Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis
Autor: | Rebecca A. Hendrickson, Darin J. Ulness, Daniel B. Turner, Erika J. Sutor, Dylan J. Howey, M. W. Gealy |
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Rok vydání: | 2012 |
Předmět: |
Models
Molecular Work (thermodynamics) Time Factors Light Molecular Conformation Color FOS: Physical sciences Electrons Electronic energy transfer 02 engineering and technology 01 natural sciences Electron spectroscopy Molecular physics Electron Transport Physics - Chemical Physics 0103 physical sciences Photosynthesis Physical and Theoretical Chemistry 010306 general physics Coupling Chemical Physics (physics.chem-ph) Quantitative Biology::Biomolecules Physics::Biological Physics Range (particle radiation) Chemistry Spectrum Analysis Intermolecular force 021001 nanoscience & nanotechnology 3. Good health 0210 nano-technology |
DOI: | 10.48550/arxiv.1210.6665 |
Popis: | 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. Comment: 30 pages, 24 figures, comments from readers encouraged! |
Databáze: | OpenAIRE |
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