Abstract
We are developing a novel method of nonlinear polarization spectroscopy which we term NSE (Nonlinear Spectroscopic Ellipsometry). NSE deals with investigations of the polarization be-havior of a probe beam passing through an isotropic medium in the presence of a strong pumping field. The probe wave polarization parameters are derived in the case of arbitrary polarized in-teracting waves in the framework of the 3rd-order nonlinear susceptibility (3NS). A new method of measuring the phase of the 3NS that is based on the use of circularly polarized probe and linearly polarized pump beams is proposed. The feasibilities of separate measurements of the dis-persion of the real and imaginary parts of the 3NS by the NSE methods are demonstrated. The re-sults of the theoretical consideration are applied to estimate the magnitude of the 3NS of some dye solutions and gaseous media under different conditions of excitation.
