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Two-dimensional electronic spectroscopy using incoherent light: Theoretical analysis

机译:使用非相干光的二维电子光谱:理论分析

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摘要

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.
机译:光合作用中的电子能量转移发生在一定的时间范围内,并在各种分子间耦合条件下发生。最近的工作表明,在用飞秒激光脉冲测量的色素-蛋白质复合物的二维电子光谱测量中,生色团之间的电子耦合会导致相干振荡。该领域中的一个长期问题是使使用飞秒激光脉冲与生理照明条件进行的测量结果相一致。噪声光光谱学可以开始解决这个问题。在这项工作中,我们提出了非相干二维电子光谱I〜((4))2D ES的理论分析。仿真显示对角峰,交叉峰和相干振荡类似于在飞秒二维电子光谱实验中观察到的。结果还揭示了飞秒脉冲技术与噪声光技术之间的根本差异;差异导致新的挑战和新的机遇。

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