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Proc Natl Acad Sci U S A. 2008 Jun 24;105(25):8525-30. doi: 10.1073/pnas.0802926105. Epub 2008 Jun 18.

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

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  • 1Department of Chemistry, 1102 Natural Sciences 2, University of California, Irvine, CA 92697-2025, USA.

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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