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...
Ultrafast, multi-dimensional coherent spectroscopy (MD-CS) has enabled scientists to probe fundamental aspects of chemical and photo-physical reactions on the nanosecond to femtosecond timescales. Using MD-CS, scientific contributions ranging from increased understanding of energy transfer in photosynthetic biological proteins to correlating the motion of electrons in semiconductors have been achieved. Concurrent...