Do Double-Hybrid Functionals Benefit from Regularization in the PT2 Term? Observations from an Extensive Benchmark

Abstract

We put to the test a recent suggestion [Shee, J., et al. <i>J. Phys. Chem. Lett.</i> <b>2021</b>, <i>12</i> (50), 12084-12097] that MP2 regularization might improve the performance of double-hybrid density functionals. Using the very large and chemically diverse GMTKN55 benchmark, we find that κ-regularization is indeed beneficial at lower percentages of Hartree-Fock exchange, especially if spin-component scaling is not applied [such as in B2GP-PLYP or ωB97M(2)]. This benefit dwindles for DSD and DOD functionals and vanishes entirely in the ∼70% HF exchange region optimal for them.