Non-centrosymmetric(NCS)structure is an indispensable prerequisite for second-order nonlinear optical(NLO)material.Currently,the mainstream approach for designing new NCS structures still relies on chemical substituti...Non-centrosymmetric(NCS)structure is an indispensable prerequisite for second-order nonlinear optical(NLO)material.Currently,the mainstream approach for designing new NCS structures still relies on chemical substitution,necessitating an urgent infusion of fresh ideas.In this work,two isomorphic sulfides AeMn_(6)Ga_(6)S_(16)(Ae=Ca,1;Sr,2)are afforded by modifying the skeleton of centrosymmetric(CS)Mn_(2)Ga_(2)S_(5) via introducing strong electropositive alkaline-earth cations.Concretely,the incorporation of Ca^(2+)/Sr^(2+)cations allows the elementary[MnGaS_(9)]_(∞)chains to reconfigure into bumpy[MnS_(6)]-[GaS_(4)]layers in a new engagement manner,thus enabling the conversion from CS to NCS structure.Such modifications cause not only strong second-harmonic generation(SHG)responses(~1.5×benchmark AgGaS_(2)@1,700 nm),but also significantly feasible bandgaps(2.60-2.64 e V)compared to the sulfide Mn_(2)Ga_(2)S_(5)(1.36 e V),which ultimately facilitate ultrahigh laser-induced damage thresholds(4.4-6.6×AgGaS_(2)@1,064 nm for compounds 1 and 2).The present study offers an ingenious approach for the transformation of CS to NCS structure.展开更多
基金supported by the National Natural Science Foundation of China(21827813,21921001,22175172,22075283,92161125,U21A20508)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2020303,2021300)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2020ZZ108)。
文摘Non-centrosymmetric(NCS)structure is an indispensable prerequisite for second-order nonlinear optical(NLO)material.Currently,the mainstream approach for designing new NCS structures still relies on chemical substitution,necessitating an urgent infusion of fresh ideas.In this work,two isomorphic sulfides AeMn_(6)Ga_(6)S_(16)(Ae=Ca,1;Sr,2)are afforded by modifying the skeleton of centrosymmetric(CS)Mn_(2)Ga_(2)S_(5) via introducing strong electropositive alkaline-earth cations.Concretely,the incorporation of Ca^(2+)/Sr^(2+)cations allows the elementary[MnGaS_(9)]_(∞)chains to reconfigure into bumpy[MnS_(6)]-[GaS_(4)]layers in a new engagement manner,thus enabling the conversion from CS to NCS structure.Such modifications cause not only strong second-harmonic generation(SHG)responses(~1.5×benchmark AgGaS_(2)@1,700 nm),but also significantly feasible bandgaps(2.60-2.64 e V)compared to the sulfide Mn_(2)Ga_(2)S_(5)(1.36 e V),which ultimately facilitate ultrahigh laser-induced damage thresholds(4.4-6.6×AgGaS_(2)@1,064 nm for compounds 1 and 2).The present study offers an ingenious approach for the transformation of CS to NCS structure.
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)。
