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Dynamic localization of electronic excitation in photosynthetic complexes revealed with chiral two-dimensional spectroscopy.


ABSTRACT: Time-resolved ultrafast optical probes of chiral dynamics provide a new window allowing us to explore how interactions with such structured environments drive electronic dynamics. Incorporating optical activity into time-resolved spectroscopies has proven challenging because of the small signal and large achiral background. Here we demonstrate that two-dimensional electronic spectroscopy can be adapted to detect chiral signals and that these signals reveal how excitations delocalize and contract following excitation. We dynamically probe the evolution of chiral electronic structure in the light-harvesting complex 2 of purple bacteria following photoexcitation by creating a chiral two-dimensional mapping. The dynamics of the chiral two-dimensional signal directly reports on changes in the d

SUBMITTER: Fidler AF 

PROVIDER: S-EPMC3976994 | biostudies-literature | 2014

REPOSITORIES: biostudies-literature