Pressure predictions at each training state point are within error of the DFT-predicted value (see Supplementary Information Figure ) , while C/N crystal cold compression curves exhibits absolute percent differences ranging from 0.1 to 1.7% (see Supplementary Information Table ). Diffusion coefficients are also in good agreement with DFT (See Supplementary Figure ), though ChIMES models underpredict these values for the two graphitic structures comprising cases 1 and 2. This disagreement is due to use of r cut,out  5, which precludes recovery of the low-lying dispersion forces that modulate inter-sheet interactions, but greatly reduces the model's computational expense. Ongoing work is exploring overcoming this limitation by explicitly including D2 corrections in the ChIMES model. Radial pair distribution functions (RDFs) and vibrational power spectra for simulations using the Hierarch model are provided in Figure . In general, we find excellent agreement with DFT, despite the diversity of structure, chemistry, and bonding across the investigated state points.