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Review

Multifunctional Optical Crystals for All-Solid-State Raman Lasers

by
Hui Zhao
1,2,
Shibo Dai
1,2,*,
Siqi Zhu
1,2,
Hao Yin
1,2,
Zhen Li
1,2,* and
Zhenqiang Chen
1,2
1
Guangdong Provincial Key Laboratory of Optical Fiber Sensing and Communications, Guangzhou 510632, China
2
Department of Optoelectronic Engineering, Jinan University, Guangzhou 510632, China
*
Authors to whom correspondence should be addressed.
Crystals 2021, 11(2), 114; https://doi.org/10.3390/cryst11020114
Submission received: 10 December 2020 / Revised: 21 January 2021 / Accepted: 23 January 2021 / Published: 26 January 2021
(This article belongs to the Special Issue Multifunctional Optical Crystals for Raman Lasers)
Browse Figures
Versions Notes

Abstract

:
In the past few decades, the multifunctional optical crystals for all-solid-state Raman lasers have been widely studied by many scholars due to their compactness, convenience and excellent performance. In this review, we briefly show two kinds of multifunctional Raman crystals: self-Raman (laser and Raman effects) crystals and self-frequency-doubled Raman (frequency-doubling and Raman effects) crystals. We firstly introduce the properties of the self-Raman laser crystals, including vanadate, tungstate, molybdate and silicate doped with rare earth ions, as well as self-frequency-doubled Raman crystals, including KTiOAsO4 (KTA) and BaTeMo2O9 (BTM). Additionally, the domestic and international progress in research on multifunctional Raman crystals is summarized in the continuous wave, passively Q-switched, actively Q-switched and mode-locked regimes. Finally, we present the bottleneck in multifunctional Raman crystals and the outlook for future development. Through this review, we contribute to a general understanding of multifunctional Raman crystals.

Graphical Abstract

1. Introduction

Stimulated Raman scattering (SRS) is a simple and efficient method to extend the spectral range from ultraviolet to mid-infrared. In 1962, the SRS phenomenon was first detected by Woodbury and Ng when they studied Q-switched ruby lasers with nitrobenzene materials [1]. Thereafter, SRS was observed in liquid and gases. Compared with gas and liquid Raman media, solid-state Raman media have many excellent features such as good thermodynamic performance, narrow Raman line width and stable chemical properties, which are conducive to the generation of the Raman lasers with high reliability and high repetition frequency. A rapid expansion in the number of international research reports have emerged on yellow and eye-safe crystalline Raman lasers aimed at the development of practical devices for a wide range of applications, such as biomedical diagnostics, remote sensing, and laser therapies. Yellow and eye-safe crystalline Raman lasers can be obtained with a combination of frequency doubling and Raman effects, as well as the laser and Raman effects, respectively. Normally, these solid-state Raman laser sources need separate laser and Raman crystals or separate Raman and frequency doubling crystals, which results in a complex structure and a large insertion loss.
During recent decades, the multifunctional Raman optical crystal has emerged as a special kind of crystal, which possesses several effects within one crystal. As a result, the multifunctional Raman optical crystal has the advantages of compactness, easy operation, and low insertion loss [2]. Up to now, most multifunctional Raman optical crystals are self-Raman crystals with laser and Raman properties [3,4], and only a few multifunctional Raman optical crystals are self-frequency-doubled Raman crystals, with both frequency-doubled and Raman properties [5,6]. There are four kinds of self-Raman crystals: tungstate, vanadate, molybdate and silicate crystals. In 1985, the first self-Raman laser was realized by Andryunas et al. [7] with Nd ion doped tungstate potassium Nd:KGW/Nd:KYW at the flashlamp pump. Afterwards, there were no reports on self-Raman lasers for more than ten years, but the types of self-Raman media have been constantly increased in number [8,9,10]. In 1999, the first passively Q-switched (PQS) self-Raman laser was demonstrated with a Yb:KGW crystal by Lagatsky et al. [11]. In the following year, the first actively Q-switched (AQS) self-Raman laser was realized by Findeisen et al. [12] with the anisotropic Nd:KGW crystal. In 2002, Grabtchikov et al. [13] demonstrated the first continuous wave (CW) self-Raman laser with Yb:KYW crystal, and the corresponding optical power conversion efficiency was 10%. The vanadate YVO4 and GdVO4 were later predicted to be excellent materials for SRS [14], and many vanadate self-Raman lasers have been gradually reported with high average powers (>5 W) and high conversion efficiencies (>20%) [15,16,17,18,19,20]. Moreover, the inclusion of second-harmonic generation (SHG) or sum-frequency generation (SFG) crystals has been verified to be an effective approach for yellow-orange-red generation with average output power up to 8.8 W and diode-visible power conversion efficiency of >30% [21]. Until now, only a few self-frequency-doubled Raman crystals have been demonstrated. For instance, in 2009, Liu et al. [5] used a single KTA crystal to perform self-frequency-doubled Raman conversion from the 1064 nm fundamental beam to the 573 nm yellow beam. Another self-frequency-doubled Raman crystal, BTM, was reported by Gao et al. [6] in 2013, and a maximum pulse energy of 5.6 mJ was attained for 589 nm yellow laser radiation.
In this review, we classify all multifunctional Raman optical crystals and list their material properties in the second section. In addition, we focus on the research progress on multifunctional Raman lasers. In parallel with the experimental studies, the theory of SRS has been the subject of several papers [22,23]; thus, a review here is not intended. The article concludes with a summary of multifunctional Raman crystals, and a discussion of opportunities for future development and applications.

2. The Classification of Multifunctional Raman Crystals

2.1. Self-Raman Crystals

2.1.1. Vanadate

As the most popular multifunctional Raman crystal, the vanadate self-Raman crystals include Nd:YVO4 [15,16,20,21,22,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38,39,40,41,42,43,44,45,46,47,48,49,50,51,52,53,54,55,56,57,58,59,60,61,62,63], Nd:GdVO4 [18,19,64,65,66,67,68,69,70,71,72,73,74,75,76,77,78], Yb:YVO4 [17], and Nd:LuVO4 [79,80]. Among these self-Raman laser crystals, Nd:YVO4 has been the most extensively researched and widely employed due to its large Raman gain coefficient, strong absorption of pump radiation over a broad bandwidth, and large emission cross section. Its strongest vibrational Raman mode is located at 890 cm−1 with Raman line width of 3.0 cm−1 and Raman gain coefficient of ~5 cm/GW [14]. In addition, two weak Raman shifts are 816 and 259 cm−1 with respective Raman gain coefficients of 2.6 and 2.3 cm/GW for c-cut Nd:YVO4 crystal with Z(XX) scattering configuration [60]; and 840 and 379 cm−1 with respective Raman gain coefficients of 2.6 and 0.9 cm/GW for a-cut Nd:YVO4 crystal with X(ZZ) scattering configuration [81]. The Nd-doped YVO4 crystal belongs to the zircon type D4h tetragonal space group, and its stimulated radiation cross section parallel to the c axis (a-cut, σ = 25 × 10−19 cm2 at 1064 nm) is four times higher than the cross section orthogonal to the c axis (c-cut, σ = 6.5 × 10−19 cm2 at 1066 nm) [24]. Table 1 gives the Raman and related optical properties of the Nd:YVO4 crystal.
In 2004, the first PQS Nd:YVO4 self-Raman laser was demonstrated by Chen [24], as shown in Figure 1. At the incident pump power of 2.0 W, the laser system produced 0.125 W of average output power at 1178.6 nm with 6.3% of conversion efficiency from diode power to Raman output power. Then, Chen [15,16] demonstrated the AQS Nd:YVO4 self-Raman lasers at 1176 and 1525 nm with maximum average output powers of 1.5 and 1.2 W, respectively, corresponding to conversion efficiencies of 13.9% and 8.9%. In 2006, the first CW Nd:YVO4 self-Raman laser was realized by Burakevich et al. [27], and the maximum output power at 1177 nm was 50 mW with optical power conversion efficiency of 2%. In 2008, a passively mode-locked Nd:YVO4 self-Raman laser at 1176 nm was obtained by M. Weitz [29] with a slow saturable absorber, and maximum average power of 420 mW was delivered with a duration of 4.8 ps and a repetition rate of 73 MHz. An efficient AQS eye-safe Raman laser at 1525 nm using a double-end diffusion-bonded Nd:YVO4 crystal was reported by Chang et al. [31] in 2009, and average power of 2.23 W was generated with a conversion efficiency of 13%. In 2016, a high power CW YVO4/Nd:YVO4/YVO4 self-Raman laser at 1176 nm, pumped by a wavelength-locked 878.9 nm diode laser, was reported by Fan et al. [20], corresponding to maximum output power of 5.3 W and optical conversion efficiency of 20%. To our knowledge, this is the highest power and efficiency among Nd:YVO4 self-Raman lasers up to now. In addition, self-Raman lasers in combination with SHG or SFG can be used to produce yellow light sources. In 2007, the first CW yellow laser at 588 nm was realized by intracavity frequency doubling Nd:YVO4 self-Raman laser [28], corresponding to maximum yellow output power of 140 mW and diode-to-yellow conversion efficiency of 4.4%, respectively. In 2019, a 4.0 W CW Nd:YVO4 self-Raman yellow laser at 588 nm was reported by Chen [59] with conversion efficiency of 12.7%. In 2020, Chen [21] demonstrated an efficient intracavity frequency-doubled AQS Nd:YVO4 self-Raman yellow laser at 588 nm with maximum output power of 8.8 W and diode-to-yellow conversion efficiency of 34%. To the best of our knowledge, this is the highest power and efficiency among self-Raman yellow lasers. In the same year, a PQS YVO4/Nd:YVO4/YVO4 self-Raman yellow laser at 589 nm was demonstrated by Chen et al. [63]. Maximum output power of 0.66 W was attained with an optical conversion efficiency of 3.8%. Table 2 shows the detailed research progress on Nd:YVO4 self-Raman lasers.
Nd:GdVO4 crystal is the isostructural body of the Nd:YVO4 crystal, which also has a zircon structure with tetragonal space group. Compared to the Nd:YVO4 crystal, the Nd:GdVO4 crystal has higher thermal conductivity, which could be beneficial for high power self-Raman laser operation. The strongest Raman shift mode of the Nd:GdVO4 crystal is 882 cm−1 with line width of 3.5 cm−1 and Raman gain coefficient of 4.5 cm/GW [66]. In addition, the secondary Raman transition is located at 382 cm−1 for the X(ZZ)X configuration, and the corresponding Raman gain was estimated to be 0.7cm/GW [73]. Table 3 shows the Raman and related optical properties of the Nd:GdVO4 crystal.
In 2004, Chen [64] reported a PQS Nd:GdVO4 self-Raman laser at 1175.6 nm by using a Cr4+:YAG saturable absorber, and maximum peak power of 8.4 kW was obtained with conversion efficiency of 7%. Due to its large emission cross section and short upper state lifetime, the Cr4+:YAG saturable absorber is not suitable for the PQS Nd:GdVO4 self-Raman laser [65]. In the same year, benefiting from its large absorption cross section and thermal conductivity, the LiF:F2− crystal was employed as a saturable absorber to realize the PQS Nd:GdVO4 self-Raman laser [65]. Maximum peak power of 9 kW was achieved with conversion efficiency of 2%. Several months later, the first AQS Nd:GdVO4 self-Raman laser operating at 1521 nm was delivered by Chen [18] as exhibited in Figure 2, and maximum output power of 1.18 W was achieved with an optical-to-optical conversion efficiency of 8.7%. In 2012, a 4.1 W CW Nd:GdVO4 self-Raman laser using double-end polarized pumping at 880 nm was realized by Lin et al. [74] with an optical conversion efficiency of 11.2%. To our knowledge, this is the highest power among Nd:GdVO4 self-Raman lasers. In 2013, Wang et al. [75] demonstrated a PQS Nd:GdVO4 self-Raman laser at 1176 nm with maximum output power of 0.52 W and optical-to-optical conversion efficiency of 10.3%. Additionally, yellow light sources were obtained through intracavity SHG or SFG of the Nd:GdVO4 self-Raman lasers. In 2008, a 2.51 W CW yellow emission at 586.5 nm was demonstrated by Lee et al. [68] through intracavity frequency-doubling of a Nd:GdVO4 self-Raman laser. Two years later, a 5.3 W CW laser emission at 559 nm with high efficiency (21%) was achieved by intracavity sum-frequency mixing of fundamental and first-Stokes emission in a self-Raman Nd:GdVO4 laser [69]. Table 4 presents the detailed research progress on Nd:GdVO4 self-Raman lasers.
Compared to Nd:YVO4 crystal, Yb:YVO4 crystal has the strong and comparatively broad absorption band near 985 nm, the extremely low quantum defect (~3.5%), and the broad gain bandwidth (~30 nm). Moreover, Yb:YVO4 crystal has a moderate Raman gain coefficient of 4.5 cm/GW at a Raman shift of 892 cm−1. In 2005, the PQS Yb:YVO4 self-Raman laser at 1119.5 nm was achieved by Kisel et al. [17] with pulse energy of 3.6 μJ and pulse duration of 6 ns.
Similar to the Nd:YVO4 and Nd:GdVO4 crystals, the Nd:LuVO4 crystal also has a zircon structure and a space group of I41/amd. Compared to the Nd:YVO4 and Nd:GdVO4 crystals, the Nd:LuVO4 crystal has larger emission cross section (14.6 × 10−19 cm2) and absorption cross section (6.9 × 10−19 cm2). Moreover, the Nd:LuVO4 crystal has a high damage threshold [83,84], and is easy to process. Its Raman frequency shift was determined to be 900 cm−1 with a line width of 5 cm−1 and Raman gain coefficient above 3.2 cm/GW [80]. In 2009, a PQS Nd:LuVO4 self-Raman laser at 1178.8 nm was demonstrated by Kaminskii et al. [79], corresponding to maximum output power of 0.12 W and conversion efficiency of 5%, respectively. In 2010, Lu et al. [80] reported an efficient CW double-end diffusion-bonded Nd:LuVO4 self-Raman yellow laser at 589 nm with maximum output power of 3.5 W and conversion efficiency of 13.3%. Table 5 summarizes the research progress of the Yb:YVO4 and Nd:LuVO4 self-Raman lasers.

2.1.2. Tungstate

According to our surveys, tungstate self-Raman crystals include Nd:KGd(WO4)2 (Nd:KGW) [2,12,85,86,87,88,89,90,91,92,93,94], Yb:KGd(WO4)2 (Yb:KGW) [11,95,96,97], Nd:PbWO4 (Nd:PWO) [98], Yb:KY(WO4)2 (Yb:KYW) [13], Nd:BaWO4 [99], Nd:SrWO4 [99,100], Yb:KLu(WO4)2 (Yb:KLuW) [101] and Nd:KLu(WO4)2 (Nd:KLuW) [102].
The anisotropic Nd:KGW crystal is the most commonly used self-Raman crystal in tungstate. Nd:KGW crystal has a large emission cross section (4.3 × 10−19 cm2) and a wide absorption spectrum [86]. In addition, this crystal can be doped with a high concentration of Nd ions without significant concentration quenching and deterioration of crystal quality. It has two strong Raman vibrational modes at 767 cm−1 (Ng) and 901 cm−1 (Nm) in orthogonal orientations with similar Raman line width of 5.4 cm−1, and the corresponding Raman gain coefficients are 4.4 and 3.3 cm/GW, respectively [26]. Table 6 gives the property parameters of the Nd:KGW crystal.
In 1985, the first self-Raman conversion was observed by Andryunas et al. [85] in Nd:KGW and Nd:KYW crystals, and output energy of 11 mJ was obtained with conversion efficiency of 6.14%. In 1999, the first PQS Nd:KGW self-Raman laser at 1181 nm was realized by Grabtchikov et al. [86], corresponding to output power of 4.8 mW and conversion efficiency of 0.7%, respectively. In 2000, the first acousto-optic Q-switched Nd:KGW self-Raman laser at 1162 nm was achieved by Findeisen et al. [12] with maximum pulse energy of 0.1 mJ. Later, Raman radiation was converted into the yellow laser at 581 nm by the external frequency-doubling technology with the LiB3O5 crystal, and the schematic diagram is displayed in Figure 3.
In 2005, Demidovich et al. [2] reported the first CW Nd:KGW self-Raman laser at 1181 nm with maximum output power of 54 mW and conversion efficiency of 2.6%, as depicted in Figure 4. In the same year, an AQS Nd:KGW self-Raman laser at 1181 nm was realized by Hamano et al. [90] with maximum output power of 0.8 W and optical conversion efficiency of 14%. In 2014, Tang et al. [94] reported a CW Nd:KGW self-Raman laser at 1077.9 nm with maximum output power of 0.42 W and conversion efficiency of 16.8%. Table 7 shows the research progress on the Nd:KGW self-Raman lasers.
Compared to Nd:KGW crystal, Yb:KGW crystal is a promising material for high efficiency due to small quantum defect, high quantum efficiency, and broad absorption bandwidth. Moreover, Yb:KGW crystal is an ideal material for the self-Raman laser because of its large absorption cross section (5.3 × 10−20 cm2), large emission cross section (2.8 × 10−20 cm2) and high nonlinear optical susceptibility [96]. Its two main Raman frequency shift modes are 768 cm−1 (Ng) and 901 cm−1 (Nm). In 1999, the first PQS Yb:KGW self-Raman laser at 1139 nm was attained by Lagatsky et al. [11]. The maximum output power and pulse energy were 7 mW and 0.4 μJ, respectively. In 2003, Kisel et al. [95] demonstrated a PQS Yb:KGW self-Raman laser at 1145 nm with maximum output power of 0.11 W and conversion efficiency from fundamental-to-first Stokes as high as 40%. In 2013, a CW Yb:KGW self-Raman laser at 1110.5 nm was attained by Chang et al. [96], corresponding to the diode-to-Stokes conversion efficiency of 21.8% and highest output power of 1.7 W. In 2019, a quasi-CW Yb:KGW self-Raman laser at 1096 nm was reported by Ferreira et al. [97] with maximum output power of 4.5 W and optical conversion efficiency of 32%.
Compared with the doped KGW crystal, tungstate Nd:PWO crystal has higher Raman gain coefficient (8.4 cm/GW), and the corresponding Raman shift is 901 cm−1 with line width of 4.3 cm−1 [103]. In 2001, a PQS Nd:PWO self-Raman laser at 1170 nm was produced by Chen et al. [98] with maximum output energy of 2.5 μJ and conversion efficiency of 0.1%.
The Yb:KYW crystal has a broad absorption band centered at 981 nm, relatively large absorption coefficient (17 cm−1 for the typical 5 at% Yb3+ concentration), and relatively inexpensive, reproducible, and easy growth [13]. Its Raman frequency shift and Raman gain coefficient are 905 cm−1 and 5.1 cm/GW, respectively [103,104]. In 2002, Grabtchikov et al. [13] reported a PQS Yb:KYW self-Raman laser at 1130 nm with maximum output power of 2 mW.
Nd:BaWO4 and Nd:SrWO4 crystals have similar stimulated Raman scattering cross sections as Nd:KGW crystal. Raman gain coefficients are 8.5 and 5 cm/GW at the Raman shift modes of 926 and 921 cm−1, respectively, corresponding to the Raman line widths of 1.6 and 3.0 cm−1 [99]. In 2004, a PQS Nd:SrWO4 self-Raman laser at 1170 nm was generated by Jelinkova et al. [100] with a pulse energy of 1.3 mJ. In 2006, the PQS Nd:SrWO4 self-Raman laser at 1170 nm and Nd:BaWO4 self-Raman laser at 1169 nm were reported by Sulc et al. [99], and the corresponding pulse energies were 1.23 and 0.81 mJ, respectively.
Yb:KLuW crystal belongs to the monoclinic space group C2/C, and its main absorption center and fluorescence lifetime are 981 nm and 375 μs, respectively. In addition, the physical and spectral properties of Yb:KLuW crystals are similar to those of Yb:KGW and Yb:KYW crystals [105]. The main Raman shift modes are located at 907 and 757 cm−1 [105]. In 2005, Liu et al. [101] demonstrated a PQS Yb:KLuW self-Raman laser at 1137.6 nm, as illustrated in Figure 5. Maximum output power of 0.4 W was obtained with conversion efficiency of 5.7%.
Nd:KLuW crystal belongs to the monoclinic space group C2/C with an emission wavelength of 1070 nm. The absorption cross section of Nd:KLuW crystal at 812 nm is 7.93 × 10−20 cm2, and the emission cross section at 1.07 μm is 2.4 × 10−19 cm2 [106]. The two strongest Raman shifts are located at 907 and 757 cm−1 [107]. In 2015, an AQS Nd:KLuW self-Raman laser at 1185 nm was produced by Cong et al. [102], as shown in Figure 6, and the maximum output power of 1.5 W was attained with conversion efficiency of 9.8%. Table 8 shows the detailed research progress on tungstate self-Raman lasers.

2.1.3. Molybdate

Molybdate self-Raman crystals consist of Nd:PbMoO4 crystal and Nd:SrMoO4 crystal. The Raman gain coefficient of Nd:PbMoO4 crystal is two or three times higher than those of YVO4, GdVO4 and KGW crystals [108]. Its Raman frequency shift is 871 cm−1 with line width of 8.0 cm−1 [107]. In 2005, the PQS Nd:PbMoO4 self-Raman laser at first Stoke wavelength of 1163 nm was reported by Basiev et al. [108] with pulse energy of 6 μJ.
The a-cut Nd:SrMoO4 crystal has a peak emission cross section of 3 × 10−19 cm2 and fluorescence decay time of 180 ms. Its Raman gain coefficient (5.7 cm/GW) is comparable to those of YVO4 and GdVO4 crystals [109]. The Raman shift of Nd:SrMoO4 crystal is 887 cm−1 with line width of 2.5 cm−1 [107]. In 2009, Basiev et al. [109] demonstrated a PQS Nd:SrMoO4 self-Raman laser, as exhibited in Figure 7. Maximum pulse energy of 21 μJ was obtained at a wavelength of 1163 nm.

2.1.4. Silicate

Nd:Y2SiO5 crystal is the only silicate self-Raman multifunctional optical crystal to our knowledge [110]. Its strongest Raman shift is 904 cm−1 with Raman gain coefficient of 2.3 cm/GW and line width of 6 cm−1. Table 9 gives the detailed property parameters of this crystal. In 2010, Kaminskii et al. [110] demonstrated an AQS Nd:Y2SiO5 self-Raman laser at 1194.7 nm, and maximum output power of 28 mW was obtained with conversion efficiency of ~0.6%.

2.2. Self-Frequency-Doubled Raman Crystals

2.2.1. KTiOAsO4 (KTA) and KTiOPO4 (KTP)

KTA crystal has an orthorhombic structure with non-centro-symmetric point group C2v (mm2) and space group Pna21 (Z58). Due to the high nonlinear coefficient (d33 = 16.2 pm/V) and high damage threshold (>300 MW/cm2), KTA crystal has been used in optical parametric oscillators (OPOs) since the 1990s [111,112]. In 1996, Tu et al. [113] proved that KTA is an excellent Raman medium with Raman gain coefficients of ~2.5 cm/GW at 234 cm−1 and ~0.6 cm/GW at 671 cm−1, respectively, and corresponding Raman line widths of 5.8 and 19 cm−1. The KTA crystal was first reported by Liu et al. [5] as a self-frequency-doubled Raman crystal in 2009, as displayed in Figure 8. The KTA self-frequency-doubled Raman laser at 573 nm was realized with Raman shift of 671 cm−1, and maximum output power of 0.82 W was obtained with conversion efficiency of 7.5%.
KTP crystal belongs to the family of KTA crystal. KTP crystal possesses the superior qualities of a high nonlinear coefficient and a high damage threshold [114]. In 2005, KTP crystal was recognized as a self-frequency-doubled Raman crystal by Chen [114], and its strongest Raman shift is 270 cm−1 with Raman gain coefficient of ~2.5 cm/GW. As depicted in Figure 9, the KTP self-frequency-doubled Raman laser at 548 nm was realized from the AQS 1064 nm Nd:YAG laser, and maximum output power of 0.25 W was obtained with conversion efficiency of 2.5%.

2.2.2. BaTeMo2O9 (BTM)

BTM crystallized in a monoclinic system with space group P21 [115]. In 2012, Yu et al. confirmed that the BTM crystal has a wide transmission band (0.4–5 μm), large nonlinear coefficient (d31 = 9.88 pm/V) and high optical damage threshold (544 MW/cm2), flexible phase-matching, and high chemical, and mechanical stabilities [116]. Its strongest Raman shift is 915.2 cm−1 with line width of ~4.4 cm−1 [6]. In 2013, the BTM crystal was employed as self-frequency-doubled Raman crystal to generate the yellow laser at 589 nm, as illustrated in Figure 10 [6]. Maximum pulse energy of 5.6 mJ was achieved at a pump pulse energy of 48 mJ, corresponding to optical-to-optical conversion efficiency of 11.7%.

3. Summary and Outlook

In this review, the Raman and related optical properties of self-Raman crystals and self-frequency-doubled Raman crystals are introduced systematically. Significant progress has been made on the self-Raman lasers in the CW, AQS and PQS regimes after years of effort, while few studies have focused on self-frequency-doubled Raman crystals. To date, the self-Raman laser has attained >5 W average power with high conversion efficiency (>20%). Several target self-Raman lasers in the red-yellow, 1.2 μm, and 1.5 μm regions were realized through adaption to different fundamental wavelengths, cascaded Raman effect, and intracavity harmonic generation. By using intracavity frequency doubling technology, the maximum average power has so far risen to 8.8 W in the yellow spectral region.
Although the self-Raman crystals make the laser system more compact and simpler, output power and conversion efficiency are severely hindered by the thermal loading from the combined laser and Raman processes. Moreover, it is difficult to separately optimize the laser mode sizes on the laser and Raman crystals, which will further impede high power and high beam quality laser output. The future developments of multifunctional Raman crystals could be carried out from the following points of view:
  • Reducing the thermal lens effect of the self-Raman crystals by using gradient doping or diffusion-bonded crystal, in-band pumping technique, double-ended pumping structure, and improving the thermal management with chemical vapor deposition (CVD)-Diamond.
  • Improving average power, conversion efficiency and beam quality by adopting various cavity arrangements instead of the simple straight cavity.
  • Generating high power (tens of watts) 1.2 μm and 1.5 μm lasers for applications in remote sensing, tracking and ranging and directed energy; generating high brightness and high spectral power density lasers in the red-yellow region for spectroscopic applications, atom cooling and sodium guide stars.
  • Narrowing the line width of the fundamental laser by using etalons or other methods, thereby improving Raman gain coefficient and Raman conversion efficiency; even a multi-watt single-longitudinal-mode self-Raman laser could be obtained based on the absence of spatial hole burning in the Raman medium.
  • Ultrafast self-Raman lasers are a potential area for special wavelength development.
  • Extending the wavelength range, such as generating deep-red lasers for applications in fluorescence imaging and photodynamic therapy; generating 1.7 μm lasers for applications in biological engineering, photoacoustic imaging, and welding high-density polymers and hydrocarbon-containing materials.

Author Contributions

Conceptualization, Z.L. and Z.C.; methodology, S.D.; investigation, H.Z.; resources, Z.C.; data curation, H.Z.; writing—original draft preparation, H.Z.; writing—review and editing, S.D.; visualization, S.Z.; supervision, H.Y.; project administration, H.Y.; funding acquisition, Z.L. and Z.C. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by National Natural Science Foundation of China (grant numbers 61935010, 61735005, 51972149, 11974146, 51872307); Research and Development Program in Key Areas of Guangdong Province (grant number 2020B090922006); National Key Research and Development Program of China (grant number 2017YFB1104500); Guangzhou Science and Technology Project (grant number 201903010042).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflict of interest.

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Crystals 11 00114 g001 550
Figure 1. Schematic of the passively Q-switched Nd:YVO4 self-Raman laser [24].
Figure 1. Schematic of the passively Q-switched Nd:YVO4 self-Raman laser [24].
Crystals 11 00114 g001
Crystals 11 00114 g002 550
Figure 2. Schematic of actively Q-switched Nd:GdVO4 self-Raman laser [18].
Figure 2. Schematic of actively Q-switched Nd:GdVO4 self-Raman laser [18].
Crystals 11 00114 g002
Crystals 11 00114 g003 550
Figure 3. Schematic of the first actively Q-switched self-Raman laser [12].
Figure 3. Schematic of the first actively Q-switched self-Raman laser [12].
Crystals 11 00114 g003
Crystals 11 00114 g004 550
Figure 4. Schematic of the first continuous-wave self-Raman laser [2].
Figure 4. Schematic of the first continuous-wave self-Raman laser [2].
Crystals 11 00114 g004
Crystals 11 00114 g005 550
Figure 5. Schematic diagram of the PQS Yb:KLuW self-Raman laser setup; LC, laser crystal; SA, saturable absorber [101].
Figure 5. Schematic diagram of the PQS Yb:KLuW self-Raman laser setup; LC, laser crystal; SA, saturable absorber [101].
Crystals 11 00114 g005
Crystals 11 00114 g006 550
Figure 6. Schematic diagram of the actively Q-switched Yb:KLuW self-Raman laser [102].
Figure 6. Schematic diagram of the actively Q-switched Yb:KLuW self-Raman laser [102].
Crystals 11 00114 g006
Crystals 11 00114 g007 550
Figure 7. Schematic diagram of the PQS Nd:GdVO4 self-Raman laser: LD, laser diode; L, focusing lens; C, laser crystal; VSA, saturable absorber with variable transmission; OC, output coupler [109].
Figure 7. Schematic diagram of the PQS Nd:GdVO4 self-Raman laser: LD, laser diode; L, focusing lens; C, laser crystal; VSA, saturable absorber with variable transmission; OC, output coupler [109].
Crystals 11 00114 g007
Crystals 11 00114 g008 550
Figure 8. Schematic diagram of the KTiOAsO4 (KTA) self-frequency-doubled Raman laser [5]: LD, laser diode; CL, coupling lens; RM, rear mirror; OC, output coupler; DM, dichroic mirror; AO, acousto-optic; AR, antireflection; HT, high transmission; HR, high reflection.
Figure 8. Schematic diagram of the KTiOAsO4 (KTA) self-frequency-doubled Raman laser [5]: LD, laser diode; CL, coupling lens; RM, rear mirror; OC, output coupler; DM, dichroic mirror; AO, acousto-optic; AR, antireflection; HT, high transmission; HR, high reflection.
Crystals 11 00114 g008
Crystals 11 00114 g009 550
Figure 9. Schematic diagram of the KTP self-frequency-doubled Raman laser [114]: AO, acousto-optic; PR, partial reflection; HT, high transmission; HR, high reflection.
Figure 9. Schematic diagram of the KTP self-frequency-doubled Raman laser [114]: AO, acousto-optic; PR, partial reflection; HT, high transmission; HR, high reflection.
Crystals 11 00114 g009
Crystals 11 00114 g010 550
Figure 10. Schematic diagram of the BaTeMo2O9 (BTM) self-frequency-doubled Raman laser at 589 nm [6].
Figure 10. Schematic diagram of the BaTeMo2O9 (BTM) self-frequency-doubled Raman laser at 589 nm [6].
Crystals 11 00114 g010
Table
Table 1. The property parameters of the Nd:YVO4 crystal [26].
Table 1. The property parameters of the Nd:YVO4 crystal [26].
ParametersValue
Space groupTetragonal
Lattice constants (nm)a = b = 0.7123, c = 0.6292
Fluorescence lifetime (μs) 100
Refractive indices (300 K)no = 1.96, ne = 2.17
Thermal conductivity (W/mK)5.10 {a}, 5.23 {c}
Thermo-optic coefficients (dn/dT 10−7 K−1)15.2 {a}, 7.9 {c}
Raman shift (cm−1)890
Raman line width (cm−1)3.0
Raman gain coefficients at 1.06 μm (cm/GW)4.5 [37];
5 [46]
Emission cross-section σem at 1.06 μm (10−19 cm2) 25 {∥c}, 6.5 {⊥c}
Thermal expansion coefficients (10−6 K−1) 4.43 {a}, 11.37 {c}
Table
Table 2. Research progress on Nd:YVO4 self-Raman lasers.
Table 2. Research progress on Nd:YVO4 self-Raman lasers.
YearsPump PowerCNdCW
/Pulse		Output
Wavelength
(nm)		Stokes
Component		Output
Power
(W)		EfficiencyRefs.
20042.0 W@808 nm 0.5%PQS1178.61st Stokes0.1256.3%[24]
200410.8 W@808 nm0.2%AQS11761st Stokes1.513.9%[15]
200413.5 W@808 nm0.2%AQS15251st Stokes1.28.9%[16]
200610.2 W@808 nm0.2%AQS11761st Stokes0.575.6%[25]
20061.8 W@808 nm0.5%AQS11761st Stokes0.18210%[26]
20062.5 W@807.5 nm0.8%CW11771st Stokes0.052%[27]
2006809 nm0.2%AQS11761st Stokes------[22]
20073.2 W@810 nm0.3%CW1176→5881st Stokes0.144.4%[28]
2008809 nm---PML11761st Stokes0.42---[29]
20087.7 W@808 nm0.5%AQS11781st Stokes1.418.2%[30]
200917.2 W@808 nm0.3%AQS15251st Stokes2.2313%[31]
20094.4 W@808 nm0.3%PQS1176→5881st Stokes0.265.9%[32]
200923.6 W@808 nm0.3%AQS1176→5881st Stokes5.724.2%[33]
200926.3 W@808 nm0.3%AQS1176→5881st Stokes7.930%[34]
200918.0 W@808 nm0.3%AQS1173.61st Stokes2.2112.28%[35]
201022.4 W@808 nm0.4%QCW1176 + 1064→5591st Stokes0.472.1%[36]
201025.0 W@808 nm0.3%AQS11761st Stokes3.112.4%[37]
201023.6 W@808 nm0.3%CW11761st Stokes1.847.8%[38]
201018.2 W@880 nm0.3%CW1176 + 1064→5591st Stokes0.894.9%[39]
201025.5 W@808 nm0.27%CW11751st Stokes2.811%[40]
201012.4 W@880 nm0.5%AQS10971st Stokes1.4511.7%[41]
20113.8 W@808 nm1%CW1176→587.81st Stokes0.225.8%[42]
201116.2 W@808 nm0.3%AQS1178→5891st Stokes2.1513.3%[43]
201114.0 W@808 nm0.3%AQS1178 + 1066→5601st Stokes0.846%[44]
201110.2 W@880 nm0.3%AQS15251st Stokes1.9519.2%[45]
201214.6 W@808 nm0.3%AQS13132nd Stokes2.3416%[46]
201214.4 W@808 nm0.3%AQS15241st Stokes1.087.5%[47]
20137.9 W@808 nm0.3%PQS11781st Stokes0.810.1%[48]
201330.0 W@808 nm0.3%AQS + ML11761st Stokes1.836.1%[49]
201430.0 W@808 nm0.3%AQS + ML1313.42nd Stokes1.334.43%[50]
201430.6 W@880 nm0.3%AQS15251st Stokes5.217%[51]
201533.3 W@880 nm1.1%CW11761st Stokes1.85.4%[52]
20165.0 W@808 nm0.27%PQS1066.8
1097.2
1129.2
1168.3
1178.8		1st Stokes/
2nd Stokes		0.2675.3%[53]
201626.5 W@879 nm0.3%CW11761st Stokes5.320%[20]
201717.0 W@808 nm0.3%AQS1215
1255
1316		1st Stokes/
2nd Stokes		1.026%[54]
201812.0 W@808 nm0.3%AQS11761st Stokes1.210%[55]
20188.1 W@808 nm0.5%PQS10971st Stokes0.759.3%[56]
201920.6 W@880 nm0.4%PQS11781st Stokes2.5312.3%[57]
201931.6 W@808 nm0.3%CW1064→532
1176+1064→559
1176→588
1st Stokes6.8
5.4
3.1		9.8%[58]
201963.0 W@808 nm0.3%CW1064→532
1176→588 		1st Stokes812.7%[59]
201926.1 W@879 nm0.3%CW1168.4/1176/
1178.7/1201.6		1st Stokes2.569.8%[60]
202010.0 W@808 nm0.3%CW1064→532
1176 + 1064→559
1176→588		1st Stokes2.424%[61]
202025.9 W@808 nm0.2%AQS1176→5881st Stokes8.834%[21]
2020878.6 nm0.3%AQS15251st Stokes------[62]
202017.4 W@808 nm0.4%PQS1178→5891st Stokes0.663.8%[63]
CNd: Nd doping concentration; CW: continuous wave; QCW: quasi continuous wave; PQS: passively Q-switched; AQS: actively Q-switched; ML: mode locked; PML: passively mode locked.
Table
Table 3. Laser characteristic parameters of the Nd:GdVO4 crystal [14,82].
Table 3. Laser characteristic parameters of the Nd:GdVO4 crystal [14,82].
ParametersValue
Space groupTetragonal
Lattice constants (nm)a = b = 0.7211, c = 0.6350
Fluorescence lifetime (μs)95
Refractive indices (300k)no = 1.97, ne = 2.19
Thermal conductivity (W/mK)10.1 {a}, 11.7 {c}
Thermo-optic coefficients (dn/dT 10−6K−1)13.8 {a}, 10.1 {c}
Raman shift (cm−1)882
Raman line width (cm−1)3.5
Raman gain coefficient at 1.06 μm (cm/GW)4.5
Emission cross-section σem at 1.06 μm (10−19cm2)7.6 {∥c}, 1.2 {⊥c}
Thermal expansion coefficients (10−6 K−1)1.5 {a}, 7.3 {c}
Table
Table 4. Research progress on the Nd:GdVO4 self-Raman lasers.
Table 4. Research progress on the Nd:GdVO4 self-Raman lasers.
YearsPump PowerC NdCW
/Pulse		Output
Wavelength
(nm)		Stokes
Component		Output
Power
(W)		EfficiencyRefs.
20042.0 W@808 nm 0.5%PQS1175.61st Stokes0.147%[64]
20044.0 W@808 nm0.5%PQS11741st Stokes0.082%[65]
200413.6 W@808 nm0.27%AQS15211st Stokes1.188.7%[18]
20061.3 W@808 nm0.5%AQS11761st Stokes0.18%[66]
20079.6 W@808 nm0.2%AQS11731st Stokes1.2212.7%[19]
200716.1 W@808 nm0.3%CW11731st Stokes212.4%[67]
200820.6 W@880 nm0.3%CW1173→586.51st Stokes2.5112.2%[68]
201025.2 W@880 nm 0.3%CW1173 + 1063→5591st Stokes5.321%[69]
201014.0 W@879 nm0.3%CW13082nd Stokes0.956.8%[70]
201025.1 W@879 nm0.3%CW1173→5861st Stokes4.317.1%[71]
2012808/879 nm0.3%CW11731st Stokes0.643.7%[72]
201229.0 W@880 nm0.3%CW1108 + 1063→542
1108→554
1156 + 1108→566
1156→577		1st Stokes/
2nd Stokes		3.4
2.8
1.4
0.8		11.7%
9.7%
4.8%
2.7%		[73]
201236.2 W@880 nm0.3%CW11731st Stokes4.111.2%[74]
20135.0 W@808 nm0.5%PQS11761st Stokes0.5210.3%[75]
20136.8 W@879 nm0.3%CW11731st Stokes0.385.6%[76]
201418.3 W@879 nm0.3%CW1173→5861st Stokes0.734%[77]
20205.6 W@879 nm0.3%CW1108
1173		1st Stokes0.05
0.13		0.9%
2.3%		[78]
C Nd: Nd doping concentration; CW: continuous wave; PQS: passively Q-switched; AQS: actively Q-switched.
Table
Table 5. Research progress on the Yb:YVO4 and Nd:LuVO4 self-Raman lasers.
Table 5. Research progress on the Yb:YVO4 and Nd:LuVO4 self-Raman lasers.
YearsPump powerCrystal CW
/Pulse		Output
Wavelength
(nm)		Stokes
Component		Output
Power
(W)		EfficiencyRefs.
20052.1 W@980 nmYb: YVO4CW
and
PQS		1023 (CW)
1018 (PQS)
1119.5 (PQS)		1st Stokes1
0.46
0.09		4.2%[17]
20092.4 W@808 nmNd: LuVO4PQS1178.81st Stokes0.125%[79]
201026.3 W@880 nmNd: LuVO4CW1178→5891st Stokes3.513.3%[80]
CW: continuous wave; PQS: passively Q-switched.
Table
Table 6. Property parameters of the Nd:KGW crystal [26].
Table 6. Property parameters of the Nd:KGW crystal [26].
ParametersValue
Space groupMonoclinic
Lattice constants (nm)a = 0.8098, b = 1.0417,
c = 0.7583, β = 94.43°
Fluorescence lifetime (μs) 110
Refractive indices (300 K)ng = 2.003, nm = 1.986, np = 1.937
Thermal conductivity (W/mK)2.6 {1 0 0}, 3.8 {0 1 0}, 3.4 {0 0 1}
Thermo-optic coefficients (dn/dT 10−7K−1)−8 {K‖p, E‖m}, −55 {K‖p, E‖g}
Raman shift (cm −1)767, 901
Raman line width (cm −1)5.4 {767}, 5.4 {901}
Raman gain coefficient (cm/GW)4.4 {767}, 3.3 {901}
Emission cross-section σem (10−19cm2) @1μm4.3
Thermal expansion coefficients (10−6K−1)4.0 {1 0 0}, 1.6 {0 1 0}, 8.5 {0 0 1}
Table
Table 7. Research progress on Nd:KGW self-Raman lasers.
Table 7. Research progress on Nd:KGW self-Raman lasers.
YearsPump Power/EnergyC NdCW
/Pulse		Output Wavelength
(nm)		Stokes
Component		Output
Power/
Energy		EfficiencyRefs.
19850.18 J3%pulse1182.71st Stokes11 mJ6.14%[85]
1999806–812 nm4%PQS11811st Stokes4.8 mW0.7%[86]
2000808 nm1%AQS11621st Stokes0.1 mJ---[12]
2000806–812 nm4%PQS11811st Stokes8.9 mW---[87]
20028.0 J---AQS15381st Stokes20 mJ0.3%[88]
200312.6 J@809 nm5%AQS11811st Stokes340 mJ2.7%[89]
20052.1 W@807.5 nm3%CW11811st Stokes54 mW2.6%[2]
20055.7 W@808 nm5%AQS11811st Stokes0.8 W14%[90]
20071.22 J1.5, 2, 3, 5%AQS15381st Stokes31.8 mJ2.6%[91]
20071.3 W@808 nm4%CW11811st Stokes0.277 W22%[92]
20080.18 mJ---ML11801st Stokes0.06 mJ33%[93]
20142.5 W@808 nm5%CW1077.91st Stokes0.42 W16.8%[94]
C Nd: Nd doping concentration; CW: continuous wave; PQS: passively Q-switched; AQS: actively Q-switched; ML: mode locked.
Table
Table 8. Research progress on tungstate self-Raman lasers.
Table 8. Research progress on tungstate self-Raman lasers.
YearsPump
Power/Energy		Crystal CW
/Pulse		Output
Wavelength
(nm)		Stokes
Component		Output
Power/
Energy		EfficiencyRefs.
1999980 nmYb:KGWPQS11391st Stokes7 mW---[11]
20012.5 mJ@802 nmNd:PWOPQS11701st Stokes2.5 μJ0.1%[98]
2002980 nmYb:KYWCW11301st Stokes---10%[13]
20030.3 W@984 nmYb:KGWPQS11451st Stokes0.11 W40%[95]
200424.1 mJ@752 nmNd:SrWO4PQS11701st Stokes1.3 mJ5.4%[100]
20057.0 W@978 nmYb:KLuWPQS1137.61st Stokes0.4 W5.7%[101]
2006752 nmNd:BaWO4
Nd:SrWO4		PQS11691st Stokes1.23 mJ---[99]
20137.8 W@980 nmYb:KGWCW1110.51st Stokes1.7 W21.8%[96]
201515.3 W@808 nmNd:KLuWAQS11861st Stokes1.5 W9.8%[102]
201914.1 W@940 nmYb:KGWQCW10961st Stokes4.5 W32%[97]
CW: continuous wave; QCW: quasi-continuous wave; PQS: passively Q-switched; AQS: actively Q-switched.
Table
Table 9. Property parameters of Nd:Y2SiO5 crystal [110].
Table 9. Property parameters of Nd:Y2SiO5 crystal [110].
ParametersValue
Space groupMonoclinic
Lattice constants (nm)a = 14.371, b = 6.710, c = 10.388, β = 122.17°
Fluorescence lifetime (μs) 250
Density (g/cm3)4.3
Thermal conductivity (W/mK)4.5
Melting temperature (°C)2000
Raman shift (cm−1)904
Raman line width (cm−1)6
Raman gain coefficient (cm/GW)2.3@1078 nm
Emission cross-section σem (10−19 cm2) 1
Optical damage threshold (J/cm2) 7.6
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Zhao, H.; Dai, S.; Zhu, S.; Yin, H.; Li, Z.; Chen, Z. Multifunctional Optical Crystals for All-Solid-State Raman Lasers. Crystals 2021, 11, 114. https://doi.org/10.3390/cryst11020114

AMA Style

Zhao H, Dai S, Zhu S, Yin H, Li Z, Chen Z. Multifunctional Optical Crystals for All-Solid-State Raman Lasers. Crystals. 2021; 11(2):114. https://doi.org/10.3390/cryst11020114

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Zhao, Hui, Shibo Dai, Siqi Zhu, Hao Yin, Zhen Li, and Zhenqiang Chen. 2021. "Multifunctional Optical Crystals for All-Solid-State Raman Lasers" Crystals 11, no. 2: 114. https://doi.org/10.3390/cryst11020114

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