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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...

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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
Descripción
Sumario: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.