Tunable two-dimensional femtosecond spectroscopy.

We have developed a two-dimensional (2D) Fourier-transform femtosecond spectroscopy technique for the visible spectral region. Three-pulse photon echo signals are generated in a phase-matched noncollinear four-wave mixing box geometry that employs a 3-kHz repetition-rate laser system and optical parametric amplification. Nonlinear signals are fully characterized in amplitude and phase by spectral interferometry. Unlike for previous setups, we achieve long-term phase stability by employing diffractive optics and interferometric accuracy of excitation-pulse time delays by using movable glass wedges. As an example of this technique, 2D correlation and relaxation spectra at 600 nm are shown for a solution of Nile Blue dye in acetonitrile.