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Microscopic theory and quantum simulation of atomic heat transport

Nature Physics volume 12, pages 8084 (2016) | Download Citation

Abstract

Quantum simulation methods based on electronic-structure theory are deemed unfit to cope with atomic heat transport within the Green–Kubo formalism, because quantum-mechanical energy densities and currents are inherently ill-defined at the atomic scale. We show that, although this difficulty would also affect classical simulations, thermal conductivity is indeed insensitive to such ill-definedness by virtue of a kind of gauge invariance resulting from energy extensivity and conservation. On the basis of these findings, we derive an expression for the adiabatic energy flux from density-functional theory, which allows heat transport to be simulated using ab initio equilibrium molecular dynamics. Our methodology is demonstrated by comparing its predictions to those of classical equilibrium and ab initio non-equilibrium (Müller–Plathe) simulations for a liquid-argon model, and by applying it to heavy water at ambient conditions.

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Acknowledgements

S.B. gratefully acknowledges useful discussions with T. Sun and D. Alfè in the early phases of this work and, more recently, with R. Car and R. Resta. All of the authors gratefully thank L. Colombo, C. Melis, S. R. Philpot and A. Chernatynskiy for communicating to them some of their unpublished material.

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Affiliations

  1. SISSA–Scuola Internazionale Superiore di Studi Avanzati, Via Bonomea 265 34136 Trieste, Italy

    • Aris Marcolongo
    •  & Stefano Baroni
  2. Dipartimento di Fisica e Astronomia, Università di Padova, Via Marzolo 8 I-35131 Padova, Italy

    • Paolo Umari

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Contributions

All authors contributed to all aspects of this work.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Stefano Baroni.

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DOI

https://doi.org/10.1038/nphys3509

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