IRMOF models were taken from the Cambridge Structural Database, with Mulliken partial charges calculated using the DFTB+ software. The DFTB3 method was employed using the 3ob-3-1 parameter set. Full details of the calculations and sample input files/results are available online at 110 (). For atomistic simulations the UFF forcefield was used for all MOF linker atoms, and DREIDING forcefield parameters were used for metal node atoms, a combination that has been proven to model adsorption behaviour well. For sorbate molecules, forcefield parameters were taken from various pre-existing models after validating that TMMC could reproduce both unbiased GCMC simulation results (Figure ) and experimental bulk surface tension 115 values. A complete list of forcefield parameters and references used is provided in Table and comparison against experimental surface tension values is shown in Figure . All framework and solvent molecules were considered to be atomically rigid during this study.