Electron-phonon thermalization in a scalable method for real-time quantum dynamics
Abstract
Here, we present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicit quantum dynamics.
- Authors:
-
- Queen's Univ. Belfast, Northern Ireland (United Kingdom)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1351135
- Alternate Identifier(s):
- OSTI ID: 1236295
- Report Number(s):
- LLNL-JRNL-727623
Journal ID: ISSN 2469-9950; PRBMDO
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 93; Journal Issue: 2; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Rizzi, Valerio, Todorov, Tchavdar N., Kohanoff, Jorge J., and Correa, Alfredo A. Electron-phonon thermalization in a scalable method for real-time quantum dynamics. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.93.024306.
Rizzi, Valerio, Todorov, Tchavdar N., Kohanoff, Jorge J., & Correa, Alfredo A. Electron-phonon thermalization in a scalable method for real-time quantum dynamics. United States. https://doi.org/10.1103/PhysRevB.93.024306
Rizzi, Valerio, Todorov, Tchavdar N., Kohanoff, Jorge J., and Correa, Alfredo A. Wed .
"Electron-phonon thermalization in a scalable method for real-time quantum dynamics". United States. https://doi.org/10.1103/PhysRevB.93.024306. https://www.osti.gov/servlets/purl/1351135.
@article{osti_1351135,
title = {Electron-phonon thermalization in a scalable method for real-time quantum dynamics},
author = {Rizzi, Valerio and Todorov, Tchavdar N. and Kohanoff, Jorge J. and Correa, Alfredo A.},
abstractNote = {Here, we present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicit quantum dynamics.},
doi = {10.1103/PhysRevB.93.024306},
journal = {Physical Review B},
number = 2,
volume = 93,
place = {United States},
year = {Wed Jan 27 00:00:00 EST 2016},
month = {Wed Jan 27 00:00:00 EST 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 17 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Vibrational instabilities in resonant electron transport through single-molecule junctions
journal, March 2011
- Härtle, R.; Thoss, M.
- Physical Review B, Vol. 83, Issue 12
Robust nonadiabatic molecular dynamics for metals and insulators
journal, December 2007
- Stella, L.; Meister, M.; Fisher, A. J.
- The Journal of Chemical Physics, Vol. 127, Issue 21
Ballistic electron transport in non-equilibrium warm dense gold
journal, September 2012
- Ogitsu, Tadashi; Ping, Yuan; Correa, Alfredo
- High Energy Density Physics, Vol. 8, Issue 3
Electronic effects in radiation damage simulations
journal, September 2009
- Duffy, D. M.; Khakshouri, S.; Rutherford, A. M.
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 267, Issue 18
Nanoscale thermal transport. II. 2003–2012
journal, March 2014
- Cahill, David G.; Braun, Paul V.; Chen, Gang
- Applied Physics Reviews, Vol. 1, Issue 1
Thermal excitation of electrons in energetic displacement cascades
journal, July 1991
- Finnis, M. W.; Agnew, P.; Foreman, A. J. E.
- Physical Review B, Vol. 44, Issue 2
Ion-electron interaction in molecular-dynamics cascades
journal, September 1989
- Caro, A.; Victoria, M.
- Physical Review A, Vol. 40, Issue 5
Beyond Ehrenfest: correlated non-adiabatic molecular dynamics
journal, November 2004
- Horsfield, Andrew P.; Bowler, D. R.; Fisher, A. J.
- Journal of Physics: Condensed Matter, Vol. 16, Issue 46
Electron-phonon interactions in energetic displacement cascades
journal, October 1988
- Flynn, C. P.; Averback, R. S.
- Physical Review B, Vol. 38, Issue 10
The treatment of electronic excitations in atomistic models of radiation damage in metals
journal, October 2010
- Race, C. P.; Mason, D. R.; Finnis, M. W.
- Reports on Progress in Physics, Vol. 73, Issue 11
Electronic effects in high-energy radiation damage in iron
journal, February 2014
- Zarkadoula, E.; Daraszewicz, S. L.; Duffy, D. M.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 8
Molecular transport junctions: vibrational effects
journal, February 2007
- Galperin, Michael; Ratner, Mark A.; Nitzan, Abraham
- Journal of Physics: Condensed Matter, Vol. 19, Issue 10
The transfer of energy between electrons and ions in solids
journal, March 2006
- Horsfield, A. P.; Bowler, D. R.; Ness, H.
- Reports on Progress in Physics, Vol. 69, Issue 4
Coherent excitations and electron–phonon coupling in Ba/EuFe 2 As 2 compounds investigated by femtosecond time- and angle-resolved photoemission spectroscopy
journal, February 2013
- Avigo, I.; Cortés, R.; Rettig, L.
- Journal of Physics: Condensed Matter, Vol. 25, Issue 9
Current-induced atomic dynamics, instabilities, and Raman signals: Quasiclassical Langevin equation approach
journal, June 2012
- Lü, Jing-Tao; Brandbyge, Mads; Hedegård, Per
- Physical Review B, Vol. 85, Issue 24
Laserlike Vibrational Instability in Rectifying Molecular Conductors
journal, July 2011
- Lü, Jing-Tao; Hedegård, Per; Brandbyge, Mads
- Physical Review Letters, Vol. 107, Issue 4
Time-Domain Ab Initio Modeling of Photoinduced Dynamics at Nanoscale Interfaces
journal, April 2015
- Wang, Linjun; Long, Run; Prezhdo, Oleg V.
- Annual Review of Physical Chemistry, Vol. 66, Issue 1
Measuring correlated electronic and vibrational spectral dynamics using line shapes in two-dimensional electronic-vibrational spectroscopy
journal, May 2015
- Lewis, Nicholas H. C.; Dong, Hui; Oliver, Thomas A. A.
- The Journal of Chemical Physics, Vol. 142, Issue 17
Current-induced forces: a simple derivation
journal, September 2014
- Todorov, Tchavdar N.; Dundas, Daniel; Lü, Jing-Tao
- European Journal of Physics, Vol. 35, Issue 6
Including the effects of electronic stopping and electron–ion interactions in radiation damage simulations
journal, December 2006
- Duffy, D. M.; Rutherford, A. M.
- Journal of Physics: Condensed Matter, Vol. 19, Issue 1
Quantum-Classical Transition Induced by Electrical Measurement
journal, June 2002
- Mozyrsky, D.; Martin, I.
- Physical Review Letters, Vol. 89, Issue 1
Atomistic simulation study of short pulse laser interactions with a metal target under conditions of spatial confinement by a transparent overlayer
journal, May 2014
- Karim, Eaman T.; Shugaev, Maxim; Wu, Chengping
- Journal of Applied Physics, Vol. 115, Issue 18
Incorporating non-adiabatic effects in embedded atom potentials for radiation damage cascade simulations
journal, March 2015
- Mason, Daniel
- Journal of Physics: Condensed Matter, Vol. 27, Issue 14
Correlated electron–ion dynamics: the excitation of atomic motion by energetic electrons
journal, July 2005
- Horsfield, Andrew P.; Bowler, D. R.; Fisher, A. J.
- Journal of Physics: Condensed Matter, Vol. 17, Issue 30
Direct measurement of nonequilibrium electron-energy distributions in subpicosecond laser-heated gold films
journal, May 1992
- Fann, W. S.; Storz, R.; Tom, H. W. K.
- Physical Review Letters, Vol. 68, Issue 18
Electron thermalization in gold
journal, November 1992
- Fann, W. S.; Storz, R.; Tom, H. W. K.
- Physical Review B, Vol. 46, Issue 20
Inelastic transport theory from first principles: Methodology and application to nanoscale devices
journal, May 2007
- Frederiksen, Thomas; Paulsson, Magnus; Brandbyge, Mads
- Physical Review B, Vol. 75, Issue 20
The effect of electronic energy loss on the dynamics of thermal spikes in Cu
journal, March 1991
- Prönnecke, S.; Caro, A.; Victoria, M.
- Journal of Materials Research, Vol. 6, Issue 3
Electronic Structure of Warm Dense Copper Studied by Ultrafast X-Ray Absorption Spectroscopy
journal, April 2011
- Cho, B. I.; Engelhorn, K.; Correa, A. A.
- Physical Review Letters, Vol. 106, Issue 16
Density Functional Theory of the Electrical Conductivity of Molecular Devices
journal, April 2005
- Burke, Kieron; Car, Roberto; Gebauer, Ralph
- Physical Review Letters, Vol. 94, Issue 14
Ab initio simulations of sodium using time-dependent density-functional theory
journal, November 1992
- Theilhaber, Joachim
- Physical Review B, Vol. 46, Issue 20
Direct measurement of nonequilibrium electron-energy distributions in sub-picosecond laser-heated gold films
journal, March 1993
- Farm, W. S.; Storz, R.; Tom, H. W. K.
- Surface Science, Vol. 283, Issue 1-3
Robust non-adiabatic molecular dynamics for metals and insulators
text, January 2007
- Stella, L.; Meister, M.; Fisher, A. J.
- arXiv
Laser-like vibrational instability in rectifying molecular conductors
text, January 2011
- Lü, Jing-Tao; Hedegård, Per; Brandbyge, Mads
- arXiv
Coherent excitations and electron phonon coupling in Ba/EuFe_2As_2 compounds investigated by femtosecond time- and angle-resolved photoemission spectroscopy
text, January 2012
- Avigo, Isabella; Cortés, Rocio; Rettig, Laurenz
- arXiv
Current-induced atomic dynamics, instabilities, and Raman signals: Quasi-classical Langevin equation approach
text, January 2012
- Lü, Jing Tao; Brandbyge, Mads; Hedegård, Per
- arXiv
Incorporating non-adiabatic effects in Embedded Atom potentials for radiation damage cascade simulations
text, January 2014
- Mason, Daniel
- arXiv
The transfer of energy between electrons and ions in solids
text, January 2006
- Horsfield, A. P.; Bowler, D. R.; Ness, H.
- arXiv
Inelastic transport theory from first-principles: methodology and applications for nanoscale devices
text, January 2006
- Frederiksen, Thomas; Paulsson, Magnus; Brandbyge, Mads
- arXiv
Molecular Transport Junctions: Vibrational Effects
text, January 2006
- Galperin, Michael; Ratner, Mark A.; Nitzan, Abraham
- arXiv
Works referencing / citing this record:
Interactions between low energy electrons and DNA: a perspective from first-principles simulations
journal, August 2017
- Kohanoff, Jorge; McAllister, Maeve; Tribello, Gareth A.
- Journal of Physics: Condensed Matter, Vol. 29, Issue 38
First principles simulation of damage to solvated nucleotides due to shock waves
journal, January 2019
- Fraile, Alberto; Smyth, Maeve; Kohanoff, Jorge
- The Journal of Chemical Physics, Vol. 150, Issue 1
Nature of Bosonic Excitations revealed by high-energy charge carriers
text, January 2016
- Kogoj, Jan; Mierzejewski, Marcin; Bonča, Janez
- arXiv