Author, as appears in the article.: Malaspina, D C; Lisal, M; Larentzos, J P; Brennan, J K; Mackie, A D; Avalos, J Bonet
Department: Enginyeria Química
URV's Author/s: Bonet Avalos, José / Mackie Walker, Allan Donald
Keywords: Energy-conservation
Abstract: This article addresses the debate about the correct application of Green-Kubo expressions for transport coefficients from dissipative particle dynamics simulations. We demonstrate that the Green-Kubo expressions are valid provided that (i) the dynamic model conserves the physical property, whose transport is studied, and (ii) the fluctuations satisfy detailed balance. As a result, the traditional expressions used in molecular dynamics can also be applied to dissipative particle dynamics simulations. However, taking the calculation of the shear viscosity as a paradigmatic example, a random contribution, whose strength scales as 1/δt1/2, with δt the time-step, can cause difficulties if the stress tensor is not separated into the different contributions. We compare our expression to that of Ernst and Brito (M. H. Ernst and R. Brito, Europhys. Lett., 2006, 73, 183-189), which arises from a diametrically different perspective. We demonstrate that the two expressions are completely equivalent and find exactly the same result both analytically and numerically. We show that the differences are not due to the lack of time-reversibility but instead from a pre-averaging of the random contributions. Despite the overall validity of Green-Kubo expressions, we find that the Einstein-Helfand relations (D. C. Malaspina et al. Phys. Chem. Chem. Phys., 2023, 25, 12025-12040) do not suffer from the need to decompose the stress tensor and can readily be used with a high degree of accuracy. Consequently, Einstein-Helfand relations should be seen as the preferred method to calculate transport coefficients from dissipative particle dynamics simulations.
Thematic Areas: Química Physics, atomic, molecular & chemical Physics and astronomy (miscellaneous) Physics and astronomy (all) Physical and theoretical chemistry Odontología Medicina ii Medicina i Materiais Matemática / probabilidade e estatística Interdisciplinar Geociências General physics and astronomy General medicine Farmacia Ensino Engenharias iv Engenharias iii Engenharias ii Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Ciência de alimentos Ciência da computação Chemistry, physical Biotecnología Biodiversidade Astronomia / física
licence for use: https://creativecommons.org/licenses/by/3.0/es/
Author's mail: allan.mackie@urv.cat josep.bonet@urv.cat
Author identifier: 0000-0002-1819-7820 0000-0002-7339-9564
Record's date: 2024-10-12
Papper version: info:eu-repo/semantics/publishedVersion
Link to the original source: https://pubs.rsc.org/en/Content/ArticleLanding/2023/CP/D3CP03791F
Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
Papper original source: Physical Chemistry Chemical Physics. 26 (2): 1328-1339
APA: Malaspina, D C; Lisal, M; Larentzos, J P; Brennan, J K; Mackie, A D; Avalos, J Bonet (2024). Green-Kubo expressions for transport coefficients from dissipative particle dynamics simulations revisited. Physical Chemistry Chemical Physics, 26(2), 1328-1339. DOI: 10.1039/d3cp03791f
Article's DOI: 10.1039/d3cp03791f
Entity: Universitat Rovira i Virgili
Journal publication year: 2024
Publication Type: Journal Publications