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Creators/Authors contains: "Wui, Jose"

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  1. Polymorphism in molecular crystals influences their properties and performance. Crystal structure prediction (CSP) can help explore the crystal structure landscape and discover potentially stable polymorphs computationally. We present a new version of the Genarris open-source code, which generates random molecular crystal structures in all space groups and applies physical constraints on intermolecular distances. The main new feature in Genarris 3.0 is the ``Rigid Press algorithm, which uses a regularized hard-sphere potential to compress the unit cell and achieve a maximally close-packed structure based on purely geometric considerations without performing any energy evaluations. In addition, Genarris 3.0 is interfaced with machine-learned interatomic potentials (MLIPs) to accelerate the exploration of the potential energy landscape. We present a new clustering and down-selection workflow that employs the MACE-OFF23(L) MLIPs to perform geometry optimization and energy ranking in the early stages. We use Genarris 3.0 to successfully predict the structure of six targets: aspirin, Target I and Target XXII from previous CSP blind tests, and the energetic materials HMX, CL-20, and DNI. We further analyze the performance of MACE-OFF23(L) compared to dispersion-inclusive density functional theory (DFT) for geometry relaxation and energy ranking. We find significant variability in the performance of MACE-OFF23(L) across chemically diverse targets with particularly poor performance for energetic materials, which is mitigated by our clustering and down-selection procedure. Genarris 3.0 can thus be used effectively to perform CSP and to generate molecular crystal datasets for training ML models. 
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    Free, publicly-accessible full text available June 30, 2026