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Published August 2021 | Published
Journal Article Open

Nonequilibrium thermomechanics of Gaussian phase packet crystals: Application to the quasistatic quasicontinuum method


The quasicontinuum (QC) method was originally introduced to bridge across length scales by coarse-graining an atomistic ensemble to significantly larger continuum scales at zero temperature, thus overcoming the crucial length-scale limitation of classical atomic-scale simulation techniques while solely relying on atomic-scale input (in the form of interatomic potentials). An associated challenge lies in bridging across time scales to overcome the time-scale limitations of atomistics at finite temperature. To address the biggest challenge, bridging across both length and time scales, only a few techniques exist, and most of those are limited to conditions of constant temperature. Here, we present a new general strategy for the space–time coarsening of an atomistic ensemble, which introduces thermomechanical coupling. Specifically, we evolve the statistics of an atomistic ensemble in phase space over time by applying the Liouville equation to an approximation of the ensemble's probability distribution (which further admits a variational formulation). To this end, we approximate a crystalline solid as a lattice of lumped correlated Gaussian phase packets occupying atomic lattice sites, and we investigate the resulting quasistatics and dynamics of the system. By definition, phase packets account for the dynamics of crystalline lattices at finite temperature through the statistical variances of atomic momenta and positions. We show that momentum–space correlation allows for an exchange between potential and kinetic contributions to the crystal's Hamiltonian. Consequently, local adiabatic heating due to atomic site motion is captured. Moreover, in the quasistatic limit, the governing equations reduce to the minimization of thermodynamic potentials (similar to maximum-entropy formulation previously introduced for finite-temperature QC), and they yield the local equation of state, which we derive for isothermal, isobaric, and isentropic conditions. Since our formulation without interatomic correlations precludes irreversible heat transport, we demonstrate its combination with thermal transport models to describe realistic atomic-level processes, and we discuss opportunities for capturing atomic-level thermal transport by including interatomic correlations in the Gaussian phase packet formulation. Overall, our Gaussian phase packet approach offers a promising avenue for finite-temperature non-equilibrium quasicontinuum techniques, which may be combined with thermal transport models and extended to other approximations of the probability distribution as well as to exploit the variational structure.

Additional Information

© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license. Received 10 January 2021, Revised 11 April 2021, Accepted 13 May 2021, Available online 17 May 2021. The support from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 770754) is gratefully acknowledged. The authors thank Miguel Angel Spinola Fandila for help with the LAMMPS simulations used for numerical validation. CRediT authorship contribution statement: Prateek Gupta: Conceptualization, Methodology, Software, Validation, Investigation, Data curation, Writing - original draft. Michael Ortiz: Conceptualization, Methodology. Dennis M. Kochmann: Conceptualization, Methodology, Writing - review & editing, Supervision, Funding acquisition. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

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August 22, 2023
October 23, 2023