Ultrafast nonequilibrium Fourier-transform two-dimensional infrared spectroscopy

Abstract

We present what we believe to be the first implementation of nonequilibrium two-dimensional IR spectroscopy (2DIR) combining electronic excitation within the Fourier transform (FT) approach. Nonequilibrium 2DIR spectra of Mn2(CO)10 and its photoproducts are obtained in two modalities: photoexcitation at 400 nm, either before a 2DIR probe or during the waiting time of the FT 2DIR measurement. Extending FT 2DIR to nonequilibrium systems offers insight into complex condensed-phase reaction dynamics.