Calculation of frequency-dependent second hyperpolarizabilities for electric field induced second harmonic generation in the second-order Moller-Plesset perturbation theory

摘要

The calculations of frequency-dependent second hyperpolarizabilities for the (static) electric field induced second harmonic generation (ESHG) [#gamma#(-2#omega#;#omega#,#omega#,0)] of the FH, H_2O, CO, and HN_3 molecules in the second-order Moller-Plesset perturbation theory (MP2) based on the quasienergy derivative (QED) method are performed by numerical differentiation of frequency-dependent first hyperpolarizabilities for the second harmonic generation (SHG) [#beta#(-2#omega#;#omega#,#omega#)] with respect to static electric fields. The QED-MP2 values of the ESHG second hyperpolarizabilities #gamma#_(||)(-2#omega#;#omega#,#omega#,0) of the H_2O, CO, and NH_3 molecules show good agreement with the experimental values.