Unbiased atomistic insight in the competing nucleation mechanisms of methane hydrates.

ABSTRACT: Methane hydrates have important industrial and climate implications, yet their formation via homogeneous nucleation under natural, moderate conditions is poorly understood. Obtaining such understanding could lead to improved control of crystallization, as well as insight into polymorph selection in general, but is hampered by limited experimental resolution. Direct molecular dynamics simulations using atomistic force fields could provide such insight, but are not feasible for moderate undercooling, due to the rare event nature of nucleation. Instead, we harvest ensembles of the rare unbiased nucleation trajectories by employing transition path sampling. We find that with decreasing undercooling the mechanism shifts from amorphous to crystalline polymorph formation. At intermediate temperat

SUBMITTER: Arjun 

PROVIDER: S-EPMC6765301 | biostudies-literature | 2019 Sep

REPOSITORIES: biostudies-literature