Nonlinear dual-comb spectroscopy with two-photon excitation

Dual frequency comb spectroscopy has proven to be a powerful method for acquiring broadband, high resolution spectra with measurement times that are much shorter than in traditional moving-mirror Fourier transform spectroscopy. Because the measurements are carried out with femtosecond lasers, this technique has great potential for decreasing the measurement times and improving the signal-to-noise ratio of nonlinear spectroscopic measurements, such as two-photon excitation or Raman processes. In the case of two-photon excitation, an entire spectrum can be obtained at a given signal level using dual-comb spectroscopy in the same time that a measurement of a single transition frequency would be obtained with a continuous laser of the same average power. In this presentation, I will show the latest results in extending the dual-comb technique to two-photon excitation spectroscopy, with measurements on gas-phase rubidium and liquid-phase dye samples.