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A polarization-resolved beam deflection technique is used to separate the bound-electronic and molecular rotational components of nonlinear refractive transients of molecular gases. Coherent rotational revivals from N(2), O(2), and two isotopologues of carbon disulfide (CS(2)), are identified in gaseous mixtures. Dephasing rates, rotational and centrifugal distortion constants of each species are measured. Polarization at the magic angle allows unambiguous measurement of the bound-electronic nonlinear refractive index of air and second hyperpolarizability of CS(2). Agreement between gas and liquid phase second hyperpolarizability measurements is found using the Lorentz-Lorenz local field correction.

Beam deflection measurement of bound-electronic and rotational nonlinear refraction in molecular gases