Unique determination of the hyperpolarizability tensor ratio through a depolarized hyper-Rayleigh scattering

Summary form only given. We introduce a depolarized hyper-Rayleigh scattering under an external electric field (e-HRS) to uniquely determine the ratio of hyperpolarizability tensor components. The e-HRS amounts to removing the degeneracy in orientational averages of the first hyperpolarizability tensor components product, (/spl beta//sup 2/) by imparting a partial polar ordering to the molecules in the orientational fluctuation through an external dc electric field. It is shown that this novel process of e-HRS permits determination of the sign and magnitude of the hyperpolarizability tensor ratios as well as the molecular dipole moment. As an experimental example, the ratio of hyperpolarizability tensor components and the permanent dipole moment for poly-/spl gamma/-benzyl-L-glutamate (PBLG) solution in ethylene dichloride (EDC) are determined as /spl beta//sub 311///spl beta//sub 333/ = - 0.81 and 4.0 Debye through e-HRS.