First-Principles Supercell Calculations of Small Polarons with Proper Account for Long-Range Polarization Effects

Abstract

We present a density functional theory (DFT) based supercell approach for modeling small polarons with proper account for the long-range elastic response of the material. Our analysis of the supercell dependence of the polaron properties (e.g., atomic structure, binding energy, and the polaron level) reveals long-range electrostatic effects and the electron-phonon interaction as the two main contributors. We develop a correction scheme for DFT polaron calculations that significantly reduces the dependence of polaron properties on the DFT exchange-correlation functional and the size of the supercell in the limit of strong electron-phonon coupling. Using our correction approach, we present accurate all-electron full-potential DFT results for small polarons in rocksalt MgO and rutile TiO${}_2$.

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• Facile ab initio approach for self-localized polarons from canonical transformations
• Identification of large polarons and exciton polarons in rutile and anatase polymorphs of titanium dioxide
• Comparison of the canonical transformation and energy functional formalisms for ab initio calculations of self-localized polarons
• Variational Polaron Equations Applied to the Anisotropic Fröhlich Model
• Ab initio typical medium theory of substitutional disorder
• General memory kernels and further corrections to the variational path integral approach for the Bogoliubov-Fröhlich Hamiltonian
• Variational first-principles approach to self-trapped polarons
• Comparison between first-principles supercell calculations of polarons and the ab initio polaron equations