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Strong Kleinman-forbidden second harmonic generation in chiral sulfide: La4InSbS9
Hua-Jun Zhao1, Yong-Fan Zhang, Ling Chen
1Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China.
Abstract:
A new chiral sulfide family, Ln(4)InSbS(9) (Ln = La, Pr, Nd), with its own structure type in space group P4(1)2(1)2 or its enantiomorph P4(3)2(1)2 has been synthesized by solid-state reaction. Remarkably, the La member shows the strongest Kleinman-forbidden second harmonic generation to date, with an intensity 1.5 times that of commercial AgGaS(2) at a laser wavelength of 2.05 μm, and exhibits type-I phase-matchable behavior. Density functional theory calculations and ab initio molecular dynamics simulations suggest that lattice vibrations may be responsible for the origin and magnitude of the strong SHG effect.
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