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Significance Mixtures of methane gas and water can form ice-like solid methane hydrates via homogeneous nucleation at natural, moderate conditions. Understanding the formation of the different hydrate polymorphs, required for improved control of crystallization, is hampered by limited experimental resolution. Direct molecular dynamics simulations could provide insight, but it would require computation times beyond the age of the Universe for a single nucleation event to take place. Yet, the nucleation event itself, while rare, occurs fast. Therefore, we sample and examine ensembles of rare unbiased nucleation trajectories. Detailed analysis shows how selection between competing amorphous and crystalline polymorph formation mechanisms takes place. The conclusions shed light onto the formation of clathrate hydrates.

Unbiased atomistic insight in the competing nucleation mechanisms of methane hydrates