Carrier mobility of strongly anharmonic materials from first principles

Physical review. B./Physical review. B, Journal Year: 2024, Volume and Issue: 110(23)

Published: Dec. 6, 2024

First-principles approaches for phonon-limited electronic transport are typically based on many-body perturbation theory and equations. With that, they rely the validity of quasiparticle picture electrons phonons, which is known to fail in strongly anharmonic systems. In this work, we demonstrate relevance effects beyond by combining molecular dynamics Kubo-Greenwood (KG) formalism establish a nonperturbative, stochastic method calculate carrier mobilities while accounting all orders electron-vibrational couplings. particular, propose exploit several numerical strategies that overcome notoriously slow convergence KG both nuclear degrees freedom crystalline solids. The capability demonstrated calculating temperature-dependent electron mobility oxide perovskites SrTiO3 BaTiO3 across wide range temperatures. We show temperature dependence largely driven anharmonic, higher-order coupling rationalize these trends terms nonperturbative spectral functions. Published American Physical Society 2024

Language: Английский

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Na Vacancy-Driven Phase Transformation and Fast Ion Conduction in W-Doped Na₃SbS₄ from Machine Learning Force Fields

Chemistry of Materials, Journal Year: 2024, Volume and Issue: 36(19), P. 9406 - 9413

Published: Sept. 19, 2024

Solid-state sodium batteries require effective electrolytes that conduct at room temperature. The Na

Language: Английский

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Thermal transport of Li$_3$PS$_4$ solid electrolytes with ab initio accuracy

arXiv (Cornell University), Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

The vast amount of computational studies on electrical conduction in solid-state electrolytes is not mirrored by comparable efforts addressing thermal conduction, which has been scarcely investigated despite its relevance to management and (over)heating batteries. reason for this lies the complexity calculations: one hand, diffusion ionic charge carriers makes lattice methods formally unsuitable, due lack equilibrium atomic positions needed normal-mode expansion. On other prohibitive cost large-scale molecular dynamics (MD) simulations heat transport large systems at ab initio levels hindered use MD-based methods. In paper, we leverage recently developed machine-learning potentials targeting different functionals (PBEsol, r$^2$SCAN, PBE0) a state-of-the-art formulation Green-Kubo theory multicomponent compute conductivity promising electrolyte, Li$_3$PS$_4$, all polymorphs ($\alpha$, $\beta$, $\gamma$). By comparing MD estimates with low-temperature, nondiffusive $\gamma$-Li$_3$PS$_4$, highlight strong anharmonicities negligible nuclear quantum effects, hence further justifying even phases. Finally, ion-conducting $\alpha$ $\beta$ phases, where approach mandatory, our indicate weak temperature dependence conductivity, glass-like behavior effective local disorder characterizing these Li-diffusing

Language: Английский

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Tracking Li atoms in real-time with ultra-fast NMR simulations

Faraday Discussions, Journal Year: 2024, Volume and Issue: unknown

Published: May 3, 2024

Using machine learning we are able simulate Li dynamics and predict the autocorrelation function for 7 spin alignment echo NMR in crystalline amorphous 3 PS 4 .

Language: Английский

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Structural and thermodynamic properties of the Li6PS5Cl solid electrolyte using first-principles calculations

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Static and dynamic ab initio simulations predict the crystallographic sites, constant-pressure heat capacity, thermodynamical stability at high temperature of Li 6 PS 5 Cl, a solid electrolyte actively considered for solid-state batteries.

Language: Английский

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