Cargando…

On the physical mechanisms underlying single molecule dynamics in simple liquids

Physical arguments and comparisons with published experimental data suggest that in simple liquids: (i) single-molecule-scale viscous forces are produced by temperature-dependent London dispersion forces, (ii) viscosity decay with increasing temperature reflects electron cloud compression and attend...

Descripción completa

Detalles Bibliográficos
Autores principales: Keanini, Russell G., Dahlberg, Jerry, Tkacik, Peter T.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7843658/
https://www.ncbi.nlm.nih.gov/pubmed/33510369
http://dx.doi.org/10.1038/s41598-021-82112-8
_version_ 1783644196906729472
author Keanini, Russell G.
Dahlberg, Jerry
Tkacik, Peter T.
author_facet Keanini, Russell G.
Dahlberg, Jerry
Tkacik, Peter T.
author_sort Keanini, Russell G.
collection PubMed
description Physical arguments and comparisons with published experimental data suggest that in simple liquids: (i) single-molecule-scale viscous forces are produced by temperature-dependent London dispersion forces, (ii) viscosity decay with increasing temperature reflects electron cloud compression and attendant suppression of electron screening, produced by increased nuclear agitation, and (iii) temperature-dependent self-diffusion is driven by a narrow band of phonon frequencies lying at the low-frequency end of the solid-state-like phonon spectrum. The results suggest that collision-induced electron cloud distortion plays a decisive role in single molecule dynamics: (i) electron cloud compression produces short-lived repulsive states and single molecule, self-diffusive hops, while (ii) shear-induced distortion generates viscosity and single-molecule-scale viscous drag. The results provide new insight into nonequilibrium molecular dynamics in nonpolar, nonmetallic liquids.
format Online
Article
Text
id pubmed-7843658
institution National Center for Biotechnology Information
language English
publishDate 2021
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-78436582021-01-29 On the physical mechanisms underlying single molecule dynamics in simple liquids Keanini, Russell G. Dahlberg, Jerry Tkacik, Peter T. Sci Rep Article Physical arguments and comparisons with published experimental data suggest that in simple liquids: (i) single-molecule-scale viscous forces are produced by temperature-dependent London dispersion forces, (ii) viscosity decay with increasing temperature reflects electron cloud compression and attendant suppression of electron screening, produced by increased nuclear agitation, and (iii) temperature-dependent self-diffusion is driven by a narrow band of phonon frequencies lying at the low-frequency end of the solid-state-like phonon spectrum. The results suggest that collision-induced electron cloud distortion plays a decisive role in single molecule dynamics: (i) electron cloud compression produces short-lived repulsive states and single molecule, self-diffusive hops, while (ii) shear-induced distortion generates viscosity and single-molecule-scale viscous drag. The results provide new insight into nonequilibrium molecular dynamics in nonpolar, nonmetallic liquids. Nature Publishing Group UK 2021-01-28 /pmc/articles/PMC7843658/ /pubmed/33510369 http://dx.doi.org/10.1038/s41598-021-82112-8 Text en © The Author(s) 2021 Open AccessThis article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Keanini, Russell G.
Dahlberg, Jerry
Tkacik, Peter T.
On the physical mechanisms underlying single molecule dynamics in simple liquids
title On the physical mechanisms underlying single molecule dynamics in simple liquids
title_full On the physical mechanisms underlying single molecule dynamics in simple liquids
title_fullStr On the physical mechanisms underlying single molecule dynamics in simple liquids
title_full_unstemmed On the physical mechanisms underlying single molecule dynamics in simple liquids
title_short On the physical mechanisms underlying single molecule dynamics in simple liquids
title_sort on the physical mechanisms underlying single molecule dynamics in simple liquids
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7843658/
https://www.ncbi.nlm.nih.gov/pubmed/33510369
http://dx.doi.org/10.1038/s41598-021-82112-8
work_keys_str_mv AT keaninirussellg onthephysicalmechanismsunderlyingsinglemoleculedynamicsinsimpleliquids
AT dahlbergjerry onthephysicalmechanismsunderlyingsinglemoleculedynamicsinsimpleliquids
AT tkacikpetert onthephysicalmechanismsunderlyingsinglemoleculedynamicsinsimpleliquids