Nonlocal pseudopotential energy density functional for orbitalfree density functional theory
Abstract
Orbitalfree density functional theory (OFDFT) is an electronic structure method with a low computational cost that scales linearly with the number of simulated atoms, making it suitable for largescale material simulations. It is generally considered that OFDFT strictly requires the use of local pseudopotentials, rather than orbitaldependent nonlocal pseudopotentials, for the calculation of electronion interaction energies, as no orbitals are available. This is unfortunate situation since the nonlocal pseudopotentials are known to give much better transferability and calculation accuracy than local ones. We report here the development of a theoretical scheme that allows the direct use of nonlocal pseudopotentials in OFDFT. In this scheme, a nonlocal pseudopotential energy density functional is derived by the projection of nonlocal pseudopotential onto the noninteracting density matrix (instead of "orbitals") that can be approximated explicitly as a functional of electron density. Our development defies the belief that nonlocal pseudopotentials are not applicable to OFDFT, leading to the creation for an alternate theoretical framework of OFDFT that works superior to the traditional approach.
 Publication:

Nature Communications
 Pub Date:
 March 2022
 DOI:
 10.1038/s41467022290023
 arXiv:
 arXiv:2201.00901
 Bibcode:
 2022NatCo..13.1385X
 Keywords:

 Condensed Matter  Materials Science;
 Physics  Computational Physics
 EPrint:
 8 pages, 4 figures