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Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics

[Image: see text] This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu–Brumer approach, which treats the thermal radiation as...

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Autor principal: Barbatti, Mario
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7426902/
https://www.ncbi.nlm.nih.gov/pubmed/32579345
http://dx.doi.org/10.1021/acs.jctc.0c00501
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author Barbatti, Mario
author_facet Barbatti, Mario
author_sort Barbatti, Mario
collection PubMed
description [Image: see text] This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu–Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps: (1) sampling initial conditions from a broad blackbody spectrum, (2) dynamics propagation using conventional methods, and (3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensembles (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a steady excited-state population. In another test case, modeling retinal photophysics, MQC-PE predicted that although the photoisomerization occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to photoactivate a single retinal. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation.
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spelling pubmed-74269022020-08-14 Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics Barbatti, Mario J Chem Theory Comput [Image: see text] This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu–Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps: (1) sampling initial conditions from a broad blackbody spectrum, (2) dynamics propagation using conventional methods, and (3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensembles (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a steady excited-state population. In another test case, modeling retinal photophysics, MQC-PE predicted that although the photoisomerization occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to photoactivate a single retinal. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation. American Chemical Society 2020-06-24 2020-08-11 /pmc/articles/PMC7426902/ /pubmed/32579345 http://dx.doi.org/10.1021/acs.jctc.0c00501 Text en Copyright © 2020 American Chemical Society This is an open access article published under an ACS AuthorChoice License (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes.
spellingShingle Barbatti, Mario
Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title_full Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title_fullStr Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title_full_unstemmed Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title_short Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics
title_sort simulation of excitation by sunlight in mixed quantum-classical dynamics
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7426902/
https://www.ncbi.nlm.nih.gov/pubmed/32579345
http://dx.doi.org/10.1021/acs.jctc.0c00501
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