Density functional perturbation theory of meta-generalized gradient approximations using algorithmic differentiation

Abstract

Density functional perturbation theory (DFPT) is an established framework for the computation of derivatives in plane-wave density functional theory. We present an implementation of DFPT for exchange-correlation (XC) functionals $E_\mathrm{xc}(ρ,τ)$ that incorporate an explicit dependence on both the density $ρ$ and the kinetic energy density $τ$. This covers the popular class of semilocal meta-generalized gradient approximations (meta-GGAs) as well as broader nonlocal parametrizations. We sidestep the derivation of cumbersome XC second energy derivative expressions by recasting these derivatives as a Jacobian-vector product of the XC potentials, which we evaluate with algorithmic differentiation (AD) techniques. Integration with our previously developed AD-DFPT framework [N. F. Schmitz et al., npj Comput. Mater. 12, 6 (2026)] provides access to derivatives of arbitrary ground state quantities with respect to arbitrary perturbations. We employ AD-DFPT to compute a range of response properties for ZnO and BaTiO3, and find that the recent r2SCAN01 meta-GGA functional generally outperforms LDA and PBE. Finally, we showcase the optimization of a neural-network meta-GGA to self-consistently reproduce hybrid-DFT reference densities of bulk silicon, using AD-DFPT gradients. Overall, these results establish AD-DFPT as a versatile route for computing DFT derivatives at the meta-GGA level, be they common response properties or the unusual derivatives required for the gradient-based training of novel XC functionals.