Gold-Standard Chemical Database 137 (GSCDB137): A Diverse Set of Accurate Energy Differences for Assessing and Developing Density Functionals

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, (intra- and intermolecular)
noncovalent 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 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. ωB97M-V and ωB97X-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 30% versus their hybrid analogues but demand
careful frozen-core, basis set, and spin contamination treatment.
GSCDB137 offers a comprehensive, openly documented platform for rigorous
validation of DFA and universal machine learning potentials, and training
of the next generation of exchange-correlation functionals.