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Experimental Access to Mode-Specific Coupling between Quantum Molecular Vibrations and Classical Bath Modes
[Image: see text] The interaction of quantum-mechanical systems with a fluctuating thermal environment (bath) is fundamental to molecular mechanics and energy transport/dissipation. Its complete picture requires mode-specific measurements of this interaction and an understanding of its nature. Here,...
Autores principales: | , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10544034/ https://www.ncbi.nlm.nih.gov/pubmed/37728562 http://dx.doi.org/10.1021/acs.jpclett.3c01974 |
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author | Seliya, Pankaj Bonn, Mischa Grechko, Maksim |
author_facet | Seliya, Pankaj Bonn, Mischa Grechko, Maksim |
author_sort | Seliya, Pankaj |
collection | PubMed |
description | [Image: see text] The interaction of quantum-mechanical systems with a fluctuating thermal environment (bath) is fundamental to molecular mechanics and energy transport/dissipation. Its complete picture requires mode-specific measurements of this interaction and an understanding of its nature. Here, we present a combined experimental and theoretical study providing detailed insights into the coupling between a high-frequency vibrational two-level system and thermally excited terahertz modes. Experimentally, two-dimensional terahertz-infrared-visible spectroscopy reports directly on the coupling between quantum oscillators represented by CH(3) streching vibrations in liquid dimethyl sulfoxide and distinct low-frequency modes. Theoretically, we present a mixed quantum-classical formalism of the sample response to enable the simultaneous quantum description of high-frequency oscillators and a classical description of the bath. We derive the strength and nature of interaction and find different coupling between CH(3) stretch and low-frequency modes. This general approach enables quantitative and mode-specific analysis of coupled quantum and classical dynamics in complex chemical systems. |
format | Online Article Text |
id | pubmed-10544034 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-105440342023-10-03 Experimental Access to Mode-Specific Coupling between Quantum Molecular Vibrations and Classical Bath Modes Seliya, Pankaj Bonn, Mischa Grechko, Maksim J Phys Chem Lett [Image: see text] The interaction of quantum-mechanical systems with a fluctuating thermal environment (bath) is fundamental to molecular mechanics and energy transport/dissipation. Its complete picture requires mode-specific measurements of this interaction and an understanding of its nature. Here, we present a combined experimental and theoretical study providing detailed insights into the coupling between a high-frequency vibrational two-level system and thermally excited terahertz modes. Experimentally, two-dimensional terahertz-infrared-visible spectroscopy reports directly on the coupling between quantum oscillators represented by CH(3) streching vibrations in liquid dimethyl sulfoxide and distinct low-frequency modes. Theoretically, we present a mixed quantum-classical formalism of the sample response to enable the simultaneous quantum description of high-frequency oscillators and a classical description of the bath. We derive the strength and nature of interaction and find different coupling between CH(3) stretch and low-frequency modes. This general approach enables quantitative and mode-specific analysis of coupled quantum and classical dynamics in complex chemical systems. American Chemical Society 2023-09-20 /pmc/articles/PMC10544034/ /pubmed/37728562 http://dx.doi.org/10.1021/acs.jpclett.3c01974 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Seliya, Pankaj Bonn, Mischa Grechko, Maksim Experimental Access to Mode-Specific Coupling between Quantum Molecular Vibrations and Classical Bath Modes |
title | Experimental
Access to Mode-Specific Coupling between
Quantum Molecular Vibrations and Classical Bath Modes |
title_full | Experimental
Access to Mode-Specific Coupling between
Quantum Molecular Vibrations and Classical Bath Modes |
title_fullStr | Experimental
Access to Mode-Specific Coupling between
Quantum Molecular Vibrations and Classical Bath Modes |
title_full_unstemmed | Experimental
Access to Mode-Specific Coupling between
Quantum Molecular Vibrations and Classical Bath Modes |
title_short | Experimental
Access to Mode-Specific Coupling between
Quantum Molecular Vibrations and Classical Bath Modes |
title_sort | experimental
access to mode-specific coupling between
quantum molecular vibrations and classical bath modes |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10544034/ https://www.ncbi.nlm.nih.gov/pubmed/37728562 http://dx.doi.org/10.1021/acs.jpclett.3c01974 |
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