Nuclear magnetic
resonance (NMR) chemical shifts are a direct probe
of local atomic environments and can be used to determine the structure
of solid materials. However, the substantial computational cost required
to predict accurate chemical shifts is a key bottleneck for NMR crystallography.
We recently introduced ShiftML, a machine-learning model of chemical
shifts in molecular solids, trained on minimum-energy geometries of
materials composed of C, H, N, O, and S that provides rapid chemical
shift predictions with density functional theory (DFT) accuracy. Here,
we extend the capabilities of ShiftML to predict chemical shifts for
both finite temperature structures and more chemically diverse compounds,
while retaining the same speed and accuracy. For a benchmark set of
13 molecular solids, we find a root-mean-squared error of 0.47 ppm
with respect to experiment for
1
H shift predictions (compared
to 0.35 ppm for explicit DFT calculations), while reducing the computational
cost by over four orders of magnitude.
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