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Double-quantum resonances and exciton-scattering in coherent 2D spectroscopy of photosynthetic complexes.

ABSTRACT: A simulation study demonstrates how the nonlinear optical response of the Fenna-Matthews-Olson photosynthetic light-harvesting complex may be explored by a sequence of laser pulses specifically designed to probe the correlated dynamics of double excitations. Cross peaks in the 2D correlation plots of the spectra reveal projections of the double-exciton wavefunctions onto a basis of direct products of single excitons. An alternative physical interpretation of these signals in terms of quasiparticle scattering is developed.

SUBMITTER: Abramavicius D

PROVIDER: S-EPMC2438408 | biostudies-literature | 2008 Jun

REPOSITORIES: biostudies-literature

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Double-quantum resonances and exciton-scattering in coherent 2D spectroscopy of photosynthetic complexes.

Abramavicius Darius D Voronine Dmitri V DV Mukamel Shaul S

Proceedings of the National Academy of Sciences of the United States of America 20080618 25

A simulation study demonstrates how the nonlinear optical response of the Fenna-Matthews-Olson photosynthetic light-harvesting complex may be explored by a sequence of laser pulses specifically designed to probe the correlated dynamics of double excitations. Cross peaks in the 2D correlation plots of the spectra reveal projections of the double-exciton wavefunctions onto a basis of direct products of single excitons. An alternative physical interpretation of these signals in terms of quasipartic ...[more]

PMID: 18562293

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