| Literature DB >> 33495319 |
Alessio Zaccone1,2,3, Matteo Baggioli4,5,6.
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.Entities:
Keywords: instantaneous normal modes; liquids; unstable states; vibrational properties
Year: 2021 PMID: 33495319 PMCID: PMC7865170 DOI: 10.1073/pnas.2022303118
Source DB: PubMed Journal: Proc Natl Acad Sci U S A ISSN: 0027-8424 Impact factor: 11.205