Electronic and vibrational correlations report on the dynamics and structure of molecular species, yet revealing these correlations experimentally has proved extremely challenging. Here, we demonstrate a method that probes correlations between states within the vibrational and electronic manifold with quantum coherence selectivity. Specifically, we measure a fully coherent four-dimensional spectrum...
Compressive sensing allows signals to be efficiently captured by exploiting their inherent sparsity. Here we implement sparse sampling to capture the electronic structure and ultrafast dynamics of molecular systems using phase-resolved 2D coherent spectroscopy. Until now, 2D spectroscopy has been hampered by its reliance on array detectors that operate in...