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

Abramavicius, Darius; Voronine, Dmitri V; Mukamel, Shaul · Proc Natl Acad Sci U S A · 2008

basic_science · Level V

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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.

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