title: Two-dimensional electronic spectroscopy using incoherent light: theoretical analysis.
abstract: Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations in two-dimensional electronic spectroscopy measurements of pigment-protein complexes measured with femtosecond laser pulses. A persistent issue in the field is to reconcile the results of measurements performed using femtosecond laser pulses with physiological illumination conditions. Noisy-light spectroscopy can begin to address this question. In this work we present the theoretical analysis of incoherent two-dimensional electronic spectroscopy, I((4)) 2D ES. Simulations reveal diagonal peaks, cross peaks, and coherent oscillations similar to those observed in femtosecond two-dimensional electronic spectroscopy experiments. The results also expose fundamental differences between the femtosecond-pulse and noisy-light techniques; the differences lead to new challenges and new opportunities.
authors.affiliation: Department of Chemistry, Institute for Optical Sciences, and Centre for Quantum Information and Quantum Control, University of Toronto, 80 Saint George Street, Toronto, Ontario M5S 3H6, Canada.
authors.forename: Daniel B
authors.initials: DB
authors.lastname: Turner
authors.forename: Dylan J
authors.initials: DJ
authors.lastname: Howey
authors.forename: Erika J
authors.initials: EJ
authors.lastname: Sutor
authors.forename: Rebecca A
authors.initials: RA
authors.lastname: Hendrickson
authors.forename: M W
authors.initials: MW
authors.lastname: Gealy
authors.forename: Darin J
authors.initials: DJ
authors.lastname: Ulness
mesh_terms: D003116:Color; D004579:Electron Transport; D004583:Electrons; D008027:Light; D008958:Models, Molecular; D008968:Molecular Conformation; D010788:Photosynthesis; D013057:Spectrum Analysis; D013997:Time Factors