The Supporting inforation contains: Figure reporting a representative coupling pattern between marginals, Analysis of the numerical error associated with inversion, Description of the whitening approach, potential energy overlaps obtained during training, qualitative comparison of configurations generated by PGM and MD simulation, convergence of the ECM calculations and spacing of the λ replicas, table summary of the absolute FE of every supercell. M.S. acknowledges funding from the Crystallization in the Real World EPSRC Programme Grant (EP/R018820/1) and from the ht-MATTER UKRI Frontier Research Guarantee Grant (EP/X033139/1). M.R.S acknowledges support from the National Science Foundation under grant no. CHE-2331939. AbbVie sponsored and partially funded the study, contributed to the design, and participated in the collection, analysis, and interpretation of data and in writing, reviewing, and approval of the final publication. A.Y.S., N.M., and Y.M.L. are employees of AbbVie and may own AbbVie stock.