Two-dimensional Fourier transform spectroscopy in the pump-probe geometry

Two-dimensional (2D) Fourier transform (FT) infrared spectroscopy is performed by using a collinear pulse-pair pump and probe geometry with conventional optics. Simultaneous collection of the third-order response and pulse-pair timing permit automated phasing and rapid acquisition of 2D absorptive spectra. To demonstrate the ability of this method to capture molecular dynamics, couplings and structure found in the conventional boxcar 2D FT spectroscopy, a series of 2D spectra of a metal carbonyl, and a beta-sheet protein are acquired.