White-Light-Continuum Spectroscopy To Determine Third-Order Nonlinear Optical Properties

The realization of all-optical switching schemes is mostly hindered by the lack of suitable materials with a refractive index change that is large and fast enough. The characterization of the linear and nonlinear optical properties of potential materials is therefore of prime importance. Various characterization methods have been proposed and are employed, yielding different parameters of the nonlinear optical response at the involved laser frequencies. However, in most techniques the resulting nonlinearities are measured only at one point in the spectral dispersion. To generate the whole nonlinear spectra, the laser source has to be tuned over the desired wavelength range and consecutive measurements have to be taken. We propose and demonstrate here a novel technique to measure the nonlinear optical response for a broad wavelength region in a pump-probe scheme that requires no laser tuning. In order to detect the two-photon absorption at several wavelengths simultaneously, we use a white-light-continuum as the probe beam. As the pump beam is held constant, the Kramers-Krönig transformation can be used to calculate the dispersion of the nonlinear refractive index from the two-photon absorption spectrum. By delaying the probe beam relative to the pump beam, the temporal behavior of the nonlinearity can be obtained