Journal of Materials Chemistry C
·
2017
·Vol. 5
·期 42
·11025-11029
·
IF 5.256
Bingqing Zhao,Yi Yang,Sangen Zhao,Yaoguo Shen,Xianfeng Li,Lina Li,Chengmin Ji,Zheshuai Lin,Junhua Luo
Nonlinear optical (NLO) crystals are key materials for generation of coherent light in solid state lasers. A new NLO material Rb2ZnSi3O8 is synthesized by the traditional solid-state reaction technique and its crystals are obtained by spontaneous crystallization using an Rb2O–B2O3 flux. It crystallizes in an asymmetric space group of C2 (No. 5) and features a three-dimensional framework composed of SiO4 and ZnO4 tetrahedral groups. Remarkably, it exhibits a phase-matchable powder second harmonic generation approximately 2.5 times that of α-SiO2, which is well known to be non-phase-matchable. The first-principle calculations reveal that the Si–O and Zn–O tetrahedra determine the optical properties in the Rb2ZnSi3O8 crystal and may be the origin of the phase matching behavior in Rb2ZnSi3O8. The UV-visual-near-infrared diffuse reflectance spectrum shows that Rb2ZnSi3O8 has a wide transparency window down to the deep-UV spectral region. In addition, Rb2ZnSi3O8 is non-hygroscopic. These results suggest that Rb2ZnSi3O8 is a potential deep-UV NLO crystal.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
Science China-Materials
·
2023
·Vol. 66
·期 7
·2795-2802
·
IF 8.1
Zheng Zhe-Xiong,Qiu Zhi-Xin,Xie Chao-Hong,Zhang Yang-Ping,Jiang Xiao-Ming,Liu Bin-Wen,Guo Guo-Cong
Strong second-harmonic generation (SHG) and phase-matchable capability at specific transmittance windows are crucial to the real application of nonlinear optical crystals. Herein, an efficient strategy of introducing Pb 2+ with stereochemically active lone-pair electrons into non-phase-match-able Ga 2 Se 3 via enhancing the anisotropy microstructure is first applied to meet phase-matchable SHG intensity requirements, offering a selenide, namely, PbGa 4 Se 7 , which is designed and synthesized with a diamond-like anionic framework, where Pb 2+ cations reside in a parallel arrangement. As expected, PbGa 4 Se 7 possesses a large SHG coefficient of 3.3 times that of AgGaS 2 under the incident laser of 1910 nm. Moreover, PbGa 4 Se 7 displays a high laser-induced damage threshold of 7.0 times that of AgGaS 2 at 2090 nm, which originates from the low anisotropy of thermal expansion coefficient (0.36) and suitable optical band gap (2.1 eV). Theoretical calculations demonstrate that the considerable phase-matchable SHG response of PbGa 4 Se 7 can be attributed to the synergies of tetrahedral GaSe 4 and pyramid PbSe 3 microstructural blocks with additional anisotropy and polarizability.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 9
·2681-2689
·
IF 6.1
Jiazheng Zhou,Hongshan Wang,Junjie Liu,Xin Su,Yu Chu,Jiale Qu,Xiangzhan Jiang
Two new thiohalides Pb3GeS4Br2 and Pb3.5GeS4Br3 have been synthesized by introducing Pb2+ into the thiogermanate system. The compounds crystallize in centrosymmetric P21/c (Pb3GeS4Br2) and non-centrosymmetric P63 (Pb3.5GeS4Br3) space groups, respectively. To the best of our knowledge, Pb3GeS4Br2 and Pb3.5GeS4Br3 are the first Pb-containing thiogermanate halides, and the latter is the first phase-matching IR nonlinear optical material in the thiogermanate halide system. Due to the presence of Pb2+ with stereochemically active lone pair electrons, Pb3GeS4Br2 exhibits a strong optical anisotropy with a birefringence of 0.131@1064 nm, while Pb3.5GeS4Br3 shows a large second-harmonic generation response (0.8 × AgGaS2) and high laser-induced damage threshold (3.0 × AgGaS2). These results enrich the structural and chemical diversity of chalcohalides.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Photonics
·
2023
·Vol. 17
·期 8
·694-701
·
IF 35
Mutailipu Miriding,Han Jian,Li Zhi,Li Fuming,Li Junjie,Zhang Fangfang,Long Xifa,Yang Zhihua,Pan Shilie
Phase-matching of light waves is a critical condition for maximizing the efficiency of nonlinear frequency conversion processes in nonlinear optical crystals; however, phase-matching, commonly achieved by tuning birefringence, is often difficult to achieve over a wide wavelength range. Here, full-wavelength phase-matching crystals that can avoid phase-mismatching across the entire optical transparency range are proposed. The anisotropic strength of bonding in the dimension of energy is confirmed theoretically to be the key to the full-wavelength phase-matching ability. We demonstrate that a crystal of guanidinium tetrafluoroborate (C(NH 2 ) 3 BF 4 ) can be phase-matched throughout its entire optical transparency range and is able to generate harmonic light as short as ~193.2 nm, which is close to its deep-ultraviolet cut-off edge. Importantly, this crystal is stable, cheap and efficient compared with commercially available nonlinear optical crystals for generation of 266 nm light. This work lays the foundation for finding a new class of crystals in which the phase-matching wavelength fully covers its optical transparency range, and also provides a high-performance crystal for generating light at 266 nm—the fourth-harmonic of a commercial 1,064 nm laser.
研究领域:
光学
·
材料科学
·
非线性光学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ming-Xin Li,Yan Guo,Meng-Na Jing,Meng-Ke Gao,Xiao-Ming Jiang,Bin-Wen Liu,Guo-Cong Guo
Achieving phase-matching (PM) behavior, which is typically derived from sufficient birefringence (Δn), is crucial for maximizing the nonlinear optics (NLO) laser power output. Δn is largely attributed to the configuration and arrangement of microstructural units, and phase transitions will significantly alter the stacking method of structural units. In this study, we successfully synthesized two diamond-like isomers of α-KGa5Se8 (P21, 1) and β-KGa5Se8 (P1, 2), which consist of open-honeycomb-like anionic frameworks interspersed with embedded K+ cations. Importantly, our analysis of frequency doubling experiment data revealed a significant finding at a laser wavelength of 1910 nm: the α-phase lacks PM capability, whereas the β-phase exhibits PM behavior. Notably, through structural and computational analysis, the distinct Δn primarily stems from the different arrangements of tetrahedral units within the two phases. Specifically, the polarizability anisotropy of the tetrahedral units in β-KGa5Se8 is 3.7 times that of α-KGa5Se8. This uniform packing improves the Δn index from 0.015 (α-phase) to 0.023 (β-phase). Furthermore, β-KGa5Se8 not only demonstrates a robust PM second-harmonic generation (SHG) response (2.1 × AgGaS2 @1910 nm) but also possesses a wide band gap of 2.56 eV, surpassing the 2.33 eV threshold that corresponds to the energy of doubly frequency light using the 1064 nm laser, a characteristic often not exceeding in most selenides. This work underscores the importance of the configuration and arrangement of microstructural units for achieving PM in NLO materials.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 29
·12331-12337
·
IF 3.5
Sujuan Yu,Jiangtao Fan,Zhanggui Hu,Yicheng Wu
The exploration of nonlinear optical crystals with ultraviolet (UV) transparent ranges and easy-to-grow large-size crystals is one of the current research interests. Herein, by combining borate and phosphate groups, a novel congruently melting alkali-mixed metal borophosphate, Li3Na7B4P6O26 (LNBPO) with UV transparency was successfully designed and synthesized using a high-temperature flux method. LNBPO crystallizes in the non-centrosymmetric (NCS) and polar orthorhombic space group Pca21 (no. 29), showcasing interesting (B2P3O13)∞ chains along the c axis. Notably, LNBPO has a moderate second harmonic generation (SHG) response (∼0.38 × KDP) and displays a wide transmission ranging from 0.22 to 3.68 μm, as measured by a [001]-oriented crystal wafer. Furthermore, a high-quality single crystal of LNBPO with sizes up to 14 × 14 × 12 mm3 was grown using the top-seeded solution growth method. The refractive indices of LNBPO were determined by applying the minimum deviation angle method. These results show that LNBPO possesses a phase-matching wavelength as short as 483 nm, indicating its potential as a new UV NLO crystal.
研究领域:
材料科学
·
晶体学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2024
·Vol. 21
·期 1
·2408485
·
IF 13
Lin-Tao Jiang,Yi-Bing Huang,Shao-Min Pei,Xiao-Ming Jiang,Bin-Wen Liu,Guo-Cong Guo
The trigonal planar unit possesses significant hyperpolarizability and polarizability anisotropy, which makes it useful for optimizing nonlinear optical (NLO) materials, however, chalcogenide with this unit has seldom been reported. In this work, a novel approach is introduced by integrating the unprecedented trigonal planar MS 3 (M = Cd/In, Hg/In) motifs into the nearly optically isotropic tetrahedral units, resulting in two novel chalcogenides CsM 2 In 2 S 6 (M = Cd/In, 1 ; Hg/In, 2 ). Notably, structures 1 and 2 feature nearly planar triangular units at the center, encircled by three trimers, further interconnecting each other to create 3D frameworks. Importantly, phases 1 and 2 display phase-matching (PM) capabilities, primarily attributed to incorporating trigonal planar MS 3 units that additionally enhance polarizability anisotropy. Furthermore, compounds 1 and 2 demonstrate moderate second-harmonic generation (SHG) signals (0.70 and 0.84 × AgGaS2@1.7 µm). This study pioneers an efficient strategy for the design of infrared NLO crystals with PM capabilities.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 11
·3133-3139
·
IF 5.934
Ya-Ping Gong,Chun-Li Hu,Yun-Xiang Ma,Jiang-Gao Mao,Fang Kong
Two new halogenated selenites, namely, Pb2Cd(SeO3)2X2 (X = Cl and Br), were synthesized via mild hydrothermal reactions. The isomorphic compounds crystallized in a noncentrosymmetric (NCS) and chiral space group. Their three-dimensional (3D) structures were formed by alternating undulated [Pb2(SeO3)X]∞+ cationic layers and flattened [Cd(SeO3)X]∞− anionic layers. Thermal analyses revealed that the compounds can remain stable up to 500 °C. The SHG efficiencies of Pb2Cd(SeO3)2X2 (X = Cl and Br) are much higher than those of commercial KDP (KH2PO4), and they are phase-matchable. UV-vis-NIR diffuse reflectance spectra revealed that the two compounds exhibited wide optical band gaps. The laser damage thresholds of Pb2Cd(SeO3)2X2 (X = Cl and Br) were measured to be about 38.5 and 35.7 times higher than that of AGS (AgGaS2). Their calculated birefringences were large enough to accomplish phase matching in SHG progression. The SHG density analyses disclosed that the lone pair electrons of the SeO3 and PbOnXm units made major contributions to their nonlinear efficiencies.
研究领域:
材料科学
·
晶体学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 7
·2030-2038
·
IF 7
He-Di Yang,Sheng-Hua Zhou,Mao-Yin Ran,Xin-Tao Wu,Hua Lin,Qi-Long Zhu
Transition-metal-based chalcogenides have recently emerged as greatly promising infrared nonlinear optical (IR-NLO) candidates due to their unique structural chemistries and rich optical properties. However, Fe-based IR-NLO chalcogenides with phase-matching (PM) features have not yet been reported. In this work, a new non-centrosymmetric (NCS) melilite oxychalcogenide, Sr2FeGe2OS6, has been prepared by an isomorphous substitution method, and the relationships between the microscopic crystal structure and macroscopic NLO activity were systematically investigated. Sr2FeGe2OS6 adopts the tetragonal space group of P21m (no. 113) and features a unique two-dimensional structure with Cairo pentagonal tiling layers formed by the alternating connection of [Ge2OS6] dimers and [FeS4] tetrahedra via corner-sharing and with the charge-balanced Sr2+ cations between these layers. Excitingly, Sr2FeGe2OS6 is the first Fe-based example capable of achieving PM in the IR-NLO chalcogenide system and displays an outstanding IR-NLO comprehensive performance, including a wide energy gap (Eg = 2.24 eV), sufficient second-harmonic-generation (SHG) efficiency (deff = 5.89 pm V−1 at 2050 nm) and strong laser-induced damage threshold (LIDT = 14.42 MW cm−2). Deeper structural and theoretical analysis suggests that the ordered arrangement of NLO-active motifs, [Ge2OS6] dimers and [FeS4] tetrahedra, makes significant contributions to the strong deff and large birefringence (Δn). This work not only demonstrates a PM Fe-based NCS material for the first time but also puts forward a new design avenue for high-performance IR-NLO materials.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 12
·2310407
·
IF 19
Yipeng Song,Hongwei Yu,Bingxuan Li,Xiaoqi Li,Yang Zhou,Yanqiang Li,Chao He,Ge Zhang,Junhua Luo,Sangen Zhao
Phase matching is indispensable for high efficiency of second-order nonlinear optical (NLO) crystals. Thousands of these crystals rely on birefringence phase matching, whereas only a few of them are quasi-phase matching without the restriction of birefringence. Herein, using oriented seeds inch-sized LiNH 4 SO 4 (LAS) single crystals are successfully grown. LAS is NLO-active with a very short deep-UV absorption edge of 171 nm and high laser damage threshold up to 1.47 GW cm −2 at 1064 nm, 10 ns, but its birefringence is merely 0.0078@532 nm, which is too small to realize birefringence phase matching in deep-UV region. Fortunately, P − E hysteresis loop, variable-temperature NLO tests, and ferroelectric domain observations confirm that LAS is ferroelectric. Furthermore, LAS exhibits small refractive index dispersion resulting in a relatively long periodic length of 1.4 µm and its single domain structure can be easily obtained by electrical poling. These attributes make LAS a scarce NLO candidate for deep-UV quasi-phase matching. This work highlights the longly overlooked potential of sulfates and provides new opportunities for deep-UV NLO materials.
研究领域:
材料科学
·
光学工程
·
凝聚态物理
·
无机化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 11
·期 1
·107-113
·
IF 7
Zihao Yu,Qingran Ding,Yuhang Jiang,Weiqi Huang,Changsheng Yang,Sangen Zhao,Junhua Luo
The research on nonlinear optical (NLO) crystals is mainly focused on two relatively separate systems, π-conjugated or non-π-conjugated systems, respectively. In this work, we report a new NLO crystal Na10Zn(NO3)4(SO3S)4 combining inorganic π-conjugated [NO3] and non-π-conjugated heteroanion [S2O3] groups, which was synthesized by the aqueous solution method. In the structure, the similar coexistence of planar triangular anionic groups (π-conjugated) and heteroanion tetrahedra (non-π-conjugated) is rarely mentioned, which provides a new approach for designing NLO crystals. Notably, this compound exhibits a phase-matching second-harmonic generation (SHG) response 1.2 times that of KH2PO4. In addition, birefringence, absorption edge and theoretical calculations are also reported in this article. This work provides a new designing route to expand NLO systems via combining planar π-conjugated and non-π-conjugated heteroanion groups.
研究领域:
材料科学
·
光学材料
·
晶体化学
·
非线性光学
·
功能材料
✓ 已验证
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2021
·
IF 9.811
Runqing Liu,Hongping Wu,Hongwei Yu,Zhanggui Hu,Jiyang Wang,Yicheng Wu
KBe2BO3F2 (KBBF) is the sole nonlinear optical (NLO) crystal that can practically generate deep-ultraviolet (UV) coherent light by a direct second-harmonic generation (SHG) process. However, the toxic BeO and crystal layer habit limit its application. With this background, a new beryllium-free borate, K5Mg2La3(BO3)6 (KMLBO), has been designed and synthesized through a high-temperature solution method. KMLBO crystallizes into the noncentrosymmetric space group P31m (No. 157) and features a three-dimensional framework structure consisting of alveolate [LaBO3]∞ layers further tightly bound via interlayer [BO3]3– groups. KMLBO not only exhibits desirable performances including deep-UV transparency, large SHG (∼3.1 × KH2PO4), and phase-matchability but also overcomes the crystal layer habit of KBBF, demonstrating that it is a potential deep-UV NLO crystal.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）