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Data-driven and constrained optimization of semi-local exchange and non-local correlation functionals for materials and surface chemistry

26 Jan 2022arXiv:2201.11106links table onlyarchive 2025-07-28

Kai Trepte, Johannes Voss

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Reliable predictions of surface chemical reaction energetics require an accurate description of both chemisorption and physisorption. Here, we present an empirical approach to simultaneously optimize semi-local exchange and non-local correlation of a density functional approximation to improve these energetics. A combination of reference data for solid bulk, surface, and gas-phase chemistry and physical exchange-correlation model constraints leads to the VCML-rVV10 exchange-correlation functional. Owing to the variety of training data, the applicability of VCML-rVV10 extends beyond surface chemistry simulations. It provides optimized gas phase reaction energetics and an accurate description of bulk lattice constants and elastic properties.

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