In order to explain the opposite phase matchability of two types of newly discovered chalcogenides, AX2MQ6 vs AX4M5Q12 belonging to the same R3 space group, the linear and nonlinear optical properties are calculated. ...In order to explain the opposite phase matchability of two types of newly discovered chalcogenides, AX2MQ6 vs AX4M5Q12 belonging to the same R3 space group, the linear and nonlinear optical properties are calculated. The calculated Electron Localization Function（ELF） show the acentricity of the bonds on the Q^2- ions with sp^3 hybridization is the main origin of the optical anisotropy. To quantify such an acentricity, a geometric parameter, the dihedral angle between the tetrahedral undersides and the xy-planes is defined. And the calculated birefringence depends on the above defined geometric parameter and the ion radius. This correlation reasonably explains the opposite phase matchability of two closely related chalcogenide families of AX2MQ6 and AX4M5Q12 and is shedding useful light on further exploration on phase matchable IR-NLO crystals.展开更多
Two new halogenated selenites,namely,Pb_(2)Cd(SeO_(3))_(2)X_(2)(X=Cl and Br),were synthesized via mild hydrothermal reactions.The isomorphic compounds crystallized in a noncentrosymmetric(NCS)and chiral space group.Th...Two new halogenated selenites,namely,Pb_(2)Cd(SeO_(3))_(2)X_(2)(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(_(3)D)structures were formed by alternating undulated[Pb_(2)(SeO_(3))X]_(∞)^(+)cationic layers and flattened[Cd(SeO_(3))X]_(∞)^(-)anionic layers.展开更多
Phosphite materials have aroused wide attention due to their diverse open frameworks and promising magnetic and optical performances.Here,the first barium scandium phosphite,BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2),was obtai...Phosphite materials have aroused wide attention due to their diverse open frameworks and promising magnetic and optical performances.Here,the first barium scandium phosphite,BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2),was obtained via a facile hydrothermal route.BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2) crystallizes in the polar space group Pn and exhibits a 3D{[Sc_(2)(HPO_(3))_(4)]^(2−)}_(∞)anion framework constructed by distorted ScO6 octahedra and HPO_(3)^(2−)anion groups.BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2) can exhibit a phase-matchable SHG response of about 0.94×KH_(2)PO_(4) at 1064 nm,and a moderate birefringence(0.036@1064 nm)to satisfy the phase-matchable behavior requirement.Deep investigation of its structure–property relationship based on theoretical calculations has also been presented in this work.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21233009,90922021,20773130,20733003,20803080,20973175)the“Knowledge Innovation Program of the Chinese Academy of Sciences”(KJCX2-YW-H20,CXJJ-11-M71)
文摘In order to explain the opposite phase matchability of two types of newly discovered chalcogenides, AX2MQ6 vs AX4M5Q12 belonging to the same R3 space group, the linear and nonlinear optical properties are calculated. The calculated Electron Localization Function（ELF） show the acentricity of the bonds on the Q^2- ions with sp^3 hybridization is the main origin of the optical anisotropy. To quantify such an acentricity, a geometric parameter, the dihedral angle between the tetrahedral undersides and the xy-planes is defined. And the calculated birefringence depends on the above defined geometric parameter and the ion radius. This correlation reasonably explains the opposite phase matchability of two closely related chalcogenide families of AX2MQ6 and AX4M5Q12 and is shedding useful light on further exploration on phase matchable IR-NLO crystals.
基金supported by the National Natural Science Foundation of China(Grant No.:21773244 and 21875248)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No:XDB20000000)the NSF of Fujian Province(Grant No:2018J01025).
文摘Two new halogenated selenites,namely,Pb_(2)Cd(SeO_(3))_(2)X_(2)(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(_(3)D)structures were formed by alternating undulated[Pb_(2)(SeO_(3))X]_(∞)^(+)cationic layers and flattened[Cd(SeO_(3))X]_(∞)^(-)anionic layers.
基金support by the National natural science foundation of China(21771159,22071212,22101248)the Priority Academic Program Development of Jiangsu Higher Education Institutions,Lvyangjinfeng Talent Program of Yangzhou(YZLYJFJH2021YXBS083)Qinglan Project of Jiangsu Province of China.
文摘Phosphite materials have aroused wide attention due to their diverse open frameworks and promising magnetic and optical performances.Here,the first barium scandium phosphite,BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2),was obtained via a facile hydrothermal route.BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2) crystallizes in the polar space group Pn and exhibits a 3D{[Sc_(2)(HPO_(3))_(4)]^(2−)}_(∞)anion framework constructed by distorted ScO6 octahedra and HPO_(3)^(2−)anion groups.BaSc_(2)(HPO_(3))_(4)(H_(2)O)_(2) can exhibit a phase-matchable SHG response of about 0.94×KH_(2)PO_(4) at 1064 nm,and a moderate birefringence(0.036@1064 nm)to satisfy the phase-matchable behavior requirement.Deep investigation of its structure–property relationship based on theoretical calculations has also been presented in this work.
基金financially supported by the National Natural Science Foundation of China(21827813,21921001,22175172,22075283,92161125,and U21A20508)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2020303 and 2021300)。
