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Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems
In this paper we present a theoretical-computational methodology specifically aimed at describing processes involving internal conversion or intersystem crossing, from atomistic (semiclassical) simulations and, hence, very suitable for treating complex atomic-molecular systems. The core of the prese...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2018
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9083445/ https://www.ncbi.nlm.nih.gov/pubmed/35542751 http://dx.doi.org/10.1039/c8ra03900c |
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author | Amadei, Andrea Aschi, Massimiliano |
author_facet | Amadei, Andrea Aschi, Massimiliano |
author_sort | Amadei, Andrea |
collection | PubMed |
description | In this paper we present a theoretical-computational methodology specifically aimed at describing processes involving internal conversion or intersystem crossing, from atomistic (semiclassical) simulations and, hence, very suitable for treating complex atomic-molecular systems. The core of the presented approach is the evaluation of the diabatic perturbed energy surfaces of a portion of the whole system, treated at the quantum level and therefore preventively selected, in semi-classical interaction with the atomic-molecular environment. Subsequently, the estimation of the coupling between the diabatic surfaces and the inclusion of the obtained observables within a properly designed kinetic model allows the reconstruction of the whole phenomenology directly comparable to the experimental (typically kinetic) data. Application to two systems has demonstrated that the proposed approach can represent a valuable tool, somewhat complementary to other methods based on explicit quantum-dynamical approaches, for the theoretical-computational investigations of large and complex atomic-molecular systems. |
format | Online Article Text |
id | pubmed-9083445 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-90834452022-05-09 Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems Amadei, Andrea Aschi, Massimiliano RSC Adv Chemistry In this paper we present a theoretical-computational methodology specifically aimed at describing processes involving internal conversion or intersystem crossing, from atomistic (semiclassical) simulations and, hence, very suitable for treating complex atomic-molecular systems. The core of the presented approach is the evaluation of the diabatic perturbed energy surfaces of a portion of the whole system, treated at the quantum level and therefore preventively selected, in semi-classical interaction with the atomic-molecular environment. Subsequently, the estimation of the coupling between the diabatic surfaces and the inclusion of the obtained observables within a properly designed kinetic model allows the reconstruction of the whole phenomenology directly comparable to the experimental (typically kinetic) data. Application to two systems has demonstrated that the proposed approach can represent a valuable tool, somewhat complementary to other methods based on explicit quantum-dynamical approaches, for the theoretical-computational investigations of large and complex atomic-molecular systems. The Royal Society of Chemistry 2018-08-06 /pmc/articles/PMC9083445/ /pubmed/35542751 http://dx.doi.org/10.1039/c8ra03900c Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Amadei, Andrea Aschi, Massimiliano Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title | Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title_full | Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title_fullStr | Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title_full_unstemmed | Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title_short | Theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
title_sort | theoretical-computational modeling of charge transfer and intersystem crossing reactions in complex chemical systems |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9083445/ https://www.ncbi.nlm.nih.gov/pubmed/35542751 http://dx.doi.org/10.1039/c8ra03900c |
work_keys_str_mv | AT amadeiandrea theoreticalcomputationalmodelingofchargetransferandintersystemcrossingreactionsincomplexchemicalsystems AT aschimassimiliano theoreticalcomputationalmodelingofchargetransferandintersystemcrossingreactionsincomplexchemicalsystems |