Self-consistent implementation of locally scaled self-interaction-correction method

Abstract

Recently proposed local self-interaction correction (LSIC) method [Zope, R. R. et al., J. Chem. Phys. 151, 214108 (2019)] is a one-electron self-interaction-correction (SIC) method that uses an iso-orbital indicator to apply the SIC at each point in space by scaling the exchange-correlation and Coulomb energy densities. The LSIC method is exact for the one-electron densities, also recovers the uniform electron gas limit of the uncorrected density functional approximation, and reduces to the well-known Perdew-Zunger SIC (PZSIC) method as a special case. This article presents the self-consistent implementation of the LSIC method using the ratio of Weizs ̈acker and Kohn-Sham kinetic energy densities as an iso-orbital indicator. The atomic forces as well as the forces on the Fermi-L ̈owdin orbitals are also implemented for the LSIC energy functional. Results show that LSIC with the simplest local spin density functional predicts atomization energies of AE6 dataset better than some of the most widely used GGA functional (e.g. PBE) and barrier heights of BH6 database better than some of the most widely used hybrid functionals (e.g. PBE0 and B3LYP). The LSIC method [mean absolute error (MAE) of 0.008 ̊A] predicts bond lengths of a small set of molecules better than the PZSIC-LSDA (MAE 0.042 ̊A) and LSDA (0.011 ̊A). This work shows that accurate results can be obtained from the simplest density functional by removing the self-interaction-errors using an appropriately designed SIC method.

Pressure-Dependent Magnetic Properties of Quasi-2D Cr2Si2Te6 and Mn3Si2Te6

“…For the analysis of pressure-dependent magnetic properties, the U values once determined are often kept fixed, , which is often a reasonable assumption, particularly when the pressure is small as in our study. However, in CST, the inclusion of Hubbard U correction has a much more significant impact on J 1 and little effect on the band gap (see Figure S2 in Supporting Information) and the magnetic moments. , While the issue can potentially be mitigated by performing self-interaction correction, − GW or dynamical mean-field theory calculations, these methods are computationally too demanding and beyond the scope of this work.…”

How Do Self-Interaction Errors Associated with Stretched Bonds Affect Barrier Height Predictions?

“…E LSIC is evaluated on the self-consistent PZSIC density. Recent studies show 31 that using a self-consistent LSIC density does not change LSIC results significantly.…”

A numerical Poisson solver with improved radial solutions for a self-consistent locally scaled self-interaction correction method

“…This results in significant improvements over PZSIC. LSIC method has provided accurate results for properties such as atomization energies [6,7], electron affinities, magnetic properties, dipole moments, and polarizabilities [8][9][10], vertical electron detachment energies [11,12], exchange-coupling constants [13] and spin-state gaps of octahedral complexes [14]. It also significantly reduces fractional electron or delocalization errors [15].…”

“…The z σ (⃗ r) is the iso-orbital indicator which is used to identify the one-electron regions and to scale the energy densities in the SIC terms. We refer the interested to [6,7] for more details. The functional derivative of E LSIC with respect to variation in density is written as follows, δE LSIC δρ (r)…”

“…In the majority of instances, Dunlap correction demonstrates quadratic convergence in energy, and combining electrostatic energies is a common practice to mitigate error accumulation. However, in specialized cases like ours in LSIC method [6,7], implementing additional correction techniques can be impractical or cost-prohibitive. In response to this challenge, we propose a straightforward method to directly enhance the accuracy of radial solutions, thereby reducing errors.…”