Unique determination of the hyperpolarizability tensor ratio through depolarized hyper-Rayleigh scattering under an external electric field

We have analyzed the depolarized hyper-Rayleigh scattering from a molecular system with partial macroscopic polar ordering. It is shown that the hyperpolarizability tensor ratio and the molecular dipole moment can be determined simultaneously by the measurement of depolarization as a function of external field strength. As an experimental example, we performed a quantitative analysis of the electric-field-dependent depolarized hyper-Rayleigh signal from a poly-γ-benzyl-L-glutamate solution, obtaining the dipole moment and the ratio of hyperpolarizability components as 4.0 D and β₃₁₁/₃₃₃ = -0.81, respectively.