Global double hybrids do not work for charge transfer: A comment on Double hybrids and time-dependent density functional theory: An implementation and benchmark on charge transfer excited states

We comment on the results published by Ottochian et al. in J. Comput Chem. 2020, 41, 1242. Therein, the authors claim that the second-order, perturbative correlation correction applied to the time-dependent version of the PBE-QIDH global double-hybrid functional approximation (DHDFA) enables the description of charge-transfer (CT) excitations. Herein, we point out some inadvertent oversights related to what had already been previously known and achieved in the field of time-dependent DHDFAs. Exemplified for the same four systems that Ottochian et al. have used to analyze intermolecular CT excitations, we show how a systematic and unacceptably large redshift in global DHDFAs is rectified when using the latest long-range corrected DHDFAs published earlier in J. Chem. Theory Comput. 2019, 15, 4735.

Automated summary

The commentary critiques the results published by Ottochian et al. in J. Comput Chem., pointing out oversights in their research and demonstrating how these errors can be corrected by utilizing the latest long-range corrected DHDFAs.