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Transport coefficients from Einstein–Helfand relations using standard and energy-conserving dissipative particle dynamics methods

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    0571358 - ÚCHP 2024 RIV GB eng J - Journal Article
    Malaspina, D.C. - Lísal, Martin - Larentzos, J.P. - Brennan, J.K. - Mackie, A.D. - Avalos, J.B.
    Transport coefficients from Einstein–Helfand relations using standard and energy-conserving dissipative particle dynamics methods.
    Physical Chemistry Chemical Physics. Roč. 25, č. 17 (2023), s. 12025-12040. ISSN 1463-9076. E-ISSN 1463-9084
    Grant - others:ARF(ES) W911NF-20-2-0227; ARF(ES) W911NF-20-2-0203; ERDF(ES) PID2021-122187NB-C33
    Institutional support: RVO:67985858
    Keywords : molecular dynamics * irreversible processes * statistical-mechanics
    OECD category: Physical chemistry
    Impact factor: 3.3, year: 2022
    Method of publishing: Limited access

    In this article we demonstrate that contrary to general belief, the standard Einstein-Helfand (EH) formulas are valid for the evaluation of transport coefficients of systems containing dissipative and random forces provided that for these mesoscopic systems: (i) the corresponding conservation laws are satisfied, and (ii) the transition probabilities satisfy detailed balance. Dissipative particle dynamics (DPD) and energy-conserving DPD methods (DPDE), for instance, are archetypical of such mesoscopic approaches satisfying these properties. To verify this statement, we have derived a mesoscopic heat flux form for the DPDE method, suitable for the calculation of the thermal conductivity from an EH expression. We have compared EH measurements against non-equilibrium simulation values for different scenarios, including many-body potentials, and have found excellent agreement in all cases. The expressions are valid notably for systems with density- and temperature-dependent potentials, such as the recently developed generalised DPDE method (GenDPDE) [Avalos et al., Phys. Chem. Chem. Phys., 2019, 21, 24891]. We thus demonstrate that traditional EH formulas in equilibrium simulations can be widely used to obtain transport coefficients, provided that the appropriate expression for the associated flux is used.
    Permanent Link: https://hdl.handle.net/11104/0342599

     
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