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Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction
Many chemical reactions of transition metal compounds involve a change in spin state via spin inversion, which is induced by relativistic spin-orbit coupling. In this work, we theoretically study the efficiency of a typical spin-inversion reaction, (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4). Structural...
Autores principales: | , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
MDPI
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7070764/ https://www.ncbi.nlm.nih.gov/pubmed/32079272 http://dx.doi.org/10.3390/molecules25040882 |
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author | Takayanagi, Toshiyuki Watabe, Yuya Miyazaki, Takaaki |
author_facet | Takayanagi, Toshiyuki Watabe, Yuya Miyazaki, Takaaki |
author_sort | Takayanagi, Toshiyuki |
collection | PubMed |
description | Many chemical reactions of transition metal compounds involve a change in spin state via spin inversion, which is induced by relativistic spin-orbit coupling. In this work, we theoretically study the efficiency of a typical spin-inversion reaction, (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4). Structural and vibrational information on the spin-inversion point, obtained through the spin-coupled Hamiltonian approach, is used to construct three degree-of-freedom potential energy surfaces and to obtain singlet-triplet spin-orbit couplings. Using the developed spin-diabatic potential energy surfaces in reduced dimensions, we perform quantum nonadiabatic transition state wave packet calculations to obtain the cumulative reaction probability. The calculated cumulative reaction probability is found to be significantly larger than that estimated from the one-dimensional surface-hopping probability. This indicates the importance of both multidimensional and nuclear quantum effects in spin inversion for polyatomic chemical reaction systems. |
format | Online Article Text |
id | pubmed-7070764 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | MDPI |
record_format | MEDLINE/PubMed |
spelling | pubmed-70707642020-03-19 Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction Takayanagi, Toshiyuki Watabe, Yuya Miyazaki, Takaaki Molecules Article Many chemical reactions of transition metal compounds involve a change in spin state via spin inversion, which is induced by relativistic spin-orbit coupling. In this work, we theoretically study the efficiency of a typical spin-inversion reaction, (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4). Structural and vibrational information on the spin-inversion point, obtained through the spin-coupled Hamiltonian approach, is used to construct three degree-of-freedom potential energy surfaces and to obtain singlet-triplet spin-orbit couplings. Using the developed spin-diabatic potential energy surfaces in reduced dimensions, we perform quantum nonadiabatic transition state wave packet calculations to obtain the cumulative reaction probability. The calculated cumulative reaction probability is found to be significantly larger than that estimated from the one-dimensional surface-hopping probability. This indicates the importance of both multidimensional and nuclear quantum effects in spin inversion for polyatomic chemical reaction systems. MDPI 2020-02-17 /pmc/articles/PMC7070764/ /pubmed/32079272 http://dx.doi.org/10.3390/molecules25040882 Text en © 2020 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Article Takayanagi, Toshiyuki Watabe, Yuya Miyazaki, Takaaki Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title | Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title_full | Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title_fullStr | Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title_full_unstemmed | Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title_short | Reduced-Dimensionality Quantum Dynamics Study of the (3)Fe(CO)(4) + H(2) → (1)FeH(2)(CO)(4) Spin-inversion Reaction |
title_sort | reduced-dimensionality quantum dynamics study of the (3)fe(co)(4) + h(2) → (1)feh(2)(co)(4) spin-inversion reaction |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7070764/ https://www.ncbi.nlm.nih.gov/pubmed/32079272 http://dx.doi.org/10.3390/molecules25040882 |
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