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Driving force and nonequilibrium vibronic dynamics in charge separation of strongly bound electron–hole pairs

Somoza, Alejandro D. and Lorenzoni, Nicola and Lim, James and Huelga, Susana F. and Plenio, Martin B. (2023) Driving force and nonequilibrium vibronic dynamics in charge separation of strongly bound electron–hole pairs. Communications Physics, 6 (65). Springer Nature. doi: 10.1038/s42005-023-01179-z. ISSN 2399-3650.

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Abstract

Electron-hole pairs in organic photovoltaics efficiently dissociate although their Coulomb-binding energy exceeds thermal energy at room temperature. The vibronic coupling of electronic states to structured vibrational environments containing multiple underdamped modes is thought to assist charge separation. However, non-perturbative simulations of such large, spatially extended, electronic-vibrational (vibronic) systems remain an unmet challenge which current methods bypass by considering effective one-dimensional Coulomb potentials or unstructured environments where the effect of underdamped modes is ignored. Here we address this challenge with a non-perturbative simulation tool and investigate the charge separation dynamics in one, two and three-dimensional donor-acceptor networks to identify under what conditions underdamped vibrational motion induces efficient long-range charge separation. The resulting comprehensive picture of ultrafast charge separation differentiates electronic or vibronic couplings mechanisms for a wide range of driving forces and identifies the role of entropic effects in extended systems. This provides a toolbox for the design of efficient charge separation pathways in artificial nanostructures.

Item URL in elib:https://elib.dlr.de/194703/
Document Type:Article
Title:Driving force and nonequilibrium vibronic dynamics in charge separation of strongly bound electron–hole pairs
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iDORCID Put Code
Somoza, Alejandro D.UNSPECIFIEDhttps://orcid.org/0000-0002-4973-8052UNSPECIFIED
Lorenzoni, NicolaInstitute of Theoretical Physics and IQST, Universität Ulm, Albert-Einstein-Allee 11, D-89069 Ulm, Germanyhttps://orcid.org/0000-0002-1372-1283UNSPECIFIED
Lim, JamesUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Huelga, Susana F.Institute of Theoretical Physics and IQST, Universität Ulm, Albert-Einstein-Allee 11, D-89069 Ulm, Germanyhttps://orcid.org/0000-0003-1277-8154UNSPECIFIED
Plenio, Martin B.UNSPECIFIEDhttps://orcid.org/0000-0003-4238-8843UNSPECIFIED
Date:8 April 2023
Journal or Publication Title:Communications Physics
Refereed publication:Yes
Open Access:Yes
Gold Open Access:Yes
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:6
DOI:10.1038/s42005-023-01179-z
Publisher:Springer Nature
ISSN:2399-3650
Status:Published
Keywords:Quantendynamik, Offene Quantensysteme, Organische Photovoltaik
HGF - Research field:Energy
HGF - Program:Materials and Technologies for the Energy Transition
HGF - Program Themes:Electrochemical Energy Storage
DLR - Research area:Energy
DLR - Program:E VS - Combustion Systems
DLR - Research theme (Project):E - Materials for Electrochemical Energy Storage, E - Materials for Chemical Energy Carriers, E - Solar Fuels
Location: Ulm
Institutes and Institutions:Institute of Engineering Thermodynamics > Computational Electrochemistry
Deposited By: Somoza, Alejandro
Deposited On:27 Apr 2023 16:15
Last Modified:27 Apr 2023 16:15

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