Facile ab initio approach for self-localized polarons from canonical transformations

Abstract

Electronic states in a crystal can localize due to strong electron-phonon (e-ph) interactions, forming so-called small polarons. Methods to predict the formation and energetics of small polarons are either computationally costly or not geared toward quantitative predictions. Here we show a formalism based on canonical transformations to compute the polaron formation energy and wavefunction using ab initio e-ph interactions. Comparison of the calculated polaron and band edge energies allows us to determine whether charge carriers in a material favor a localized small polaron over a delocalized Bloch state. Due to its low computational cost, our approach enables efficient studies of the formation and energetics of small polarons, as we demonstrate by investigating electron and hole polaron formation in alkali halides and metal oxides and peroxides. We outline refinements of our scheme and extensions to compute transport in the polaron hopping regime.

arXiv comment6 pages, 3 figures

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• The Wannier Function Software Ecosystem for Materials Simulations
• Identification of large polarons and exciton polarons in rutile and anatase polymorphs of titanium dioxide
• Computational protocol to evaluate electron-phonon interactions within density matrix perturbation theory
• Data-driven compression of electron-phonon interactions
• 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
• Polarons in the Cubic Generalized Fröhlich Model: Spontaneous Symmetry Breaking
• Variational first-principles approach to self-trapped polarons
• Comparison between first-principles supercell calculations of polarons and the ab initio polaron equations