Published March 15, 2022 | Version v1
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One-shot approach for enforcing piecewise linearity on hybrid functionals: application to band-gap predictions

  • 1. Chaire de Simulation à l'Echelle Atomique, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

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Description

We present an efficient procedure for constructing nonempirical hybrid functionals to accurately predict band gaps of extended systems. We determine mixing parameters by enforcing the generalized Koopmans' condition on localized electron states, which are achieved by inserting an optimized potential probe. Application of this scheme to a large set of materials yields band gaps with a mean error of 0.30 eV with respect to experiment. Next, we consider a perturbative one-shot approach in which the single- particle eigenvalues are calculated with the wave functions obtained at the semilocal level. In this way, the computational cost is reduced by ∼85% without loss of accuracy. The scheme is found to be robust upon consideration of different defect species and functional forms.

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References

Journal reference
J. Yang, S. Falletta, A. Pasquarello, Journal of Physical Chemistry Letters, 13, 3066–3071 (2022), doi: 10.1021/acs.jpclett.2c00414

Journal reference
J. Yang, S. Falletta, A. Pasquarello, Journal of Physical Chemistry Letters, 13, 3066–3071 (2022)