Quantum bath augmented stochastic nonequilibrium atomistic simulations for molecular heat conduction

Renai Chen*, Mohammadhasan Dinpajooh, Abraham Nitzan

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


Classical molecular dynamics (MD) has been shown to be effective in simulating heat conduction in certain molecular junctions since it inherently takes into account some essential methodological components which are lacking in the quantum Landauer-type transport model, such as many-body full force-field interactions, anharmonicity effects and nonlinear responses for large temperature biases. However, the classical MD reaches its limit in the environments where the quantum effects are significant (e.g. with low-temperatures substrates, presence of extremely high frequency molecular modes). Here, we present an atomistic simulation methodology for molecular heat conduction that incorporates the quantum Bose-Einstein statistics into an “effective temperature” in the form of a modified Langevin equation. We show that the results from such a quasi-classical effective temperature MD method deviates drastically when the baths temperature approaches zero from classical MD simulations and the results converge to the classical ones when the bath approaches the high-temperature limit, which makes the method suitable for full temperature range. In addition, we show that our quasi-classical thermal transport method can be used to model the conducting substrate layout and molecular composition (e.g. anharmonicities, high-frequency modes). Anharmonic models are explicitly simulated via the Morse potential and compared to pure harmonic interactions to show the effects of anharmonicities under quantum colored bath setups. Finally, the chain length dependence of heat conduction is examined for one-dimensional polymer chains placed in between quantum augmented baths.

Original languageEnglish
Article number134110
JournalJournal of Chemical Physics
Issue number13
StatePublished - 7 Oct 2023


FundersFunder number
Center for Nonlinear Studies
National Science FoundationCHE1953701
U.S. Department of Energy
Office of Science
Basic Energy Sciences
University of Pennsylvania
Los Alamos National Laboratory
Chemical Sciences, Geosciences, and Biosciences DivisionFWP 16249


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