Double-quantum resonances and exciton-scattering in coherent 2D spectroscopy of photosynthetic complexes.
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.
Department of Chemistry, 1102 Natural Sciences 2, University of California, Irvine, CA 92697-2025, USA.
Darius
D
Abramavicius
Dmitri V
DV
Voronine
Shaul
S
Mukamel
D004735:Energy Transfer; D005583:Fourier Analysis; D008958:Models, Molecular; D045322:Photosynthetic Reaction Center Complex Proteins / Q000737:chemistry*; D011789:Quantum Theory; D013057:Spectrum Analysis / Q000379:methods*; D013816:Thermodynamics
D045322:Photosynthetic Reaction Center Complex Proteins