Exact simulation of pigment-protein complexes unveils vibronic renormalization of electronic parameters in ultrafast spectroscopy

F. Caycedo-Soler, A. Mattioni, J. Lim, T. Renger, S. F. Huelga () and M. B. Plenio ()
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F. Caycedo-Soler: Ulm University
A. Mattioni: Ulm University
J. Lim: Ulm University
T. Renger: Department of Theoretical Biophysics, Johannes Kepler University Linz
S. F. Huelga: Ulm University
M. B. Plenio: Ulm University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract The primary steps of photosynthesis rely on the generation, transport, and trapping of excitons in pigment-protein complexes (PPCs). Generically, PPCs possess highly structured vibrational spectra, combining many discrete intra-pigment modes and a quasi-continuous of protein modes, with vibrational and electronic couplings of comparable strength. The intricacy of the resulting vibronic dynamics poses significant challenges in establishing a quantitative connection between spectroscopic data and underlying microscopic models. Here we show how to address this challenge using numerically exact simulation methods by considering two model systems, namely the water-soluble chlorophyll-binding protein of cauliflower and the special pair of bacterial reaction centers. We demonstrate that the inclusion of the full multi-mode vibronic dynamics in numerical calculations of linear spectra leads to systematic and quantitatively significant corrections to electronic parameter estimation. These multi-mode vibronic effects are shown to be relevant in the longstanding discussion regarding the origin of long-lived oscillations in multidimensional nonlinear spectra.

Date: 2022
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DOI: 10.1038/s41467-022-30565-4

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