Year: 2019
Type: article
Abstract: electronic structure simulations of molecules and materials. The central ingredient setting subsystem DFT apart from Kohn-Sham DFT is the nonadditive kinetic energy functional (NAKE). Currently employed NAKEs are at most semilocal (i.e., they only depend on the electron density and its gradient), and as a result of this approximation, so far large-scale simulations only included systems composed of weakly interacting subsystems. In this work, we advance the state-of-the-art by introducing fully nonlocal NAKEs in subsystem DFT simulations for the first time. A benchmark analysis based on the S22-5 test set shows that nonlocal NAKEs considerably improve the computed interaction energies and electron densities compared to commonly employed GGA NAKEs, especially when increasing intersubsystem electron density overlap is considered. Most importantly, we resolve the long-standing problem of too attractive interaction energy curves typically resulting from the use of GGA NAKEs.
Authors: Wenhui Mi, Michele Pavanello
Institution: Rutgers, The State University of New Jersey
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Funder: Division of Chemistry
Award: G3043815781
OpenAlex ID: W2986509199