Cargando…

Interference of nuclear wavepackets in a pair of proton transfer reactions

Quantum mechanics revolutionized chemists’ understanding of molecular structure. In contrast, the kinetics of molecular reactions in solution are well described by classical, statistical theories. To reveal how the dynamics of chemical systems transition from quantum to classical, we study femtoseco...

Descripción completa

Detalles Bibliográficos
Autores principales: Zhang, Xinzi, Schwarz, Kyra N., Zhang, Luhao, Fassioli, Francesca, Fu, Bo, Nguyen, Lucas Q., Knowles, Robert R., Scholes, Gregory D.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9618146/
https://www.ncbi.nlm.nih.gov/pubmed/36252025
http://dx.doi.org/10.1073/pnas.2212114119
_version_ 1784820989806247936
author Zhang, Xinzi
Schwarz, Kyra N.
Zhang, Luhao
Fassioli, Francesca
Fu, Bo
Nguyen, Lucas Q.
Knowles, Robert R.
Scholes, Gregory D.
author_facet Zhang, Xinzi
Schwarz, Kyra N.
Zhang, Luhao
Fassioli, Francesca
Fu, Bo
Nguyen, Lucas Q.
Knowles, Robert R.
Scholes, Gregory D.
author_sort Zhang, Xinzi
collection PubMed
description Quantum mechanics revolutionized chemists’ understanding of molecular structure. In contrast, the kinetics of molecular reactions in solution are well described by classical, statistical theories. To reveal how the dynamics of chemical systems transition from quantum to classical, we study femtosecond proton transfer in a symmetric molecule with two identical reactant sites that are spatially apart. With the reaction launched from a superposition of two local basis states, we hypothesize that the ensuing motions of the electrons and nuclei will proceed, conceptually, in lockstep as a superposition of probability amplitudes until decoherence collapses the system to a product. Using ultrafast spectroscopy, we observe that the initial superposition state affects the reaction kinetics by an interference mechanism. With the aid of a quantum dynamics model, we propose how the evolution of nuclear wavepackets manifests the unusual intersite quantum correlations during the reaction.
format Online
Article
Text
id pubmed-9618146
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher National Academy of Sciences
record_format MEDLINE/PubMed
spelling pubmed-96181462023-04-17 Interference of nuclear wavepackets in a pair of proton transfer reactions Zhang, Xinzi Schwarz, Kyra N. Zhang, Luhao Fassioli, Francesca Fu, Bo Nguyen, Lucas Q. Knowles, Robert R. Scholes, Gregory D. Proc Natl Acad Sci U S A Physical Sciences Quantum mechanics revolutionized chemists’ understanding of molecular structure. In contrast, the kinetics of molecular reactions in solution are well described by classical, statistical theories. To reveal how the dynamics of chemical systems transition from quantum to classical, we study femtosecond proton transfer in a symmetric molecule with two identical reactant sites that are spatially apart. With the reaction launched from a superposition of two local basis states, we hypothesize that the ensuing motions of the electrons and nuclei will proceed, conceptually, in lockstep as a superposition of probability amplitudes until decoherence collapses the system to a product. Using ultrafast spectroscopy, we observe that the initial superposition state affects the reaction kinetics by an interference mechanism. With the aid of a quantum dynamics model, we propose how the evolution of nuclear wavepackets manifests the unusual intersite quantum correlations during the reaction. National Academy of Sciences 2022-10-17 2022-10-25 /pmc/articles/PMC9618146/ /pubmed/36252025 http://dx.doi.org/10.1073/pnas.2212114119 Text en Copyright © 2022 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) .
spellingShingle Physical Sciences
Zhang, Xinzi
Schwarz, Kyra N.
Zhang, Luhao
Fassioli, Francesca
Fu, Bo
Nguyen, Lucas Q.
Knowles, Robert R.
Scholes, Gregory D.
Interference of nuclear wavepackets in a pair of proton transfer reactions
title Interference of nuclear wavepackets in a pair of proton transfer reactions
title_full Interference of nuclear wavepackets in a pair of proton transfer reactions
title_fullStr Interference of nuclear wavepackets in a pair of proton transfer reactions
title_full_unstemmed Interference of nuclear wavepackets in a pair of proton transfer reactions
title_short Interference of nuclear wavepackets in a pair of proton transfer reactions
title_sort interference of nuclear wavepackets in a pair of proton transfer reactions
topic Physical Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9618146/
https://www.ncbi.nlm.nih.gov/pubmed/36252025
http://dx.doi.org/10.1073/pnas.2212114119
work_keys_str_mv AT zhangxinzi interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT schwarzkyran interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT zhangluhao interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT fassiolifrancesca interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT fubo interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT nguyenlucasq interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT knowlesrobertr interferenceofnuclearwavepacketsinapairofprotontransferreactions
AT scholesgregoryd interferenceofnuclearwavepacketsinapairofprotontransferreactions