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

Abstract

We analyzed the depolarized hyper-Rayleigh scattering from molecular system with a partial macroscopic polar ordering. It is shown that hyperpolarizability tensor ratio and molecular dipole moment can be determined simultaneously by the depolarization measurement as a function of the 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 Debye and β 311/β333 = -0.81.