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Na2ZnSn_2S6:A mixed-metal thiostannate with large second-harmonic generation response activated by penta-tetrahedral [ZnSn4S(14)]^(10-) clusters

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Science China(Technological Sciences) 2017年第10期60卷 1465-1472页

作者： LI GuangMao WU Kui LIU Qiong YANG ZhiHua pan shilie Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Key Laboratory of Electronic Information Materials and Devices Xinjiang Technical Institute of Physics & Chemistry Chinese Academy of Sciences Urumqi 830011 China University of Chinese Academy of Sciences Beijing 100049 China

A sodium zinc thiostannate Na2ZnSn2S6 is reported with its interesting structural features and property characteristics. It crystallizes in the polar space group Fdd2 （No. 43） with the unit cell parameters ofa=12.945（3） A, b=23.556（5） A, c=7.2774（15）/k and Z=8. In its structure, Zn-centered penta-tetrahedra [ZnSn4S15]Z2- clusters arrange regularly along the diagonals of ab and ac planes to form a 3D tunnel structure with charge-balanced Na＋ cations located inside the tunnels. Note that SnS4 tetrahedra connect with each other by sharing comers to form infinite ∞[SnS3]n chains that are rarely found in known alkali-thiostannates. Remarkably, NazZnSnzS6 exhibits the good NLO performances, such as large SHG response （4 times that of AgGaS2 at 55-88 μm under the 2.09 μm radiation）, wide infrared （IR） transmission region （0.35-25 μm） and relatively high laser damage threshold （77.5 MW/cm2, -2 times that of AgGaS2）. Theoretical calculations have also been performed to investigate the structure-property relationship and the results indicate that the origin of NLO effect can be attributed to the penta-tetrahedra [ZnSn4S15]12- clusters.

关键词： Na2ZnSn2S6 nonlinear optical infrared second-harmonic generation

A Cation-Driven Approach toward Deep-Ultraviolet Nonlinear Optical Materials

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Research 2023年第3期2023卷 781-791页

作者： Cong Hu Meng Cheng Wenqi Jin Jian Han Zhihua Yang shilie pan Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special EnvironmentsXinjiang Technical Institute of Physics&ChemistryCAS40–1 South Beijing RoadUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The design of new materials with special performances is still a great challenge,especially for the deep-ultraviolet nonlinear optical materials in which it is difficult to balance large bandgaps and strong second harmonic generation responses due to their inverse *** variation not only influences the whole structure frameworks but also directly participates in the formation of electronic structures,both of which could lead to the uncontrollability of the properties of the designed ***,a novel approach,aiming at purposeful and foreseeable material designs,is proposed to characterize the role of *** the verification of several series of borates,the influences of cation variation on property changes are explored ***,a feasible strategy of designing deep-ultraviolet nonlinear optical materials by substituting barium for lead has been concluded,which could obviously blue-shift the ultraviolet cutoff edge and maintain the relatively strong second harmonic generation response(more than 2 times of KH2PO4),achieving the property optimization,and especially works efficiently in *** property optimization design strategy and the cation characterization method are not only helpful in exploring nonlinear optical materials but also enlightening in material design and selection.

关键词： materials ultraviolet property

Review on birefringence in borates based on birefringence-active functional groups and arrangements

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Science China Chemistry 2024年第7期67卷 2155-2170页

作者： Qianzhen Zhang Ran An Zhihua Yang Xifa Long shilie pan Yun Yang Research Center for Crystal Materials State Key Laboratory of Functional Materials and Devices for Special Environmental ConditionsXinjiang Key Laboratory of Functional Crystal MaterialsThe Xinjiang Technical Institute of Physics&ChemistryChinese Academy of SciencesUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

As a fundamental parameter of the optical crystals,birefringence plays a vital role in many optical applications,such as phase modulation,light splitting,and polarization,especially the phase matching process of the nonlinear optical *** big birefringence not only benefits to the miniaturization of related devices,but also broadens the phase-matching wavelength range of nonlinear optical *** design and synthesis of crystals with large birefringence becomes a hot research topic due to its more and more important applications in the optical modulation and laser technology ***,crystals with birefringence greater than 0.05 in the borate system are reviewed and classified according to different birefringent active groups,and the relationship between structure and properties is thoroughly *** is hoped that this review will provide a clear understanding of what kinds of building units and arrangements would have more opportunity to get adequate birefringence in borate systems and provide the statistical references to encourage the emergence of better crystal materials with large birefringence.

关键词： birefringence borate optical functional crystal structural anisotropy arrangement of functional units

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Ba_(2)B_(9)O_(13)F_(4)·BF_(4):first fluorooxoborate with unprecedented infinite [B_(18)O_(26)F_(8)] tubes and deep-ultraviolet cutoff edge

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Science China Chemistry 2023年第4期66卷 1073-1077页

作者： Huan Pei Xuefei Wang Jie Zhang Fangfang Zhang Zhihua Yang shilie pan Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special EnvironmentsXinjiang Technical Institute of Physics and ChemistryChinese Academy of SciencesUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Fluorooxoborate has emerged as a promising system for exploring optical materials due to their rich structural chemistry and physicochemical properties,yet so far not fully ***,we report a new fluorooxoborate,Ba_(2)B_(9)O_(13)F_(4)·BF_(4),which contains the greatest variety of structural basic units,[BO_(3)],[BO_(2)F_(2)],[BO_(3)F],and[BF_(4)],and exhibits unprecedented 1D infinite[B_(18)O_(26)F_(8)]*** unique structure avoids the dangling bonds caused by terminal oxygens,which is beneficial to the large bandgap and deep-ultraviolet cutoff *** article expands the crystal structure of fluorooxoborates and contributes to the exploration of deep-ultraviolet optical materials in fluorooxoborate systems.

关键词： fluorooxoborate unprecedented infinite tubes four basic units deep-ultraviolet

Rb_(5)Ba_(2)(B_(10)O_(17))_(2)(BO_(2)):The formation of unusual functional [BO_(2)]^(-) in borates with deep-ultraviolet transmission window

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Science China Chemistry 2022年第4期65卷 719-725页

作者： Yanhui Zhang Fuming Li Rong Yang Yun Yang Fangfang Zhang Zhihua Yang shilie pan CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics&ChemistryChinese Academy of SciencesXinjiang Key Laboratory of Electronic Information Materials and DevicesUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The design and synthesis of new deep-ultraviolet(DUV)optical materials are important but *** is well known that the polarizability anisotropy of linear[BO_(2)]^(−)is larger than those of[BO_(3)]^(3−)and[BO_(4)]^(5−),which is the better choice for exploring excellent optical ***,we search for such crystals in borate systems based on the unusual fundamental structural unit[BO_(2)]^(−).By combining the linear[BO_(2)]^(−)with the traditional triangular[BO_(3)]^(3−)and tetrahedral[BO_(4)]^(5−)units,a new mixed metal borate,Rb_(5)Ba_(2)(B_(10)O_(17))_(2)(BO_(2))was obtained via high-temperature solution *** exhibits excellent optical properties including a DUV transmission window(188 nm)and suitable birefringence(0.06).It also has good thermal stability and its crystal plates can be prepared ***,the strategies of designing borates with[BO_(2)]^(−)units have been proposed from the transformation of crystal framework and the preparation method.

关键词： isolate BO_(2) borate crystal deep-ultraviolet transmission birefringence

From borophosphate to fluoroborophosphate:a rational design of fluorine-induced birefringence enhancement

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Science China Chemistry 2021年第9期64卷 1498-1503页

作者： Wenyao Zhang Zhizhong Zhang Wenqi Jin Ruonan Zhang Meng Cheng Zhihua Yang shilie pan CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics&ChemistryCASXinjiang Key Laboratory of Electronic Information Materials and DevicesUrumqi830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

The introduction of oxofluoride anion into anionic group assists to tune optical properties owing to the change of coordination,electronegativity,and according anionic ***,we proposed a rational design of new compounds by fluorine-driven structure and optical property evolution.A new borophosphate Ba_(2)BP_(3)O_(11)with the monoclinic space group P2_(1/c) has been synthesized in the sealed ***_(2)BP_(3)O_(11)exhibits a rare P-O-P bridge formation,which is the first example in alkaline-earth metal *** further substituting[BO_(4)]^(3-)with[BO_(3)F]^(4-),the first alkaline-earth metal/lead fluoroborophosphates M_(2)BP_(2)O_(8)F(M=Ba and Pb)with the same space group were *** the scissors effect of fluorine,in M_(2)BP_(2)O_(8)F(M=Ba and Pb),a BO_(3)F tetrahedron corner-sharing with three PO_(4)tetrahedra forms 1D chains along the b-axial direction,which are filled by MO_(n)(M=Ba/Pb,n=5,6,8)distorted *** first principles calculation shows that the borophosphate Ba_(2)BP_(3)O_(11)has a birefringence about 0.013@1,064 nm,while the fluoroborophosphates M_(2)BP_(2)O_(8)F(M=Ba and Pb)have the values of 0.035 and 0.043@1,064 nm,*** an apparent enhancement in birefringence is derived from synergies of the oxyfluoride and *** introduction of fluorine-containing heteroanionic groups provides a feasible strategy to design novel promising optical materials.

关键词： borophosphate fluoroborophosphates P-O-P bridges formation birefringence

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An excellent deep-ultraviolet birefringent material based on[BO2]∞ infinite chains

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Light(Science & Applications) 2022年第9期11卷 2217-2224页

作者： FANGFANG ZHANG XINGLONG CHEN MIN ZHANG WENQI JIN SHUJUAN HAN ZHIHUA YANG shilie pan Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special EnvironmentsXinjiang Technical Institute of Physics and ChemistryCAS40-1 South Beijing RoadUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences100049 BeijingChina

Birefringent materials play indispensable roles in modulating the polarization of light and are vital in the laser science and ***,the design of birefringent materials operating in the deep-ultraviolet region(DUV,λ≤200 nm)is still a great *** this work,we developed a new DUV birefringent crystal LiBO_(2) based on[BO2]∞infinite chains in the Li-B-O system,which simultaneously achieves the shortest UV cutoff edge(164 nm)and the largest birefringence(≥0.168 at 266 nm)among all the reported borate-based DUV birefringent *** crystals of LiBO_(2) with dimensions up to Ø55×34 mm^(3) were grown by the Czochralski method,providing access to large-sized single crystal with low ***,it has a high laser damage threshold and stable physicochemical *** outstanding characters unambiguously support that LiBO_(2) can be an excellent birefringent material for DUV application.

关键词： birefringent polarization ultraviolet

Toward the Enhancement of Critical Performance for Deep-Ultraviolet Frequency-Doubling Crystals Utilizing Covalent Tetrahedra

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Accounts of Materials Research 2021年第4期2卷 282-291页

作者： Miriding Mutailipu Zhihua Yang shilie pan CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Technical Institute of Physics&ChemistryUrumqi 830011China Xinjiang Key Laboratory of Electronic Information Materials and Devices Urumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Deep-ultraviolet(deep-UV,λ<200 nm)coherent light is emerging as an indispensable driving force behind the innovation of optics and materials *** deep-UV-driven applications range from laser interference photolithography to precise micromachining to futuristic ideas such as space propulsion using remotely controlled positioning *** conventional approaches to obtaining deep-UV light,for instance,synchrotron radiation,direct laser excitation,and gas discharge,nonlinear frequency conversion can be regarded as a more attractive way to endow such resource with high photon energy,high photon flux,and high spectral ***,the nonlinear frequency conversion can be efficient only with the use of highperforming frequency-doubling crystals,which should be well-suited to the physics of nonlinear optical ***,the necessary prerequisites for a practical frequency-doubling crystal are extremely strict,and thus very few crystals can be used to generate the deep-UV *** with this,sustained effort has been expended by chemists and materials scientists toward discovering novel deep-UV frequency-doubling *** have so far indicated that the main difficulty in finding a perfect candidate comes from the combination of three critical properties(absorption edge,nonlinear optical coefficients,and birefringence)into one crystal because they share the mutual relation of restriction and *** this Account,we present recent progress in discovering emergent deep-UV frequency-doubling crystals with the discussion of our efforts to balance the three critical properties by introducing the covalent tetrahedra[MO4−nXn](n=1−3),in which M refers to central atoms such as B,P,Si,S,Al,Zn,and Be and X can be apical atoms such as F,Cl,Br,and *** analyzing the influence of the covalent tetrahedra on optical properties,we came to the conclusion of how to use the oxidized tetrahedra to achieve the improvement of the absorption edge,nonlinear op

关键词： doubling mutual bonds

Clamping effect driven design and fabrication of new infrared birefringent materials with large optical anisotropy

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Science China Chemistry 2023年第4期66卷 1086-1093页

作者： Linan Wang Chenchen Tu Hongbo Gao Jiazheng Zhou Hongshan Wang Zhihua Yang shilie pan Junjie Li Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special EnvironmentsXinjiang Technical Institute of Physics&ChemistryChinese Academy of SciencesUrumqi 830011China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Infrared(IR)birefringent materials with large optical anisotropy and wide transparency range are important for efficient light manipulation in various IR optical ***,two new IR birefringent materials AMgGeSe_(3)(A=Li,Na)with large optical anisotropy were rationally designed by a rigid octahedron and flexible dimer combined strategy and fabricated in *** introduction of rigid[LiSe_(6)]/[NaSe_(6)]and[MgSe_(6)]octahedra effectively regulates the geometry and arrangement of the flexible[Ge2Se6]dimers,resulting in the birefringence as large as 0.334@1,064 nm in LiMgGeSe_(3) and 0.445@1,064 nm(the largest one in the reported[Ge_(2)Se_(6)]dimer-contained selenides)in NaMgGeSe_(3).Density functional theory(DFT)calculations and statistical analyses highlight the influence of polarizability anisotropy,density,arrangement of units,as well as layer distance on *** results indicate that AMgGeSe_(3)(A=Li,Na)crystals are the promising IR birefringent materials and it gives an insight into the exploration of new IR birefringent materials with large birefringence based on the clamping effect from rigid groups.

关键词： birefringence clamping effect AMgGeSe_(3) [Ge_(2)Se_(6)]dimer octahedra