Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

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...

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Bibliographic Details
Published in:The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2013-07, Vol.117 (29), p.5926-5954
Main Authors: Turner, Daniel B, Howey, Dylan J, Sutor, Erika J, Hendrickson, Rebecca A, Gealy, M. W, Ulness, Darin J
Format: Article
Language:English
Subjects:
Biological and medical sciences
Coherence
Color
Coupling (molecular)
Electron Transport
Electrons
Energy transfer
Femtosecond
Fundamental and applied biological sciences. Psychology
Lasers
Light
Models, Molecular
Molecular biophysics
Molecular Conformation
Oscillations
Photochemistry. Photosynthesis. Bioluminescence
Photosynthesis
Radiation-biomolecule interaction
Spectroscopy
Spectrum Analysis
Time Factors
Two dimensional
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Summary: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.
ISSN:1089-5639
1520-5215
DOI:10.1021/jp310477y