Seeking for reliable double-hybrid density functionals without fitting parameters: The PBE0-2 functional

TL;DR

The paper introduces PBE0-2, a double-hybrid density functional that does not rely on empirical fitting, achieving high accuracy and reducing common errors in density functional approximations.

Contribution

It presents a new non-empirical double-hybrid functional, PBE0-2, combining Hartree-Fock exchange and MP2 correlation with PBE, improving accuracy without fitting parameters.

Findings

PBE0-2 reduces self-interaction errors.

It outperforms traditional functionals in noncovalent interactions.

Comparable to MP2 in accuracy.

Abstract

Without the use of any empirical fitting to experimental or high-level ab initio data, we present a double-hybrid density functional approximation for the exchange-correlation energy, combining the exact Hartree-Fock exchange and second-order Moller-Plesset (MP2) correlation with the Perdew-Burke-Ernzerhof (PBE) functional. This functional, denoted as PBE0-2, is shown to be accurate for a wide range of applications, when compared with other functionals and the ab initio MP2 method. The qualitative failures of conventional density functional approximations, such as self-interaction error and noncovalent interaction error, are significantly reduced by PBE0-2.