Abstract
A nonlinear optical (NLO) carbonatoperoxovanadate, Rb3 VO(O2 )2 CO3 , was synthesized through a simple solution-evaporation method in phase-pure form. Single-crystal X-ray diffraction revealed that the structure of Rb3 VO(O2 )2 CO3 consists of important noncentrosymmetric (NCS) chromophores, that is, π-delocalized (CO3 )2- groups, a second-order Jahn-Teller (SOJT) distortive V5+ cation, and π-localized distorted O22- groups, as well as charge-balancing polarizable Rb+ ions. The powder second-harmonic generation (SHG) measurements indicated that Rb3 VO(O2 )2 CO3 is phase-matchable (Type I) and exhibits a remarkably strong SHG response circa 21.0 times that of potassium dihydrogen phosphate (KDP), which is the largest efficiency observed among carbonate NLO materials. First-principles calculation analysis suggests that the extremely large SHG response of Rb3 VO(O2 )2 CO3 is attributed to the synergistic effect of the cooperation of all the constituting NCS chromophores.
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