Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

作者：Turner Daniel B; Howey Dylan J; Sutor Erika J; Hendrickson Rebecca A; Gealy M W; Ulness Darin J^*

来源：Journal of Physical Chemistry A, 2013, 117(29): 5926-5954.

DOI：10.1021/jp310477y

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.

• 出版日期2013-7-25