A low-symmetry ground state of dense two-dimensional hydrogen

Abstract

Hydrogen under pressure is an extremely complex system featuring molecular dissociation, metallization, and anomalous melting. While bulk hydrogen has been studied for nearly a century, its two-dimensional counterpart remains unexplored. Using first-principles structural searches and relaxations in supercells containing up to 512 atoms, we identify ground-state structures of dense two-dimensional hydrogen showing no evidence of long-range crystalline order over the simulated length scales. Within density functional theory, these structures have lower enthalpy than all crystalline candidates considered over an intermediate pressure interval between molecular and atomic crystals. This preference already emerges with classical nuclei and persists as the supercell size increases, while the dominant structure-factor peaks grow substantially more slowly than in the crystalline reference phases. Although crystals with very large primitive cells cannot be rigorously excluded, these findings support the possibility of a disordered ground state and identify dense two-dimensional hydrogen as a promising setting for investigating competition between crystallization and structural disorder.