Implementation of Perdew–Zunger self-interaction correction in real space using Fermi–Löwdin orbitals

Diaz, Carlos M.; Suryanarayana, Phanish; Xu, Qimen; Baruah, Tunna; Pask, John E.; Zope, Rajendra R.

doi:10.1063/5.0031341

Cited by 13 publications

(10 citation statements)

References 121 publications

(128 reference statements)

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“…The exchange-correlation potential V xc [n](r,t) is approximated based on LDA proposed by Perdew and Zunger [66,67]. The external potential due to the laser is defined in velocity gauge as…”

Section: Calculation Methodsmentioning

confidence: 99%

Investigation of parameters affecting the high harmonic generation from monolayer WS₂

Sadeghifaraz

Irani

Monfared

2022

Int J of Quantum Chemistry

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The effect of crystal symmetry in the high harmonic generation of monolayer WS2 is investigated using the three‐dimensional time‐dependent density functional theory. The role of linearly and elliptically polarized laser, as well as the crystall orientation in the enhancement of harmonics yield, is explored. Also, the wavelength dependence of the harmonic yield and the intensity dependence of cutoff harmonic order are studied. The former shows an exponential decay with increasing the driving laser wavelength, and the latter reveals a linear dependency of cutoff harmonic to the driving laser field. Moreover, a dual pulse system as a driving laser, a fundamental 1.3 μm laser pulse synthesized by its second harmonic, is proposed which could increase the cutoff harmonic order up to 24th (22 eV). Our results pave the way for controlling and enhancing high harmonic spectra from solids.

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Section: Calculation Methodsmentioning

confidence: 99%

Investigation of parameters affecting the high harmonic generation from monolayer WS₂

Sadeghifaraz

Irani

Monfared

2022

Int J of Quantum Chemistry

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“…The FLOs and the unoccupied virtual orbitals are made orthogonal through pairwise Jacobi rotations which are carried out iteratively until the matrix elements for the i th orbital Hamiltonian between φ i and a virtual orbital vanishes. Alternative schemes such as a unified Hamiltonian [25,67] and a generalized-Slater scheme in real space [56] have also been used.…”

Section: B Fermi-löwdin Orbital Sic (Flo-sic)mentioning

confidence: 99%

Fermi-Löwdin orbital self-interaction correction using the optimized effective potential method within the Krieger-Li-Iafrate approximation

Diaz,

Baruah,

Zope

2021

Preprint

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Perdew-Zunger self-interaction correction (PZ-SIC) offers a route to remove self-interaction errors on an orbital-by-orbital basis. A recent formulation of PZ-SIC by Pederson, Ruzsinszky and Perdew proposes restricting the unitary transformation to localized orbitals called Fermi-Löwdin orbitals. This formulation, called the FLOSIC method, simplifies PZ-SIC calculations and was implemented self-consistently using a Jacobi-like (FLOSIC-Jacobi) iteration scheme. In this work we implement the FLOSIC approach using the Krieger-Li-Iafrate (KLI) approximation to the optimized effective potential (OEP). We compare the results of present FLOSIC-KLI approach with FLOSIC-Jacobi scheme for atomic energies, atomization energies, ionization energies, barrier heights, polarizability of chains of hydrogen molecules etc. to validate the FLOSIC-KLI approach. The FLOSIC-KLI approach, which is within the realm of Kohn-Sham theory, predicts smaller energy gaps between frontier orbitals due to the lowering of eigenvalues of the lowest unoccupied orbitals. Results show that atomic energies, atomization energies, ionization energy as an absolute of highest occupied orbital eigenvalue, and polarizability of chains of hydrogen molecules between the two methods agree within 2%. Finally the FLOSIC-KLI approach is used to determine the vertical ionization energies of water clusters.

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“…In the original implementation of the FLOSIC method in the FLOSIC code, the occupied subspace relaxation was achieved by means of Jacobi-type rotations to zero the overlap between the occupied and virtual orbitals at each self-consistent iteration, much like traditional implementations of Foster–Boys, , Edmiston–Ruedenberg, or Pipek–Mezey localization schemes. Other implementations of FLOSIC are based on unified Hamiltonian schemes and effective potentials. − In this work, we introduce an implementation of FLOSIC based on the minimization of E DFT‑SIC . An effective mean-field Kohn–Sham Hamiltonian, including self-interaction, is derived as a derivative of E DFT‑SIC with respect to the 1-particle density matrix, leading to a set of standard self-consistent Roothaan–Hall equations that determine the occupied orbitals and hence the density matrix.…”

Section: Introductionmentioning

confidence: 99%

Density Matrix Implementation of the Fermi–Löwdin Orbital Self-Interaction Correction Method

2023

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The Fermi−Loẅdin orbital self-interaction correction (FLOSIC) method effectively provides a transformation from canonical orbitals to localized Fermi−Loẅdin orbitals which are used to remove the self-interaction error in the Perdew−Zunger (PZ) framework. This transformation is solely determined by a set of points in space, called Fermi−Loẅdin descriptors (FODs), and the occupied canonical orbitals or the density matrix. In this work, we provide a detailed workflow for the implementation of the FLOSIC method for removal of self-interaction error in DFT calculations in an orbital-by-orbital basis that takes advantage of the unitary invariant nature of the FLOSIC method. In this way, it is possible to cast the self-consistent energy minimization at fixed FODs in the same manner than standard Kohn−Sham with one additional term in the Kohn−Sham Hamiltonian that introduces the PZ self-interaction correction. Each energy minimization iteration is divided in two substeps, one for the density matrix and one for the FODs. Expressions for the effective Kohn−Sham matrix and FOD gradients are provided such that its implementation is suitable for most electronic structure codes. We analyze the convergence characteristics of the algorithm and present applications for the evaluation of NMR shielding constants and real-time time-dependent DFT simulations based on the Liouville−von Neumann equation to calculate excitation energies.

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Implementation of Perdew–Zunger self-interaction correction in real space using Fermi–Löwdin orbitals

Cited by 13 publications

References 121 publications

Investigation of parameters affecting the high harmonic generation from monolayer WS₂

Investigation of parameters affecting the high harmonic generation from monolayer WS₂

Fermi-Löwdin orbital self-interaction correction using the optimized effective potential method within the Krieger-Li-Iafrate approximation

Density Matrix Implementation of the Fermi–Löwdin Orbital Self-Interaction Correction Method

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Implementation of Perdew–Zunger self-interaction correction in real space using Fermi–Löwdin orbitals

Cited by 13 publications

References 121 publications

Investigation of parameters affecting the high harmonic generation from monolayer WS2

Investigation of parameters affecting the high harmonic generation from monolayer WS2

Fermi-Löwdin orbital self-interaction correction using the optimized effective potential method within the Krieger-Li-Iafrate approximation

Density Matrix Implementation of the Fermi–Löwdin Orbital Self-Interaction Correction Method

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Investigation of parameters affecting the high harmonic generation from monolayer WS₂

Investigation of parameters affecting the high harmonic generation from monolayer WS₂