English

Construction of meta-GGA functionals through restoration of exact constraint adherence to regularized SCAN functionals

Materials Science 2022-02-02 v1 Chemical Physics Computational Physics

Abstract

The SCAN meta-GGA exchange-correlation functional [Phys. Rev. Lett. 115, 036402 (2015)] is constructed as a chemical environment-determined interpolation between two separate energy densities: one describes single orbital electron densities accurately, and another describes slowly-varying densities accurately. To conserve constraints known for the exact exchange-correlation functional, the derivatives of this interpolation vanish in the slowly-varying limit. While theoretically convenient, this choice introduces numerical challenges that degrade the functional's efficiency. We have recently reported a modification to the SCAN functional, termed r2^2SCAN [J. Phys. Chem. Lett. 11, 8208 (2020)] that introduces two regularizations into SCAN which improve its numerical performance at the expense of not recovering the fourth order term of the slowly-varying density gradient expansion for exchange. Here we show the derivation of a progression of functionals (rSCAN, r++SCAN, r2^2SCAN, and r4^4SCAN) with increasing adherence to exact conditions while maintaining a smooth interpolation. The greater smoothness of r2^2SCAN seems to lead to better general accuracy than the additional exact constraint of SCAN or r4^4SCAN does.

Keywords

Cite

@article{arxiv.2110.00647,
  title  = {Construction of meta-GGA functionals through restoration of exact constraint adherence to regularized SCAN functionals},
  author = {James W. Furness and Aaron D. Kaplan and Jinliang Ning and John P. Perdew and Jianwei Sun},
  journal= {arXiv preprint arXiv:2110.00647},
  year   = {2022}
}