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TT: Fachverband Tiefe Temperaturen

TT 14: Frontiers of Electronic-Structure Theory: Correlated Electron Materials I (joint session O/MM/DS/TT/CPP)

TT 14.8: Vortrag

Montag, 12. März 2018, 12:15–12:30, HL 001

First-principles modeling of mixed-valence compounds from extended Hubbard-corrected functionals — •Matteo Cococcioni and Nicola Marzari — Theory and Simulations of Materials and MARVEL, EPFL, Lausanne, Switzerland

Modeling the electronic properties of mixed valence compounds is central to developing many materials of technological relevance. Unfortunately, most approximate implementations of density functional theory (DFT) fail in capturing the localization of valence electrons on low dispersion states (e.g., of d or f kind) and mis-represent many properties of these systems. Quantitatively predictive first-principles calculations thus require, for these systems, the use of corrective functionals able to improve the description of electronic localization. Using the results of a recent study on materials for cathodes of Li-ion batteries this work shows how an extended Hubbard correction to DFT functionals, including on-site (U) and inter-site (V) interactions (named DFT+U+V) improves considerably on simpler approximations for electronic, magnetic and structural properties and correctly describes localized states even in presence of significant inter-site hybridization. The work also demonstrates that evaluating the effective interaction parameters (U and V) consistently with the electronic and crystal structures, and treating them as material-specific quantities, improves the prediction of thermodynamic quantities and of average voltages. Finally, a novel method to compute these interactions from density-functional perturbation theory is shown to guarantee unprecedented efficiency, accuracy and convergence control.