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Polysubstitution Induced Centrosymmetric-to-Noncentrosymmetric Structural Transformation and Nonlinear-Optical Behavior: The Case of Na 0.45 Ag 0.55 Ga 3 Se 5 .
Inorganic Chemistry 2024 March 23
Obtaining compounds with large nonlinear-optical (NLO) coefficients and wide band gaps is challenging due to their competitive requirements for chemical bonds. Herein, the first member with mixed cations on the A site in the A-M3 -Q5 or A-Ag-M6 -Q10 (A = alkali metal; M = Ga, In; Q = S, Se, Te) family, viz. Na0.45 Ag0.55 Ga3 Se5 (NAGSe), was obtained by a solid-state reaction. Its structure features [GaSe4 ] tetrahedra built three-dimensional {[Ga3 Se5 ]- }∞ network, with Na and Na/Ag cations located at the octahedral cavities. Noncentrosymmetric ( R 32) NAGSe can also be transformed from centrosymmetric RbGa3 S5 ( P 21 / c ) via multiple-site cosubstitution. NAGSe exhibits the highest NLO response (1.9 × AGS) in the A-Ag-M-Q family. Crystal structure analysis and theoretical calculations suggest that the NLO response is mainly contributed by the regularly arranged [GaSe4 ] units. This work enriches the exploration of the undeveloped A-M3 -Q5 or A-Ag-M6 -Q10 family as potential infrared NLO materials.
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