Traditionally, validation of our X-ray HAR analysis would be performed by comparison with experimental neutron diffraction data however our crystals were too small to conduct such a measurement. Instead we used the already conducted periodic DFT calculations as an independent validation tool. This method gives geometry parameter values comparable to those of neutron diffraction. The theoretical geometry parameters thus obtained were then compared with the geometry parameters from experimental SC-XRD refinements. For the bond length comparison, the twelve imidazolate C-H bond lengths in the asymmetric unit of ZIF-2 were averaged for each given method and basis set (Figure pVTZ). Importantly, despite being significantly computationally less demanding, the cc-pVDZ basis set shows very close agreement with cc-pVTZ, suggesting that the use of the double-zeta basis set may offer an optimal balance between structural accuracy and computational cost of the refinement. The smaller basis sets (6-31G, 6-311G) lack polarisation functions (p-functions on H atoms and d-functions on heavier atoms), which might be the reason for their poorer performance. In terms of the method choice, the HF approach appears to deviate from the DFT methods, consistent with HAR studies of molecular crystals. Finally, we performed detailed analysis of hydrogen ADPs obtained with different QMs.