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arXiv · 2508.13468

Gold-Standard Chemical Database 137 (GSCDB137): A diverse set of accurate energy differences for assessing and developing density functionals

Jiashu Liang·Martin Head-Gordon
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Abstract

We present GSCDB137, a rigorously curated benchmark library of 137 data sets (8377 entries) covering main-group and transition-metal reaction energies and barrier heights, (intramolecular) non-covalent interactions, dipole moments, polarizabilities, electric-field response energies, and vibrational frequencies. Legacy data from GMTKN55 and MGCDB84 have been updated to today's best reference values; redundant, spin-contaminated, or low-quality points were removed, and many new, property-focused sets were added. Testing 29 popular density functional approximations (DFAs) confirms the expected Jacob's-ladder hierarchy overall but also reveals notable exceptions: functional performance for frequencies and electric-field properties correlates poorly with that for other ground-state energetics. {\omega}B97M-V and {\omega}B97X-V are the most balanced hybrid meta-GGA and hybrid GGA, respectively; B97M-V and revPBE-D4 lead the meta-GGA and GGA classes. Double hybrids lower mean errors by about 25 % versus the best hybrids but demand careful frozen-core, basis-set, and multi-reference treatment. GSCDB137 offers a comprehensive, openly documented platform for stringent DFA validation and for training the next generation of non-empirical and machine-learned functionals.

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Jiashu Liang, Martin Head-Gordon. 2025-08-19. Gold-Standard Chemical Database 137 (GSCDB137): A diverse set of accurate energy differences for assessing and developing density functionals. https://arxiv.org/abs/2508.13468

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