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Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy

Theoretical and experimental methodologies that can characterize electronic and nuclear dynamics, and the coupling between the two, are needed to understand photoinduced charge transfer in molecular building blocks used in organic photovoltaics. Ongoing developments in ultrafast pump-probe technique...

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Autores principales: Khalili, Khadijeh, Inhester, Ludger, Arnold, Caroline, Welsch, Ralph, Andreasen, Jens Wenzel, Santra, Robin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Crystallographic Association 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6656576/
https://www.ncbi.nlm.nih.gov/pubmed/31372369
http://dx.doi.org/10.1063/1.5097653
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author Khalili, Khadijeh
Inhester, Ludger
Arnold, Caroline
Welsch, Ralph
Andreasen, Jens Wenzel
Santra, Robin
author_facet Khalili, Khadijeh
Inhester, Ludger
Arnold, Caroline
Welsch, Ralph
Andreasen, Jens Wenzel
Santra, Robin
author_sort Khalili, Khadijeh
collection PubMed
description Theoretical and experimental methodologies that can characterize electronic and nuclear dynamics, and the coupling between the two, are needed to understand photoinduced charge transfer in molecular building blocks used in organic photovoltaics. Ongoing developments in ultrafast pump-probe techniques such as time-resolved X-ray absorption spectroscopy, using an X-ray free electron laser in combination with an ultraviolet femtosecond laser, present desirable probes of coupled electronic and nuclear dynamics. In this work, we investigate the charge transfer dynamics of a donor-acceptor pair, which is widely used as a building block in low bandgap block copolymers for organic photovoltaics. We simulate the dynamics of the benzothiadiazole-thiophene molecule upon photoionization with a vacuum ultraviolet (VUV) pulse and study the potential of probing the subsequent charge dynamics using time-resolved X-ray absorption spectroscopy. The photoinduced dynamics are calculated using on-the-fly nonadiabatic molecular dynamics simulations based on Tully's Fewest Switches Surface Hopping approach. We calculate the X-ray absorption spectrum as a function of time after ionization at the Hartree-Fock level. The changes in the time-resolved X-ray absorption spectrum at the sulfur K-edge reveal the ultrafast charge carrier dynamics in the molecule occurring on a femtosecond time scale. These theoretical findings anticipate that ultrafast time-resolved X-ray absorption spectroscopy using an X-ray probe in combination with a VUV pump offers a new approach to investigate the detailed dynamics of organic photovoltaic materials.
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spelling pubmed-66565762019-08-01 Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy Khalili, Khadijeh Inhester, Ludger Arnold, Caroline Welsch, Ralph Andreasen, Jens Wenzel Santra, Robin Struct Dyn ARTICLES Theoretical and experimental methodologies that can characterize electronic and nuclear dynamics, and the coupling between the two, are needed to understand photoinduced charge transfer in molecular building blocks used in organic photovoltaics. Ongoing developments in ultrafast pump-probe techniques such as time-resolved X-ray absorption spectroscopy, using an X-ray free electron laser in combination with an ultraviolet femtosecond laser, present desirable probes of coupled electronic and nuclear dynamics. In this work, we investigate the charge transfer dynamics of a donor-acceptor pair, which is widely used as a building block in low bandgap block copolymers for organic photovoltaics. We simulate the dynamics of the benzothiadiazole-thiophene molecule upon photoionization with a vacuum ultraviolet (VUV) pulse and study the potential of probing the subsequent charge dynamics using time-resolved X-ray absorption spectroscopy. The photoinduced dynamics are calculated using on-the-fly nonadiabatic molecular dynamics simulations based on Tully's Fewest Switches Surface Hopping approach. We calculate the X-ray absorption spectrum as a function of time after ionization at the Hartree-Fock level. The changes in the time-resolved X-ray absorption spectrum at the sulfur K-edge reveal the ultrafast charge carrier dynamics in the molecule occurring on a femtosecond time scale. These theoretical findings anticipate that ultrafast time-resolved X-ray absorption spectroscopy using an X-ray probe in combination with a VUV pump offers a new approach to investigate the detailed dynamics of organic photovoltaic materials. American Crystallographic Association 2019-07-23 /pmc/articles/PMC6656576/ /pubmed/31372369 http://dx.doi.org/10.1063/1.5097653 Text en © 2019 Author(s). 2329-7778/2019/6(4)/044102/8 All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle ARTICLES
Khalili, Khadijeh
Inhester, Ludger
Arnold, Caroline
Welsch, Ralph
Andreasen, Jens Wenzel
Santra, Robin
Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title_full Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title_fullStr Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title_full_unstemmed Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title_short Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy
title_sort hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved x-ray absorption spectroscopy
topic ARTICLES
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6656576/
https://www.ncbi.nlm.nih.gov/pubmed/31372369
http://dx.doi.org/10.1063/1.5097653
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