Two-photon spectroscopy and analysis with a white-light continuum probe.

We present a powerful experimental tool and analysis for characterization of two-photon absorption (2PA) spectra. We demonstrate this method with ZnS and then apply it to organic dyes in solution. We also compare the results with those from other methods such as two-photon fluorescence spectroscopy. This femtosecond pump-probe method uses a white-light continuum (WLC) as the probe to produce a nondegenerate 2PA spectrum. The extreme chirp of the WLC requires that transmittance data be collected over a range of temporal delays between pump and probe pulses. These data then need to be corrected for the effects of this chirp as well as for the temporal walk-off of the pulses in the sample that result from the frequency nondegenerate nature of the experiment. We present a simple analytic solution for the transmitted fluence through the sample, which is applicable for most practical cases.