 560]
YAlO3 300 ∼ 0.8 [468]
Y3 Al5 O12 300 ∼ 0.963 [561–563]
Y3 Sc2 Ga3 O12 300 ∼ 0.973 [562, 564]
Gd3 Ga5 O12 300 ∼ 0.79 [565]
∼ 0.97 [562, 564]
SrY4 (SiO4 )3 O 300 ∼ 0.98 [566]
4
I13/2 → I15/2
4
α-KY(WO4 )2 :Yb 3+
300 ∼ 0.965 [567]
Ca4 Y(BO3 )3 O:Yb 3+
300 ∼ 0.976 [568]
Ca4 Gd(BO3 )3 O:Yb3+ 300 ∼ 0.975 [778]
Sc2 SiO5 :Yb 3+
300 ∼ 0.98 [569]
SrY4 (SiO4 )3 O:Yb3+ 300 ∼ 0.98 [566]
Y3 Al5 O12 293 ∼ 0.964 [571]
300 ∼ 1.5 [779]
Y3 Al5 O12 :Yb3+ 300 ∼ 0.946 [530]
YVO4 300 ∼ 0.975 [573]
YVO4 :Yb3+ 300 ∼ 0.975 [573]
LaSc3 (BO3 )4 :Yb 3+
300 ∼ 0.975 [574]
Tm 3+ 1
D2 → H43
β-Ba(Y,Yb)2 F8 d)
300 ∼ 0.96 [193]
1
D2 → H53
β−Ba(Y,Yb)2 F8 d)
300 ∼ 0.96 [193]
3
F4 → 3 H4 LiYF4 :Yb3+ 300 ∼ 0.962 [780]
β-Ba(Y,Yb)2 F8 d)
300 ∼ 0.96 [193]
3
F4 → 3 H5 LiYF4 :Tb3+ 300 ∼ 0.782 [576]
LiYF4 :Ho3+ 300 ∼ 0.791 [577]
LiYF4 :Yb3+ 300 0.685 + 0.960 m)
3
H4 → 3 H6 LiYF4 300 ∼ 0.781 [578]
β-BaY2 F8 300 ∼ 0.781 [781]
α-KY(WO4 )2 :Yb 3+
300 ∼ 1.75 [782]


Ln3+ ion
T (K) LD type a)
α-KY(WO4 )2 :Yb3+ 300 ∼ 0.806 [575]

∼ 0.981
Sc2 O3 300 ∼ 0.786 [579]
Y 2 O3 300 ∼ 0.808 [579]
YAlO3 300 ∼ 0.795 [540, 541]
Y3 Al5 O12 300 ∼ 0.785 [580]
∼ 0.805 [581]
Y3 Al5 O12 :Yb3+ 300 ∼ 0.970 [545]
Y2 SiO5 300 ∼ 0.79 [582]
(Y,Lu)3 Al5 O12 300 ∼ 0.785 [583]
GdVO4 300 ∼ 0.806 [584]
Lu3 Al5 O12 300 ∼ 0.782 [583, 585]
n)
LuVO4 300 0.799–0.803
NaGd(WO4 )2 300 ∼ 0.801 [810]
Ca2 Al2 SiO7 300 ∼ 0.785 [582]
Yb3+ 2
F5/2 → 2 F7/2 Li(Y,Yb)F4 300 ∼ 0.936 [586, 587]
KYF4 300 ∼ 0.97 [783]
CaF2 300 ∼ 0.98 [784]
LiNbO3 :MgO 300 ∼ 0.978 [413]
α-KY(WO4 )2 300 ∼ 0.981 [588]
∼ 0.993 [785]
α-KGd(WO4 )2 300 ∼ 0.981 [434, 588]
α-KYb(WO4 )2 300 ∼ 0.981 [700]
α-KLu(WO4 )2 300 ∼ 0.978 [765]
Ca4 Y(BO3 )3 O 300 0.9764 [589]
Ca4 Gd(BO3 )3 O 300 ∼ 0.976 [590]
Sc2 O3 300 ∼ 0.973 [591, 592]
∼ 0.942 [588]
Sc2 O3 (ceramic) 300 ∼ 0.94 [205, 291, 627]
Sr3 Y(BO3 )3 300 ∼ 0.975 [593]
Y 2 O3 300 ∼ 0.975 [678]
Y2 O3 (ceramic) 300 ∼ 0.94 [291]
Y3 Al5 O12 300 ∼ 0.940 [594, 729, 730]
∼ 0.978 [595]
Y3 Al5 O12 (ceramic) 300 ∼ 0.941 [701]
Y3 (Sc,Al)2 Al3 O12 (ceramic) 300 ∼ 0.970 [711]
β-YAl3 (BO3 )4 300 ∼ 0.976 [417]
Y2 SiO5 300 ∼ 0.978 [596, ]
YVO4 300 ∼ 0.984 [785, 786]
Sr5 (PO4 )3 F 300 0.9004 [599]
Sr5 (VO4 )3 F 300 ∼ 0.907 [600]
SrY4 (SiO4 )3 O 300 ∼ 0.975 [681]
LaSc3 (BO3 )4 300 ∼ 0.974 o)
BaGd2 (MoO4 )4 300 ∼ 0.97 [808]

Gd2 SiO5 300 ∼ 0.975 [790]


Ln3+ ion a)
T (K) LD type
Yb3 Al5 O12 300 ∼ 0.941 [597]
Lu2 O3 300 ∼ 0.950 [588]
Lu2 O3 (ceramic) 300 ∼ 0.95 [715]
Lu3 Al5 O12 100 – 250 ∼ 0.97 [598]
Lu2 SiO5 300 ∼ 0.976 [768]
LuVO4 ∼ 295 0.974-0.981 [789]
NaLa(MoO4 )2 300 ∼ 0.978 [787]
NaLa(WoO4 )2 300 ∼ 0.98 [809]
NaGd(WO4 )2 300 ∼ 0.975 [788]
CaGdAlO4 300 ∼ 0.975 [791]
(Y,Gd)2 SiO5 300 ∼ 0.975 [792]
β-GdAl3 (BO3 )4 300 ∼ 0.974 [807]
U3+ 4
I11/2 → 4 I9/2 CaF2 ∼ 4.2 ∼ 0.840 [223]
Cr 2+ 5
E → T2
5
ZnS 300 ∼ 1.6 [793]
ZnSe 300 ∼ 1.54 [601, 602]
∼ 1.610 [603]
∼ 1.9; ∼2.0
CdMnTe h) 300 ∼ 1.9; ∼2.0 [603]
Cr3+ 2
E → 4 A2 BeAl2 O4 300 ∼ 0.676 [604]
LiCaAlF6 300 ∼ 0.672 [605]
LiSrAlF6 300 ∼ 0.667 [606, 607]
∼ 0.670 [608]
∼ 0.752 g) [609]
LiSrGaF6 300 ∼ 0.672 [610, 611]
Cr4+ p) 3
T2 → 4 A2 Mg2 SiO4 300 ∼ 0.980 [271]
Ca2 GeO4 300 ∼ 0.980 [271]
Y3 Al5 O12 i)
300 ∼ 0.98 [612]
∼ 0.968 [680]
a)
Most extensively employed LDs are: AlGaInP/GaAs type (0.64–0.69 µm), AlGaAs (0.79–0.82 µm), InGaAs (0.9–0.98 µm), and
InGaAsP/InP (1.5–1.9 µm), as well as AlGaIn/AsSb [613]. Pumping wavelength given in µm.
b)
Combined active medium.
c)
Light-emitting diode pumping.
d)
Up conversion lasing.
e)
Crystal grown by Czochralski method.
f)
Laser operation under deactivation process.
g)
(4 A2 → 4 T2 )-absorption-wing-pumped laser.
h)
The composition of crystal was Cd0.55 Mn0.45 Te [603].
i)
“Fibre”-like laser as well [614].
j)
Three-level laser operation at 0.985 µm wavelength.
k)
CW laser action was achieved with (Sr0.7 Ca0.3 )Y(BO3 )3 :Yb3+ crystal [794].
l)
Presentation TuB21 of T.T. Basiev, S.V. Vasiliev, M.E. Doroshenko, and V.V. Osiko in Advanced Solid-State Photonics, OSA
Topical Meeting (Incline Village, Nevada, USA 2006).
m)
Presentation TuB5 of P.S.F. de Matos and N.U. Wetter in Advanced Solid-State Photonics, OSA Topical Meeting (Incline Village,
Nevada, USA 2006).
n)
Presentation WB20 of P. Cerny, J. Oswald, J. Sulc, H. Jelinkova, Y. Urata, and M. Higuchi in Advanced Solid-State Photonics,
OSA Topical Meeting (Incline Village, Nevada, USA 2006).
o)
Presentation WD2 of C. Krakel, J. Johannsen, M. Mond, K. Petermann, and G. Huber in Advanced Solid-State Photonics, OSA
Topical Meeting (Incline Village, Nevada, USA 2006).
p)

Table 18 Crystalline “fibre” lasers with laser pumping.
“fibre” lasing ion SE channel SE generation fibre size a) ref.
T (K) mode diameter length,

(µm) l (mm)
α-Al2 O3 Cr3+ 2
E → 4 A2 77 CW ∼ 60 15 [617]
300 ∼ 40 15 [618]
Y 2 O3 Nd3+ 4
F3/2 → 4 I11/2 300 CW ∼ 60 2.5 [619]
4
F3/2 → 4 I13/2
Y3 Al5 O12 Nd3+ 4
F3/2 → 4 I11/2 300 CW ∼ 50 5–10 [620]
4
F3/2 → 4 I13/2 [621, 622]
La0.5 Nd0.5 P5 O14 Nd3+ 4
F3/2 → 4 I11/2 300 CW ∼ 12 12 [623]
a)
Compared to real fibre glass lasers, the crystalline “fibre” lasers listed here can be considered as fibre lasers only conditionally
(only known “fibre” lasers with active element diameters of less than 100 µm are given in this table). Several crystalline fibre-like
lasers are also known with active element diameters of 0.1–1 mm, e.g. α-Al2 O3 :Ti3+ (∅ = 350 µm and l = 11.2 mm) [683],
Y3 Al5 O12 :Tm3+ (∅ = 1 mm and l = 3 mm) [624], and LiNdP4 O12 :Nd3+ (∅ = 130 µm and l = 1.33 mm) [625], YVO4 :Nd3+
(∅ = 400 µm and l = 1 mm) [795], and Y3 Al5 O12 :Nd3+ (ceramic, (∅ = 0.9 mm and l = 65 mm)) [796]
Table 19 Crystalline waveguide lasers.
active crystalline layer lasing some generation characteristics size of lasing layer pumping ref.
Ln3+ ion source b)
SE channel λSE T mode a) thickness length
(µm) (K) (µm) (mm)
LiYF4 Nd3+ 4
F3/2 → 4 I11/2 1.053 300 CW c) ∼ 12 8 LD [629]
LaF3 Nd 3+ 4
F3/2 → I11/2 ∼ 1.05
4
300 CW , P d) c)
∼ 3.6 7.5 Al2 O3 :Ti 3+
laser [630, 631]
∼ 1.064
4
F3/2 → 4 I13/2 ∼ 1.3 300 CW d) – 7.5 Al2 O3 :Ti3+ laser [631]
LiNbO3 Nd 3+ 4
F3/2 → I11/2 ∼ 1.084
4
300 CW d)
few 27 Al2 O3 :Ti3+ laser [440]
Er3+ 4
I13/2 → 4 I15/2 ∼ 1.532 300 CW, ps c) ∼4 ∼ 50 NaCl–CC laser [632, 633]
∼ 1.563 300 CW, P ∼ 2.55 52 Tl:KCl–CC laser [634]
∼ 1.576
Yb3+ 2
F5/2 → 2 F7/2 ∼ 1.008 300 CW d) few 43 Al2 O3 :Ti3+ laser [635]
∼ 1.030
∼ 1.060
LiNbO3 :MgO Nd3+ 4
F3/2 → 4 I11/2 ∼ 1.085 300 CW, Q- 4–6 8–33 DL, LD, [636–643]
sw c,d) Al2 O3 :Ti3+ laser
∼ 1.091 300 CW few 10 Al2 O3 :Ti3+ laser [427, 644, 645]
LiNbO3 :ZnO Nd 3+ 4
F3/2 → I11/2 1.0846
4
300 CW d)
– ∼ 0.9 Al2 O3 :Ti3+ laser [646]
LiNdP4 O12 Nd3+ 4
F3/2 → 4 I11/2 ∼ 1.047 300 CW, P c,e,f) 4–6 0.5–1.1 DL, Ar ion laser [647–649]
3+
LiTaO3 Nd 1.0763 300 q-CW d) few 20 Al2 O3 :Ti3+ laser [650, 651]
1.0918
1.0923
KY(MoO4 )2 Nd3+ 4
F3/2 → 4 I11/2 1.0643 300 CW, P h) ∼ 50 15–30 Xe, Ar ion laser [652]
1.0669
α-KY(WO4 )2 Yb3+ 2
F5/2 → 2 F7/2 ∼ 1.030 300 CW ∼ 25 3×5 Al2 O3 :Ti3+ laser [797]
KNdP4 O12 Nd 3+ 4
F3/2 → I11/2 ∼ 1.05
4
300 q-CW c)
∼ 28 0.72 Ar ion laser [653, 654]
YAlO3 Nd 3+ 4
F3/2 → I11/2 1.0729
4
300 CW c)
∼4 0.66 DL [655]
1.0795
Y3 Al5 O12 Nd3+ 4
F3/2 → 4 I11/2 1.0641 300 CW, P c,d) 6–8 5–10 Xe, DL, LD [656–659]
4
F3/2 → I13/2 1.3383
4
300 CW 2 10×15 Al2 O3 :Ti3+ laser [798]

active crystalline layer lasing some generation characteristics size of lasing layer pumping ref.
Ln3+ ion source b)
SE channel λSE T mode a) thickness length
(µm) (K) (µm) (mm)
Tm3+ 3
H4 → 3 H6 ∼ 2.02 300 CW d) ∼ 15 4 LD [660, 661]
Yb 3+ 2
F5/2 → F7/2
2
∼ 1.03 300 CW c,g) ∼6 1.6 LD [662–664]
1.048
Y3 Al5 O12 :Yb3+ Er3+ 4
I13/2 → 4 I15/2 ∼ 1.64 300 CW few 1.8 Al2 O3 :Ti3+ [665]
laser
(Y,Yb)3 Al5 O12 i)
Yb3+ 2
F5/2 → 2 F7/2 1.030 300 CW ∼5 5 Al2 O3 :Ti3+ [666]
laser
(Y,Lu)3 (Al,Ga)5 O12 j)
Nd3+ 4
F3/2 → 4 I9/2 ∼ 0.946 300 CW ∼ 3.8 0.95 DL [667]
(Y,Er,Tm,Yb)3 Al5 O12 k)
Ho 3+ 5
I7 → I8
5
∼ 2.098 77 CW ∼ 100 7 W [656, 675]
Gd3 Ga5 O12 Nd3+ 4
F3/2 → 4 I9/2 ∼ 0.937 300 CW d) ∼8 1.2 Al2 O3 :Ti3+ [669]
laser
4
F3/2 → 4 I11/2 ∼ 1.059 300 CW ∼ 2.7 1.25 LD, DL [670–672]
∼ 1.062
Gd3 Ge3 O12 :Nd3+ Yb3+ 2
F5/2 → 2 F7/2 ∼ 1.025 300 CW d) ∼ 3.6 5 Al2 O3 :Ti3+ [673]
laser
Nd3+ 4
F3/2 → 4 I11/2 ∼ 1.067
Ta2 O5 Nd 3+ 4
F3/2 → I11/2
4
∼ 1.068 300 CW ∼3 ∼ 5.5 Al2 O3 :Ti3+ [703]
laser
Bi4 Ga3 O12 Nd3+ 4
F3/2 → 4 I11/2 ∼ 1.064 300 q-CW c) ∼3 5 DL [674]
a)
P, CW, q-CW, Q-sw, and ps: pulse, continuous-wave, quasi-continuous-wave, Q-switched mode, and picosecond pulse lasing
generation modes, respectively.
b)
CC, colour-centre laser; DL, dye laser; Xe and W, xenon and tungsten-iodine lamp pumping sources, respectively (as in Table 10).
c)
Planar waveguide.
d)
Strip or channel waveguide.
e)
Planar slab waveguide with side pumping.
f)
Planar waveguide contains also about 0.01 at.% Bi3+ ions.
g)
Planar waveguide contains also Lu3+ and Ga3+ ions.
h)
Ribbon and sheet waveguides.
i)
According to [666], the real formula for the active crystalline layer is Y2.40 Yb0.49 Nd0.11 Al4.84 Ga0.16 O12 .
j)
According to [667], the active crystalline layer was co-doped with 12 at.% Ga3+ and 35 at.% Lu3+ ions.
k)
According to [675], the real formula for the active crystalline layer is Y1.25 Ho0.1 Er0.55 Tm0.5 Yb0.6 Al5 O12 .
Acknowledgements The author would like to acknowledge cor- the Joint Open Laboratory for Laser Crystals and Precise Laser
dially his numerous scientific friends, primary Professors S. N. Systems, which is a very good foundation for efficient scientific
Bagayev, L. Bohatý, H. J. Eichler, J. Garcia-Sole, A. Z. Grasyuk, cooperation. The author also thanks his other co-workers at the
J. Hanuza, S. Haussühl, R. J. Hemley, H. Klapper, V. I. Konov, Institute of Crystallography for their kind help and cooperation.
O. N. Krokhin, and K. Ueda, as well as Doctors M. Sh. Akchurin, The author acknowledges the assistance and support at different
P. Becker, E. Haussühl, D. Jaque, J. Lu, V. G. Ralchenko, A. Shi- periods of time from the Russian Academy of Sciences, the Rus-
rakawa, K. Takaichi, and H. Yagi, and others who are the co- sian Foundation for Basic Research, as well as from the Alexander
authors of many articles jointly published during last years and von Humboldt Foundation.
cited in this review article. Most of them are active members of

[8] E. Sorokin, I. T. Sorokina, and E. Wintner, Appl. Phys. B

Alexander A. Kaminskii received 72, 3 (2001).
his two scientific degrees (as PhD [9] N. V. Kravtsov, Quantum Electron. 31, 661 (2001).
and doctor) in physical and math- [10] T. Yanagitani, H. Yagi, and M. Ichikawa, Japanese patent
ematical sciences from Institute 10-101333 (1998); T. Yanagitani, H. Yagi, and Y. Hiro,
of Crystallography of the Russian Japanese patent 10-101411 (1998).
Academy of Sciences in 1965 and [11] A. A. Kaminskii, phys. stat. sol. (a) 200, 215 (2003).
1974, respectively. Since 1982, he [12] J. Lu, T. Murai, K. Takaichi, K. Misawa, M. Prabhu, J. Xu,
has been a Full Professor of physics. K. Ueda, H. Yagi, T. Yanagitani, A. Kudryashov, and A. A.
In 2006, Prof. Kaminskii was elected as a Correspond- Kaminskii, Laser Phys. 11, 1053 (2001).
ing Member of the Russian Academy of Science. Since [13] J. Lu, K. Ueda, H. Yagi, T. Yanagitani, Y. Akiyama, and
1994, he has been the Director of the Joint Open Lab- A. A. Kaminskii, J. Alloys Comp. 341, 220 (2002).
oratory for Laser Crystals and Precise Laser Systems [14] G. A. Pasmanik, Laser Focus World 35, 17 (1999).
under the auspices of the Division of Physical Science, [15] J. Hulliger, A. A. Kaminskii, and H. J. Eichler, Adv. Funct.
Russian Academy of Sciences. Currently, he is Head Mater. 11, 243 (2001).
of the Laser Crystal Physics Laboratory at the Insti- [16] W. F. Krupke, IEEE J. Sel. Top. Quantum Electron. 6, 1287
tute of Crystallography, Russian Academy of Sciences, (2000).
Moscow. Prof. Kaminskii is a founder and permanent [17] S. Kück, Appl. Phys. B 72, 515 (2001).
Chairman (since 1976) of the All-Moscow seminar on [18] A. A. Kaminskii, Crystalline Lasers: Physical Processes
physics and spectroscopy of laser crystals. and Operating Schemes (CRC Press, Boca Raton, FL,
Prof. Kaminskii discovered almost half of all known 1996).
laser crystals with lanthanide activators and most of the [19] M. J. Weber, Handbook of Laser Wavelengths (CRC Press,
known SRS-active inorganic and organic crystalline ma- Boca Raton, FL, 2000).
terials. He has opened the door for many practical lasing [20] A. A. Kaminskii, phys. stat. sol. (a) 102, 389 (1987).
[21] A. A. Kaminskii, Laser Crystals: Their Physics and Prop-
oxide and fluoride crystals and discovered many new
erties (Springer, Berlin, 1981 and 1990).
laser channels of triply ionized generated lanthanides
[22] A. A. Kaminskii, B. V. Mill, and A. V. Butashin, Inorg.
which enriched lasing potential of activated crystals.
Mater. 19, 2056 (1983).
His current scientific interests are in the field of physics
[23] A. A. Kaminskii, B. V. Mill, A. V. Butashin, and V. D.
and spectroscopy of laser and nonlinear-laser crystals. Shigorin, Inorg. Mater. 28, 1995 (1992).
Prof. Kaminskii has authored and co-authored over 750 [24] A. A. Kaminskii and N. M. Khaidukov, phys. stat. sol. (a)
scientific research publications, among them are also 47 129, K65 (1992).
review articles and 6 books. [25] A. A. Kaminakii and N. M. Khaidukov, Sov. Phys.-Dokl.
Prof. Kaminskii received several scientific prizes and 37, 143 (1992).
awards for his original contributions in the field of [26] A. A. Kaminskii, V. S. Mironov, S. N. Bagaev, N. M.
laser crystals, including the Alexander von Hum- Khaidukov, M. F. Joubert, B. Jacquier, and G. Boulon,
boldt Research Prize and the Rozhdevstvenskii Prize phys. stat. sol. (a) 145, 177 (1994).
from the Russian Academy of Sciences. Currently, [27] P. L. Summers, H. Weidner, R. E. Peale, and B. H. T. Chai,
Prof. Kaminskii is Vice-chairman of the Quantum Elec- J. Appl. Phys. 75, 2184 (1994).
tronics Commission (C-17) of the International Union [28] W. W. Krühler and G. Huber, Appl. Phys. 8, 261 (1975).
on Pure and Applied Physics (IUPAP). Since the end of [29] G. Wang, M. He, W. Chen, Z. Lin, S. Lu, and Q. Wu,
2006 he is Chairman of the Scientific Council on Atomic Mater. Res. Innov. 2, 341 (1999).
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Laser & Photon. Rev. 1, No. 2, 93–177 (2007) / DOI 10.1002/lpor.

Abstract After a brief examination of known insulating laser crys-

Section of the crystal structure of Na3 Li(SeO4 )2 · 6H2 O, rep-

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Laser crystals and ceramics: recent advances

Received: 31 January 2007, Accepted: 25 February 2007

PACS: 42.55.-f, 42.65.-k, 78.20.-e, 78.45.+h

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

space Ln3+ Ln2+ Ac3+

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

Table 3 Oxide laser host crystals with

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 4 Oxide laser host crystals with ordered

Table 5 Fluoride laser host crystals with disordered

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 6 Oxide laser host crystals with dis-

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

La3 Ga5.5 Nb0.5 O14 D3 2 +

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

mid-IR SE generation can be excited also at wavelengths

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

space Ln3+ Ln2+ TM5+

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

No. SE channel crystal and pumping ref.

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

Figure 3 Example of a simplified chromaticity

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 10 Spectral generation ranges and SE

generation in the vacuum UV

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

0.792 to 0.799 Tm3+ 1

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

2.234 to 2.827 k) U3+ 4

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

No. SE channel crystal and pumping ref.

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

No. SE channel crystal and pumping ref.

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

No. SE channel crystal and pumping ref.

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

No. SE channel crystal and pumping ref.

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

No. SE channel crystal and pumping ref.

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

No. SE channel crystal and pumping ref.

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

No. SE channel crystal and pumping ref.

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

No. SE channel crystal and pumping ref.

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

No. SE channel crystal and pumping ref.

www.lpr-journal.org © 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

the broadband tunable laser operation (1.35–1.55 µm). SE 6. Laser potential

© 2007 by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.lpr-journal.org

R ~ 99.5% 6 6 R~~ 93%

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ceramic space laser and nonlinear-laser characteristics c)

(Y0.5 Er0.5 )3 Al5 O12 k)