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Main Authors: Schmitz, Niklas Frederik, Ploumhans, Bruno, Herbst, Michael F.
Format: Preprint
Published: 2025
Subjects:
Online Access:https://arxiv.org/abs/2509.07785
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author Schmitz, Niklas Frederik
Ploumhans, Bruno
Herbst, Michael F.
author_facet Schmitz, Niklas Frederik
Ploumhans, Bruno
Herbst, Michael F.
contents We present a differentiation framework for plane-wave density-functional theory (DFT) that combines the strengths of forward-mode algorithmic differentiation (AD) and density-functional perturbation theory (DFPT). In the resulting AD-DFPT framework derivatives of any DFT output quantity with respect to any input parameter (e.g. geometry, density functional or pseudopotential) can be computed accurately without deriving gradient expressions by hand. We implement AD-DFPT into the Density-Functional ToolKit (DFTK) and show its broad applicability. Amongst others we consider the inverse design of a semiconductor band gap, the learning of exchange-correlation functional parameters, or the propagation of DFT parameter uncertainties to relaxed structures. These examples demonstrate a number of promising research avenues opened by gradient-driven workflows in first-principles materials modeling.
format Preprint
id arxiv_https___arxiv_org_abs_2509_07785
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Algorithmic differentiation for plane-wave DFT: materials design, error control and learning model parameters
Schmitz, Niklas Frederik
Ploumhans, Bruno
Herbst, Michael F.
Materials Science
Computational Physics
We present a differentiation framework for plane-wave density-functional theory (DFT) that combines the strengths of forward-mode algorithmic differentiation (AD) and density-functional perturbation theory (DFPT). In the resulting AD-DFPT framework derivatives of any DFT output quantity with respect to any input parameter (e.g. geometry, density functional or pseudopotential) can be computed accurately without deriving gradient expressions by hand. We implement AD-DFPT into the Density-Functional ToolKit (DFTK) and show its broad applicability. Amongst others we consider the inverse design of a semiconductor band gap, the learning of exchange-correlation functional parameters, or the propagation of DFT parameter uncertainties to relaxed structures. These examples demonstrate a number of promising research avenues opened by gradient-driven workflows in first-principles materials modeling.
title Algorithmic differentiation for plane-wave DFT: materials design, error control and learning model parameters
topic Materials Science
Computational Physics
url https://arxiv.org/abs/2509.07785