Koopmans Spectral Functionals in Periodic Boundary Conditions.

@article{Colonna2022KoopmansSF,
  title={Koopmans Spectral Functionals in Periodic Boundary Conditions.},
  author={Nicola Colonna and Riccardo De Gennaro and Edward B. Linscott and Nicola Marzari},
  journal={Journal of chemical theory and computation},
  year={2022}
}
Koopmans spectral functionals aim to describe simultaneously ground-state properties and charged excitations of atoms, molecules, nanostructures, and periodic crystals. This is achieved by augmenting standard density functionals with simple but physically motivated orbital-density-dependent corrections. These corrections act on a set of localized orbitals that, in periodic systems, resemble maximally localized Wannier functions. At variance with the original, direct supercell implementation… 

Figures and Tables from this paper

References

SHOWING 1-10 OF 125 REFERENCES

Koopmans-Compliant Spectral Functionals for Extended Systems

Koopmans-compliant functionals have been shown to provide accurate spectral properties for molecular systems; this accuracy is driven by the generalized linearization condition imposed on each

Bloch's theorem in orbital-density-dependent functionals: Band structures from Koopmans spectral functionals

Koopmans-compliant functionals provide a novel orbital-density-dependent framework for an accurate evaluation of spectral properties; they are obtained by imposing a generalized piecewise-linearity

Koopmans Meets Bethe-Salpeter: Excitonic Optical Spectra without GW.

TLDR
Conveniently, the new framework reduces the parameter space controlling the accuracy of the calculation, thereby simplifying the simulation of charge-neutral excitations, offering the potential to expand the applicability of first-principles spectroscopies to larger systems of applied interest.

Improved band gaps and structural properties from Wannier–Fermi–Löwdin self-interaction corrections for periodic systems

TLDR
This work presents a new formulation and implementation of Wannier function-derived Fermi-Löwdin (WFL) orbitals for correcting the SIE in periodic systems and shows that the WFL self-interaction correction approach gives better band gaps and bulk moduli compared to semilocal functionals.

Screening in Orbital-Density-Dependent Functionals.

TLDR
The role of Koopmans-compliant functionals are reiterated as simple and accurate quasiparticle approximations to the exact spectral functional, bypassing diagrammatic expansions and relying only on the physics of the local density or generalized-gradient approximation.

Performance and Self-Consistency of the Generalized Dielectric Dependent Hybrid Functional.

TLDR
This work analyzes the performance of the recently proposed screened exchange constant functional (SX) on the GW100 test set, and discusses results obtained at different levels of self-consistency, and finds excellent agreement, on par with recent state of the art methods based on many body perturbation theory.

First-principles photoemission spectroscopy and orbital tomography in molecules from koopmans-compliant functionals.

TLDR
Koopmans-compliant functionals, constructed to enforce piecewise linearity and the correct discontinuity derivative in energy functionals with respect to fractional occupation, provide molecular photoemission spectra and momentum maps of Dyson orbitals that are in excellent agreement with experimental ultraviolet photoemissions spectroscopy and orbital tomography data.

Koopmans-Compliant Functionals and Potentials and Their Application to the GW100 Test Set.

TLDR
It is argued that KC potentials can be considered as local and orbital-dependent approximations to the electronic self-energy, already including approximate vertex corrections.

Koopmans-compliant functionals and their performance against reference molecular data

Koopmans-compliant functionals emerge naturally from extending the constraint of piecewise linearity of the total energy as a function of the number of electrons to each fractional orbital

Curvature and Frontier Orbital Energies in Density Functional Theory.

TLDR
It is shown that optimally tuned range-separated hybrid functionals can inherently minimize both DD and curvature, thus requiring no correction, and that this can be used as a sound theoretical basis for novel tuning strategies.
...