Multiscale Interfacial Structure and Organization of sII Gas Hydrate Interfaces Using Molecular Dynamics

Gas hydrate systems display complex structural arrangements in their bulk and interfacial configurations. Controlling nucleation and growth in the context of potential applications requires a characterization of these structures such that they can be manipulated at the atomic and molecular scale to fine tune macroscale applications. This work uses molecular dynamics to show the different methods of identifying interface location and thickness, the drawbacks of certain methods, and proposes improved methodology to overcome sampling issues. We characterize the interfacial position and thickness using structure and dipole-based methods at different conditions for water/sII natural gas hydrate mixtures. We find that phases with similar densities are particularly sensitive to the regression technique employed and may not resolve the thickness of the complex pre-melting layer adequately, while the dipole moments may provide better resolution. The dipole shows the complex natural of the small and compressed layer that presents on the hydrate surface. These results show that the interface is thin but dynamic and careful characterization required analysis of multiple molecular phenomena.