Articles producció científica> Enginyeria Química

Green-Kubo expressions for transport coefficients from dissipative particle dynamics simulations revisited

  • Identification data

    Identifier: imarina:9333649
    Authors:
    Malaspina, D CLisal, MLarentzos, J PBrennan, J KMackie, A DAvalos, J Bonet
    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.
  • Others:

    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
  • Keywords:

    Chemistry, Physical,Physical and Theoretical Chemistry,Physics and Astronomy (Miscellaneous),Physics, Atomic, Molecular & Chemical
    Energy-conservation
    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
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