Frustrated supermolecules: the high-pressure phases of crystalline methane
Using molecular dynamics based on density functional theory, this study reveals that the complex high-pressure crystal phases of methane arise from the packing of specific supermolecular clusters (icosahedral and polyhedral) where a trade-off between efficient packing and suppressed rotational entropy, driven by orientation-dependent intermolecular interactions, explains the observed non-cubic symmetries and sluggish phase transitions.