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.
Abramavicius
Darius
D
Department of Chemistry, 1102 Natural Sciences 2, University of California, Irvine, CA 92697-2025, USA.
Voronine
Dmitri V
DV
Mukamel
Shaul
S
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