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A novel nonlinear optical (NLO) carbonatoperoxovanadate, Cs 3 VO(O 2 ) 2 CO 3 , with an exceptionally high thermostability was successfully synthesized by introducing highly polarizable Cs + cations and inorganic polydentate carbonate anions into asymmetric peroxovanadates. The structure of Cs 3 VO(O 2 ) 2 CO 3 is composed of distorted [VO(O 2 ) 2 CO 3 ] 3- units and charge balancing Cs + cations. The title compound exhibits the largest NLO intensity ever found in the current carbonate NLO materials, i. e., 23.0 times that of KH 2 PO 4 (KDP). The remarkably strong second-harmonic generation (SHG) response originates from the synergistic effect of the exceedingly polarizable Cs + cations, distortive polyhedra of the V 5+ cation, delocalized π orbitals in CO 3 groups, and distorted localized π orbitals in O 2 groups. First-principles calculations indicated that introducing the polarizable cations into peroxovanadates not only induces the enhancement of the SHG response but also improves the thermal stability of the framework.

chemical science

Cs3VO(O2)2CO3: an exceptionally thermostable carbonatoperoxovanadate with an extremely large second-harmonic generation response