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.

Universal law for the vibrational density of states of liquids / A. Zaccone, M. Baggioli. - In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA. - ISSN 0027-8424. - 118:5(2021), pp. e2022303118.1-e2022303118.3. [10.1073/pnas.2022303118]

Universal law for the vibrational density of states of liquids

A. Zaccone
;
2021

Abstract

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.
liquids; vibrational properties; unstable states; instantaneous normal modes
Settore FIS/02 - Fisica Teorica, Modelli e Metodi Matematici
Settore FIS/03 - Fisica della Materia
2021
Article (author)
File in questo prodotto:
File Dimensione Formato  
DOS_liquids_PNAS_2021.pdf

accesso aperto

Tipologia: Publisher's version/PDF
Dimensione 802.87 kB
Formato Adobe PDF
802.87 kB Adobe PDF Visualizza/Apri
Pubblicazioni consigliate

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2434/810696
Citazioni
  • ???jsp.display-item.citation.pmc??? 3
  • Scopus 29
  • ???jsp.display-item.citation.isi??? 24
social impact