Enhanced-Resolution Single-Shot 2DFT Spectroscopy by Spatial Spectral Interferometry


We demonstrate use of spatial interference for the complete electric field reconstruction of two-dimensional (2D) coherent spectroscopic signals generated through four-wave mixing (4WM) in a single laser shot. Until now, the amplitude and phase characterization of 4WM signals has relied primarily on Fourier transform spectral interferometry (FTSI), which limits the measurement?s sensitivity and resolution. We show that spatial spectral interferometry (SSI) is a generalized approach to 4WM signal detection that eliminates these inherent limitations of FTSI without introducing additional experimental complexity. SSI is used to measure the 2D photon echo spectra of two systems with dramatically different line widths, the coupled D line transitions in rubidium vapor and the energy-transfer dynamics in the light-harvesting protein LH2.

J. Phys. Chem. Lett.