NONLINEAR OPTICAL-PROPERTIES OF H-2 AND D-2

Accurate wave functions of the James-Coolidge type, which account for electron correlation, are used to calculate for H2 and D2 the dynamic second hyperpolarizabilities (γ) which mediate the nonlinear optical processes: dc Kerr, dc electric-field-induced second-harmonic generation and third-harmonic generation. Values are given for a range of frequencies (ω = 0 to ω = 0.05 a.u.) as well as for some common laser frequencies. The effects of vibration are explicitly considered. As well, values of the dynamic field-gradient polarizabilities B and C are found. The results are more accurate than those previously published. © 1990 American Institute of Physics.