Description
The effective design of new materials for sustainable energy conversion can be facilitated by the accurate prediction of electronic properties with moderate computational complexity and cost. The self-interaction error (SIE) of Kohn-Sham density functional theory (KS-DFT) leads to a non-physical, non-linear dependence of an orbital's energy on its own fractional occupation [Dabo et al., Phys. Rev. B, 82:115121, 2010]. A generalized piecewise-linearity condition (GPWL) ensures an atomic orbital's eigenenergy is free of self-interaction. In this work, the effective potential of the Kohn-Sham equations is thereby constrained to be orbital-density dependent, with a total energy functional linear with respect to variation of its orbital densities. That is, the KS multiplicative effective potential $v_{\text{s}}[{n}]$ for an orbital $\varphi_i[{n}]$ is constrained to a functional $v_{\text{eff}}[{n - n_i}]$. The result complies with the Hohenberg-Kohn theorems. Fundamental band gaps of various semiconductor materials show an accuracy comparable to state-of-the-art many-body perturbation theory (MBPT). The result is an accurate, ab initio method with a computational cost comparable to the generalized gradient approximation (GGA) of KS-DFT.
| I am the presenting author | Yes |
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