For this application, DFT-D offers a competitive balance between accuracy and cost, relative to other high accuracy ab initio methods. As alluded to before, most modern CSP workflows utilize DFT-D as a final refinement tool, making it a rational choice of 'ground truth'. Finally, calculations using DFT-D can be performed quite routinely using modern software packages. To ensure that the datasets exhibit broad chemical diversity, we generate them in two steps. First, a primary dataset is constructed by searching the CSD for experimental structures using relatively strict search criteria. These include restrictions on molecular size, molecular rigidity, and the completeness of the reported geometric data.