Quantum coherence selective 2D Raman-2D electronic spectroscopy.

ABSTRACT: 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 which simultaneously encodes vibrational-vibrational, electronic-vibrational and electronic-electronic interactions. By combining near-impulsive resonant and non-resonant excitation, the desired fifth-order signal of a complex organic molecule in solution is measured free of unwanted lower-order contamination. A critical feature of this method is electronic and vibrational frequency resolution,

SUBMITTER: Spencer AP 

PROVIDER: S-EPMC5353627 | biostudies-literature | 2017 Mar

REPOSITORIES: biostudies-literature