Real-time mapping of electronic structure with single-shot two-dimensional electronic spectroscopy.

ABSTRACT: Electronic structure and dynamics determine material properties and behavior. Important time scales for electronic dynamics range from attoseconds to milliseconds. Two-dimensional optical spectroscopy has proven an incisive tool to probe fast spatiotemporal electronic dynamics in complex multichromophoric systems. However, acquiring these spectra requires long point-by-point acquisitions that preclude observations on the millisecond and microsecond time scales. Here we demonstrate that imaging temporally encoded information within a homogeneous sample allows mapping of the evolution of the electronic Hamiltonian with femtosecond temporal resolution in a single-laser-shot, providing real-time maps of electronic coupling. This method, which we call GRadient-Assisted Photon Echo spectroscopy

SUBMITTER: Harel E 

PROVIDER: S-EPMC2944741 | biostudies-literature | 2010 Sep

REPOSITORIES: biostudies-literature