Daniel B. Turner | Searcharxiv

arXiv2013

Two-dimensional electronic spectroscopy for the quantum-optics enthusiast

Recent interest in the role of quantum mechanics in the primary events of photosynthetic energy transfer has led to a convergence of nonlinear optical spectroscopy and quantum optics on the topic of energy-transfer dynamics in pigment-protein complexes. The convergence of these two communities has unveiled a mismatch between the background and terminology of the respective fields. To make connections, we provide a pedagogical guide to understanding the basics of two-dimensional electronic spectra aimed at researchers with a background in quantum optics.

quant-ph↗

arXiv2012

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 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.

physics.chem-ph↗