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Equilibrium molecular dynamics simulations, in combination with the Green-Kubo (GK) method, have been extensively used to compute the thermal conductivity of liquids. However, the GK method relies on an ambiguous definition of the…

计算物理 · 物理学 2020-09-30 Bingqing Cheng , Daan Frenkel

The Green-Kubo (GK) method is a rigorous framework for heat transport simulations in materials. However, it requires an accurate description of the potential-energy surface and carefully converged statistics. Machine-learning potentials can…

Water's unique hydrogen-bonding network and anomalous properties pose significant challenges for accurately modeling its structural, thermodynamic, and transport behavior across varied conditions. Although machine-learned potentials have…

化学物理 · 物理学 2025-08-29 Ke Xu , Ting Liang , Nan Xu , Penghua Ying , Shunda Chen , Ning Wei , Jianbin Xu , Zheyong Fan

We report on an extensive study of the viscosity of liquid water at near-ambient conditions, performed within the Green-Kubo theory of linear response and equilibrium ab initio molecular dynamics (AIMD), based on density-functional theory…

材料科学 · 物理学 2022-07-05 Cesare Malosso , Linfeng Zhang , Roberto Car , Stefano Baroni , Davide Tisi

We present a method, based on the classical Green-Kubo theory of linear response, to compute the heat conductivity of extended systems, leveraging energy-density, rather than energy-current, fluctuations, thus avoiding the need to devise an…

材料科学 · 物理学 2024-02-01 Enrico Drigo , Maria Grazia Izzo , Stefano Baroni

Thermodynamic properties of liquid water as well as hexagonal (Ih) and cubic (Ic) ice are predicted based on density functional theory at the hybrid-functional level, rigorously taking into account quantum nuclear motion, anharmonic…

材料科学 · 物理学 2025-10-06 Bingqing Cheng , Edgar A. Engel , Jörg Behler , Christoph Dellago , Michele Ceriotti

We develop a neuroevolution-potential (NEP) framework for generating neural network based machine-learning potentials. They are trained using an evolutionary strategy for performing large-scale molecular dynamics (MD) simulations. A…

计算物理 · 物理学 2022-01-25 Zheyong Fan , Zezhu Zeng , Cunzhi Zhang , Yanzhou Wang , Haikuan Dong , Yue Chen , Tapio Ala-Nissila

The evaluation of transport coefficients in extended systems, such as thermal conductivity or shear viscosity, is known to require impractically long simulations, thus calling for a paradigm shift that would allow to deploy state-of-the-art…

统计力学 · 物理学 2019-09-30 Loris Ercole , Aris Marcolongo , Stefano Baroni

Simulating water from first principles remains a significant computational challenge due to the slow dynamics of the underlying system. Although machine-learned interatomic potentials (MLPs) can accelerate these simulations, they often fail…

化学物理 · 物理学 2026-01-30 Tobias Hilpert , Georg Kresse

Using a neural network potential (ANI-1ccx) generated from quantum data on a large data set of molecules and pairs of molecules, isothermal, constant volume simulations demonstrate that the model can be as accurate as ab initio molecular…

化学物理 · 物理学 2021-01-11 Alexander S. Lyons, , Steven W. Rick

The accuracy of the training data limits the accuracy of bulk properties from machine-learned potentials. For example, hybrid functionals or wave-function-based quantum chemical methods are readily available for cluster data but effectively…

计算物理 · 物理学 2023-12-05 Viktor Zaverkin , David Holzmüller , Robin Schuldt , Johannes Kästner

We have applied path integral simulations, in combination with new ab initio based water potentials, to investigate nuclear quantum effects in liquid water. Because direct ab initio path integral simulations are computationally expensive, a…

化学物理 · 物理学 2015-04-21 Thomas Spura , Christopher John , Scott Habershon , Thomas D. Kühne

Simulation techniques based on accurate and efficient representations of potential energy surfaces are urgently needed for the understanding of complex aqueous systems such as solid-liquid interfaces. Here, we present a machine learning…

We calculate the energy and heat capacity of a liquid on the basis of its elastic properties and vibrational states. The experimental decrease of liquid heat capacity with temperature is attributed to the increasing loss of two transverse…

软凝聚态物质 · 物理学 2009-11-13 Kostya Trachenko

The thermal conductivity of classical multi-component fluids is seemingly affected by the intrinsic arbitrariness in the definition of the atomic energies and it is ill-conditioned numerically, when evaluated from the Green-Kubo theory of…

统计力学 · 物理学 2019-09-30 Riccardo Bertossa , Federico Grasselli , Loris Ercole , Stefano Baroni

Quantum simulation methods based on density-functional theory are currently deemed unfit to cope with atomic heat transport within the Green-Kubo formalism, because quantum-mechanical energy densities and currents are inherently ill-defined…

材料科学 · 物理学 2016-01-20 Aris Marcolongo , Paolo Umari , Stefano Baroni

We introduce a scheme based on machine learning and deep neural networks to model the environmental dependence of the electronic polarizability in insulating materials. Application to liquid water shows that training the network with a…

化学物理 · 物理学 2020-06-24 Grace M. Sommers , Marcos F. Calegari Andrade , Linfeng Zhang , Han Wang , Roberto Car

The Green-Kubo theory of thermal transport has long be considered incompatible with modern simulation methods based on electronic-structure theory, because it is based on such concepts as energy density and current, which are ill-defined at…

统计力学 · 物理学 2018-08-20 Stefano Baroni , Riccardo Bertossa , Loris Ercole , Federico Grasselli , Aris Marcolongo

We propose an efficient approach for simultaneous prediction of thermal and electronic transport properties in complex materials. Firstly, a highly efficient machine-learned neuroevolution potential is trained using reference data from…

材料科学 · 物理学 2024-04-08 Zheyong Fan , Yang Xiao , Yanzhou Wang , Penghua Ying , Shunda Chen , Haikuan Dong

It is shown that the hydrodynamic modes of a dilute granular gas of inelastic hard spheres can be identified, and calculated in the long wavelength limit. Assuming they dominate at long times, formal expressions for the Navier-Stokes…

统计力学 · 物理学 2009-11-10 J. Javier Brey , M. J. Ruiz-Montero , P. Maynar , I. Garcia de Soria
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