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arXiv · 2408.13813

Modified Opposite-Spin-Scaled Double-Hybrid Functionals

Golokesh Santra·Markus Bursch·Lukas Wittmann
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Abstract

We investigate the potential performance improvements of double-hybrid density functionals by replacing the standard opposite-spin-scaled MP2 (SOS-MP2) with the modified opposite-spin-scaled MP2 (MOS-MP2) in the nonlocal correlation component. Using the large and diverse GMTKN55 dataset, we find that MOS-double hybrids provide significantly better accuracy compared to SOS-MP2-based double hybrids when empirical dispersion correction is not employed. The non-covalent interaction subsets account for the majority of this improvement. Adding the DFT-D4 dispersion correction to MOS-type double hybrids does not provide any superior performance over conventional dispersion-corrected SOS-MP2-based double hybrids. Nevertheless, for nine tested transition metal sets, dispersion-corrected spin-component-scaled (SCS) double hybrids are still significantly better than any MOS-double hybrid functional.

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Golokesh Santra, Markus Bursch, Lukas Wittmann. 2024-08-25. Modified Opposite-Spin-Scaled Double-Hybrid Functionals. https://arxiv.org/abs/2408.13813

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