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Title: Langevin Dynamics with Spatial Correlations as a Model for Electron-Phonon Coupling

Abstract

Stochastic Langevin dynamics has been traditionally used as a tool to describe nonequilibrium processes. When utilized in systems with collective modes, traditional Langevin dynamics relaxes all modes indiscriminately, regardless of their wavelength. In this paper, we propose a generalization of Langevin dynamics that can capture a differential coupling between collective modes and the bath, by introducing spatial correlations in the random forces. This allows modeling the electronic subsystem in a metal as a generalized Langevin bath endowed with a concept of locality, greatly improving the capabilities of the two-temperature model. The specific form proposed here for the spatial correlations produces a physical wave-vector and polarization dependency of the relaxation produced by the electron-phonon coupling in a solid. We show that the resulting model can be used for describing the path to equilibration of ions and electrons and also as a thermostat to sample the equilibrium canonical ensemble. By extension, the family of models presented here can be applied in general to any dense system, solids, alloys, and dense plasmas. Finally, as an example, we apply the model to study the nonequilibrium dynamics of an electron-ion two-temperature Ni crystal.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Quantum Simulations Group
  2. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Arlington, VA (United States). Dept. of Mechanical Engineering
  3. George Washington Univ., Ashburn, VA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  5. Uppsala Univ. (Sweden). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Dissipation to Defect Evolution (EDDE); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1458684
Alternate Identifier(s):
OSTI ID: 1436003; OSTI ID: 1459271
Report Number(s):
LLNL-JRNL-743460
Journal ID: ISSN 0031-9007; 898486; TRN: US1901505
Grant/Contract Number:  
AC52-07NA27344; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 18; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; electron-phonon coupling; phonons; Langevin equation; molecular dynamics

Citation Formats

Tamm, Artur, Caro, Magdalena, Caro, Alfredo, Samolyuk, German D., Klintenberg, Mattias, and Correa, Alfredo A. Langevin Dynamics with Spatial Correlations as a Model for Electron-Phonon Coupling. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.185501.
Tamm, Artur, Caro, Magdalena, Caro, Alfredo, Samolyuk, German D., Klintenberg, Mattias, & Correa, Alfredo A. Langevin Dynamics with Spatial Correlations as a Model for Electron-Phonon Coupling. United States. doi:10.1103/PhysRevLett.120.185501.
Tamm, Artur, Caro, Magdalena, Caro, Alfredo, Samolyuk, German D., Klintenberg, Mattias, and Correa, Alfredo A. Fri . "Langevin Dynamics with Spatial Correlations as a Model for Electron-Phonon Coupling". United States. doi:10.1103/PhysRevLett.120.185501. https://www.osti.gov/servlets/purl/1458684.
@article{osti_1458684,
title = {Langevin Dynamics with Spatial Correlations as a Model for Electron-Phonon Coupling},
author = {Tamm, Artur and Caro, Magdalena and Caro, Alfredo and Samolyuk, German D. and Klintenberg, Mattias and Correa, Alfredo A.},
abstractNote = {Stochastic Langevin dynamics has been traditionally used as a tool to describe nonequilibrium processes. When utilized in systems with collective modes, traditional Langevin dynamics relaxes all modes indiscriminately, regardless of their wavelength. In this paper, we propose a generalization of Langevin dynamics that can capture a differential coupling between collective modes and the bath, by introducing spatial correlations in the random forces. This allows modeling the electronic subsystem in a metal as a generalized Langevin bath endowed with a concept of locality, greatly improving the capabilities of the two-temperature model. The specific form proposed here for the spatial correlations produces a physical wave-vector and polarization dependency of the relaxation produced by the electron-phonon coupling in a solid. We show that the resulting model can be used for describing the path to equilibration of ions and electrons and also as a thermostat to sample the equilibrium canonical ensemble. By extension, the family of models presented here can be applied in general to any dense system, solids, alloys, and dense plasmas. Finally, as an example, we apply the model to study the nonequilibrium dynamics of an electron-ion two-temperature Ni crystal.},
doi = {10.1103/PhysRevLett.120.185501},
journal = {Physical Review Letters},
number = 18,
volume = 120,
place = {United States},
year = {2018},
month = {5}
}

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Works referenced in this record:

Role of thermal spikes in energetic displacement cascades
journal, October 1987


Simulating Microscopic Hydrodynamic Phenomena with Dissipative Particle Dynamics
journal, June 1992


Phase Transition for a Hard Sphere System
journal, November 1957

  • Alder, B. J.; Wainwright, T. E.
  • The Journal of Chemical Physics, Vol. 27, Issue 5
  • DOI: 10.1063/1.1743957

Statistical Mechanics of Dissipative Particle Dynamics
journal, May 1995


Effects of two-temperature model on cascade evolution in Ni and NiFe
journal, November 2016


Studies in Molecular Dynamics. I. General Method
journal, August 1959

  • Alder, B. J.; Wainwright, T. E.
  • The Journal of Chemical Physics, Vol. 31, Issue 2
  • DOI: 10.1063/1.1730376

Role of Tensorial Electronic Friction in Energy Transfer at Metal Surfaces
journal, May 2016


Electron-Phonon Interactions, d Resonances, and Superconductivity in Transition Metals
journal, March 1972


Theory of thermal relaxation of electrons in metals
journal, September 1987


Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films
journal, January 2016

  • Chase, T.; Trigo, M.; Reid, A. H.
  • Applied Physics Letters, Vol. 108, Issue 4
  • DOI: 10.1063/1.4940981

Molecular dynamics with electronic frictions
journal, December 1995

  • Head‐Gordon, Martin; Tully, John C.
  • The Journal of Chemical Physics, Vol. 103, Issue 23
  • DOI: 10.1063/1.469915

Electron-hole pair contributions to scattering, sticking, and surface diffusion: CO on Cu(100)
journal, September 1998

  • Kindt, James T.; Tully, John C.; Head-Gordon, Martin
  • The Journal of Chemical Physics, Vol. 109, Issue 9
  • DOI: 10.1063/1.476960

Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals
journal, June 1984


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Nonadiabatic Forces in Ion-Solid Interactions: The Initial Stages of Radiation Damage
journal, May 2012


Electron-phonon interaction within classical molecular dynamics
journal, July 2016


Plane-wave pseudopotential implementation of explicit integrators for time-dependent Kohn-Sham equations in large-scale simulations
journal, December 2012

  • Schleife, André; Draeger, Erik W.; Kanai, Yosuke
  • The Journal of Chemical Physics, Vol. 137, Issue 22
  • DOI: 10.1063/1.4758792

Reference systems for computational free energy calculations of binary solutions: role of the constrained center of mass motion
journal, November 2002


Interatomic potentials for monoatomic metals from experimental data and ab initio calculations
journal, February 1999


Warm dense matter created by isochoric laser heating
journal, June 2010


Ultrashort pulse laser ablation of silicon: an MD simulation study
journal, January 1998

  • Herrmann, R. F. W.; Gerlach, J.; Campbell, E. E. B.
  • Applied Physics A: Materials Science & Processing, Vol. 66, Issue 1
  • DOI: 10.1007/s003390050634

Including the effects of electronic stopping and electron–ion interactions in radiation damage simulations
journal, December 2006


Unified Approach for Molecular Dynamics and Density-Functional Theory
journal, November 1985


Spin-lattice-electron dynamics simulations of magnetic materials
journal, May 2012


Adiabatic perturbation theory of electronic stopping in insulators
journal, June 2016


Incorporating non-adiabatic effects in embedded atom potentials for radiation damage cascade simulations
journal, March 2015


Molecular dynamics with electronic transitions
journal, July 1990

  • Tully, John C.
  • The Journal of Chemical Physics, Vol. 93, Issue 2
  • DOI: 10.1063/1.459170

Electronically non-adiabatic interactions of molecules at metal surfaces: Can we trust the Born–Oppenheimer approximation for surface chemistry?
journal, October 2004

  • Wodtke *, Alec M.; Tully, John C.; Auerbach, Daniel J.
  • International Reviews in Physical Chemistry, Vol. 23, Issue 4
  • DOI: 10.1080/01442350500037521

The fluctuation-dissipation theorem
journal, January 1966