Real-time Simulations of Photoinduced Coherent Charge Transfer and Proton-Coupled Electron Transfer

Photoinduced electron transfer (ET) and proton‐coupled electron transfer (PCET) are fundamental processes in natural phenomena, most noticeably in photosynthesis. Time‐resolved spectroscopic evidence of coherent oscillatory behavior associated with these processes has been reported both in complex b...

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Veröffentlicht in:Chemphyschem 2014-10, Vol.15 (15), p.3258-3263
Hauptverfasser: Eisenmayer, Thomas J., Buda, Francesco
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Buda, Francesco
description Photoinduced electron transfer (ET) and proton‐coupled electron transfer (PCET) are fundamental processes in natural phenomena, most noticeably in photosynthesis. Time‐resolved spectroscopic evidence of coherent oscillatory behavior associated with these processes has been reported both in complex biological environments, as well as in biomimetic models for artificial photosynthesis. Here, we consider a few biomimetic models to investigate these processes in real‐time simulations based on ab initio molecular dynamics and Ehrenfest dynamics. This allows for a detailed analysis on how photon‐to‐charge conversion is promoted by a coupling of the electronic excitation with specific vibrational modes and with proton displacements. The ET process shows a characteristic coherence that is linked to the nuclear motion at the interface between donor and acceptor. We also show real‐time evidence of PCET in a benzimidazole–phenol redox relay. A dynamic approach: Photoinduced electron transfer is shown to be coherently coupled to specific vibrational modes by using attosecond dynamics. The proton‐coupled electron transfer in an artificial redox mediator is simulated in real time.
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subjects Benzimidazoles - chemistry
Chemistry
coherence
Ehrenfest dynamics
Electron transfer
Electron Transport
Electrons
Exact sciences and technology
General and physical chemistry
Light
molecular dynamics
Molecular Dynamics Simulation
Oxidation-Reduction
Phenol - chemistry
Photochemistry
Physical chemistry of induced reactions (with radiations, particles and ultrasonics)
proton-coupled electron transfer
Protons
Quantum Theory
Triazines - chemistry
title Real-time Simulations of Photoinduced Coherent Charge Transfer and Proton-Coupled Electron Transfer
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