Nonlinear quasilocalized excitations in glasses. I. True representatives of soft spots

TL;DR

This paper introduces nonlinear quasilocalized excitations (NQEs) as true, non-hybridized representatives of soft spots in glasses, providing a new framework to understand low-energy excitations and their role in glassy phenomena.

Contribution

It presents a theoretical framework for NQEs, demonstrating their distinction from harmonic modes and their relevance as true soft spot representatives in glasses.

Findings

NQEs do not hybridize with other low-energy excitations.

Energies of NQEs converge to the softest harmonic modes.

Statistical analysis predicts distributions of energy barriers and strain thresholds.

Abstract

Structural glasses formed by quenching a melt possess a population of soft quasilocalized excitations --- often called `soft spots' --- that are believed to play a key role in various thermodynamic, transport and mechanical phenomena. Under a narrow set of circumstances, quasilocalized excitations assume the form of vibrational (normal) modes, that are readily obtained by a harmonic analysis of the multi-dimensional potential energy. In general, however, direct access to the population of quasilocalized modes via harmonic analysis is hindered by hybridizations with other low-energy excitations, e.g.~phonons. In this series of papers we re-introduce and investigate the statistical-mechanical properties of a class of low-energy quasilocalized modes --- coined here \emph{nonlinear quasilocalized excitations} (NQEs) --- that are defined via an anharmonic (nonlinear) analysis of the potential energy landscape of a glass, and do not hybridize with other low-energy excitations. In this first paper, we review the theoretical framework that embeds a micromechanical definition of NQEs. We demonstrate how harmonic quasilocalized modes hybridize with other soft excitations, whereas NQEs properly represent soft spots without hybridization. We show that NQEs' energies converge to the energies of the softest, non-hybridized harmonic quasilocalized modes, cementing their status as true representatives of soft spots in structural glasses. Finally, we perform a statistical analysis of the mechanical properties of NQEs, which results in a prediction for the distribution of potential energy barriers that surround typical inherent states of structural glasses, as well as a prediction for the distribution of local strain thresholds to plastic instability.