First-principles diagrammatic Monte Carlo for electron–phonon interactions and polaron
Creators
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1.
California Institute of Technology
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2.
University of Chicago
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3.
Pohang University of Science and Technology
Abstract
In condensed matter, phonons—quanta of the lattice vibration field—couple with electrons, leading to the formation of entangled electron–phonon states called polarons. In the intermediate- and strong-coupling regimes common to many conventional and quantum materials, a many-body treatment of polarons requires adding up a large number of electron–phonon Feynman diagrams. In this regard, diagrammatic Monte Carlo is an efficient method for diagram summation and has been used to study polarons within simplified electron–phonon models. Here we develop diagrammatic Monte Carlo calculations based on accurate first-principles electron–phonon interactions, enabling numerically exact results for the ground-state and dynamical properties of polarons in real materials. We implement these calculations in LiF, SrTiO3, and rutile and anatase TiO2, and describe both localized and delocalized polarons. Our work enables the precise modeling of electron–phonon interactions and polarons in coupling regimes ranging from weak to strong. The results will provide deeper insights into transport phenomena, linear response and superconductivity within the strong electron–phonon coupling regime.
Copyright and License (English)
2025, The Author(s), under exclusive licence to Springer Nature Limited. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
Acknowledgement (English)
Y.L. thanks I. Maliyov, J. Yang and A. Lee for fruitful discussions. Y.L. acknowledges partial support from the Eddleman Graduate Fellowship. M.B. is grateful to the Scuola Normale Superiore in Pisa, Italy, for hosting him during the writing of this manuscript. J.P. acknowledges support from the Chicago Prize Postdoctoral Fellowship in Theoretical Quantum Science. Methods development was supported by the US Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, and Office of Basic Energy Sciences, Scientific Discovery through Advanced Computing (SciDAC), program under award no. DESC0022088. Code development was supported by the National Science Foundation under grant no. OAC-2209262. Calculations of transport and polarons in oxides were supported by the AFOSR and Clarkson Aerospace Corp under award no. FA9550-24-1-0004. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility using NERSC award no. DDR-ERCAP0026831.
Supplemental Material
Supplementary Sections I and II, Figs. 1–13, Equations (1)–(56), Table 1, and theory and implementation details :
41567_2025_2954_MOESM1_ESM.pdf
Data Availability
The datasets generated and analysed in this study are available in the Materials Cloud repository75. Additional data and information are available from the corresponding author upon reasonable request. Source data are provided with this paper.
- Luo, Y., Park, J. & Bernardi, M. Dataset for first-principles diagrammatic Monte Carlo for electron-phonon interactions and polaron. Materials Cloud Archive https://doi.org/10.24435/materialscloud:zy-t3 (2025).
Code Availability
The Perturbo code used to generate the datasets is an open-source software, which can be downloaded at https://perturbo-code.github.io/. The first-principle e–ph DMC routines are available via GitHub at https://github.com/yaoluo/FEP-DMC.
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Additional details
Related works
- Describes
- Journal Article: https://rdcu.be/ewR52 (ReadCube)
Funding
- Office of Advanced Scientific Computing Research
- Scientific Discovery through Advanced Computing (SciDAC) DESC0022088
- National Science Foundation
- OAC-2209262
- United States Air Force Office of Scientific Research
- FA9550-24-1-0004