Spatial Spectral Interferometry and Compressive Sensing Detection in Single-Shot 2DFT Spectroscopy

Abstract

Multidimensional spectroscopies have the power to uncover coupling in complex systems of electronic and vibrational transitions. In particular, two-dimensional Fourier-transform (2DFT) spectra contain the frequency correlation of dipole oscillations between two time intervals (τ and t) separated by a waiting time (T) with molecule-limited frequency and time resolution. Peak amplitudes and beatings in the spectrum expose population kinetics and coherent coupling between states. Of particular interest are off-diagonal cross peaks, which mark coupled transitions, yielding valuable molecular information including vibronic coupling and energy transfer dynamics.