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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...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2021
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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 |
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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 |