Extending Density-Corrected Density Functional Theory to Large Molecular Systems

Abstract

Practical density-corrected density functional theory (DC-DFT) calculations rely on Hartree–Fock (HF) densities, which can be computationally expensive for systems with over a hundred atoms. We extend the applicability of HF-DFT using the dual-basis method, where the density matrix from a smaller basis set is used to estimate the HF solution on a larger basis set. Benchmarks on many systems, including the GMTKN55 database for main-group chemistry, and the L7 and S6L data sets for large molecular systems demonstrate the efficacy of our approach. We apply the dual-basis method to both DNA and HIV systems and compare with the literature. The details of a recent reparameterization of HF-r²SCAN-DC4 are explained, showing no loss of performance.