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Area of Science:

  • Computational chemistry
  • Quantum mechanics
  • Electronic structure theory

Background:

  • Koopmans-compliant (KC) functionals offer accurate spectral properties via piecewise energy linearity.
  • This principle relates to electron addition/removal from molecular orbitals.

Purpose of the Study:

  • To evaluate the performance of various KC functionals.
  • To compare their accuracy for vertical ionization potentials against established methods and experiments.

Main Methods:

  • Analysis of 100 molecules from the GW100 test set.
  • Comparison of calculated vertical ionization potentials (opposite of orbital energies) with accurate quantum chemistry and experimental data.

Main Results:

  • Excellent agreement between KC functionals and reference data was observed.
  • The KIPZ functional achieved a mean absolute error of 0.20 eV for the first ionization potential.
  • This performance is state-of-the-art for density functional theory (DFT) and many-body perturbation theory.

Conclusions:

  • KC functionals demonstrate high accuracy for predicting ionization potentials.
  • KC potentials can be viewed as local, orbital-dependent approximations of the electronic self-energy, incorporating vertex corrections.