Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis
| Autor: | Turner, Daniel B., Howey, Dylan J., Sutor, Erika J., Hendrickson, Rebecca A., Gealy, M. W., Ulness, Darin J. |
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| Rok vydání: | 2012 |
| Předmět: | |
| Druh dokumentu: | Working Paper |
| DOI: | 10.1021/jp310477y |
| 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: | arXiv |
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