Proposed experiment to measure nonlinear optical susceptibilities in the saturated regime.

When an optical beam passes through a thin slice of a homogeneous material, the change of its phase and amplitude is characterized by the material's linear and nonlinear susceptibility, the latter also known as the hyperpolarizability. The standard method for measuring the nonlinear susceptibility is the scan. This widely used method is sometimes applied outside of its range of validity, leading to systematic errors. These errors are illustrated for a two-level system with parameters taken from atomic rubidium. The present paper proposes a method called the phase retrieval of modes to determine the nonlinear susceptibility without an assumption about its functional form, in contrast to both the -scan method and variants intended to apply in cases of saturation. In brief, a Gaussian beam passes through a thin sample and is detected on three planes in a focal scan. Phase retrieval methods are used to find coefficients of the modes which in turn determine the optical nonlinear susceptibility. Nearly exact recovery of the nonlinear susceptibility is shown numerically in the no-noise case. Additionally, two types of noise are considered: shot noise on the detector and intensity fluctuations of the input.