Cargando…

Universal law for the vibrational density of states of liquids

An analytical derivation of the vibrational density of states (DOS) of liquids, and, in particular, of its characteristic linear in frequency low-energy regime, has always been elusive because of the presence of an infinite set of purely imaginary modes—the instantaneous normal modes (INMs). By comb...

Descripción completa

Detalles Bibliográficos
Autores principales: Zaccone, Alessio, Baggioli, Matteo
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7865170/
https://www.ncbi.nlm.nih.gov/pubmed/33495319
http://dx.doi.org/10.1073/pnas.2022303118
_version_ 1783647786470735872
author Zaccone, Alessio
Baggioli, Matteo
author_facet Zaccone, Alessio
Baggioli, Matteo
author_sort Zaccone, Alessio
collection PubMed
description An analytical derivation of the vibrational density of states (DOS) of liquids, and, in particular, of its characteristic linear in frequency low-energy regime, has always been elusive because of the presence of an infinite set of purely imaginary modes—the instantaneous normal modes (INMs). By combining an analytic continuation of the Plemelj identity to the complex plane with the overdamped dynamics of the INMs, we derive a closed-form analytic expression for the low-frequency DOS of liquids. The obtained result explains, from first principles, the widely observed linear in frequency term of the DOS in liquids, whose slope appears to increase with the average lifetime of the INMs. The analytic results are robustly confirmed by fitting simulations data for Lennard-Jones liquids, and they also recover the Arrhenius law for the average relaxation time of the INMs, as expected.
format Online
Article
Text
id pubmed-7865170
institution National Center for Biotechnology Information
language English
publishDate 2021
publisher National Academy of Sciences
record_format MEDLINE/PubMed
spelling pubmed-78651702021-02-17 Universal law for the vibrational density of states of liquids Zaccone, Alessio Baggioli, Matteo Proc Natl Acad Sci U S A Physical Sciences An analytical derivation of the vibrational density of states (DOS) of liquids, and, in particular, of its characteristic linear in frequency low-energy regime, has always been elusive because of the presence of an infinite set of purely imaginary modes—the instantaneous normal modes (INMs). By combining an analytic continuation of the Plemelj identity to the complex plane with the overdamped dynamics of the INMs, we derive a closed-form analytic expression for the low-frequency DOS of liquids. The obtained result explains, from first principles, the widely observed linear in frequency term of the DOS in liquids, whose slope appears to increase with the average lifetime of the INMs. The analytic results are robustly confirmed by fitting simulations data for Lennard-Jones liquids, and they also recover the Arrhenius law for the average relaxation time of the INMs, as expected. National Academy of Sciences 2021-02-02 2021-01-25 /pmc/articles/PMC7865170/ /pubmed/33495319 http://dx.doi.org/10.1073/pnas.2022303118 Text en Copyright © 2021 the Author(s). Published by PNAS. http://creativecommons.org/licenses/by/4.0/ https://creativecommons.org/licenses/by/4.0/This open access article is distributed under Creative Commons Attribution License 4.0 (CC BY) (http://creativecommons.org/licenses/by/4.0/) .
spellingShingle Physical Sciences
Zaccone, Alessio
Baggioli, Matteo
Universal law for the vibrational density of states of liquids
title Universal law for the vibrational density of states of liquids
title_full Universal law for the vibrational density of states of liquids
title_fullStr Universal law for the vibrational density of states of liquids
title_full_unstemmed Universal law for the vibrational density of states of liquids
title_short Universal law for the vibrational density of states of liquids
title_sort universal law for the vibrational density of states of liquids
topic Physical Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7865170/
https://www.ncbi.nlm.nih.gov/pubmed/33495319
http://dx.doi.org/10.1073/pnas.2022303118
work_keys_str_mv AT zacconealessio universallawforthevibrationaldensityofstatesofliquids
AT baggiolimatteo universallawforthevibrationaldensityofstatesofliquids