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 β<sub>311</sub>/β<sub>333</sub>=−0.81, respectively.
© 2002 Optical Society of America
(190.2620) Nonlinear optics : Harmonic generation and mixing
(190.4160) Nonlinear optics : Multiharmonic generation
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials
(290.5870) Scattering : Scattering, Rayleigh
Jisoo Hwang, Byoungchoo Park, H. J. Chang, and J. W. Wu, "Unique determination of the hyperpolarizability tensor ratio through depolarized hyper-Rayleigh scattering under an external electric field," J. Opt. Soc. Am. B 19, 1620-1626 (2002)