Variational umbrella seeding for calculating nucleation barriers

In this work, we introduce variational umbrella seeding, a novel technique for computing nucleation barriers. This new method, a refinement of the original seeding approach, is far less sensitive to the choice of order parameter for measuring the size of a nucleus. Consequently, it surpasses seeding...

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Bibliographic Details
Published in:The Journal of chemical physics 2024-05, Vol.160 (17)
Main Authors: Gispen, Willem, Espinosa, Jorge R., Sanz, Eduardo, Vega, Carlos, Dijkstra, Marjolein
Format: Article
Language:English
Subjects:
Accuracy
Cavitation
Nucleation
Order parameters
Parameter sensitivity
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Summary:In this work, we introduce variational umbrella seeding, a novel technique for computing nucleation barriers. This new method, a refinement of the original seeding approach, is far less sensitive to the choice of order parameter for measuring the size of a nucleus. Consequently, it surpasses seeding in accuracy and umbrella sampling in computational speed. We test the method extensively and demonstrate excellent accuracy for crystal nucleation of nearly hard spheres and two distinct models of water: mW and TIP4P/ICE. This method can easily be extended to calculate nucleation barriers for homogeneous melting, condensation, and cavitation.
ISSN:0021-9606
1089-7690
DOI:10.1063/5.0204540