First-principles study on second-order optical nonlinearity of some ferrocenyl complexes

Abstract

The first static hyperpolarizabilities of some ferrocenyl complexes have been well predicted at MP2 quantum chemical level satisfactorily through the comparison with the recent experiments and the HF and DFT theoretical results. The electronic excitation contribution to the first hyperpolarizability has been elucidated in terms of the two-level model and the linear optical parameters from time-dependent density functional theory calculations. Interestingly, the first hyperpolarizability of neutral complex has a small negative value. But for complex cation, the first hyperpolarizability has a large positive value, and the low-energy charge-transfer excited state may have the dipole moment larger than that of the ground state.