Pressure-Driven Moiré Potential Enhancement and Tertiary Gap Opening in Graphene/h-BN Heterostructure.

Moiré superlattices enable engineering of correlated quantum states through tunable periodic potentials, where twist angle controls periodicity but dynamic potential strength modulation remains challenging. Here, we develop a high-pressure quantum transport technique for van der Waals heterostructures, achieving the ultimate pressure limit (∼9  GPa) in encapsulated moiré devices. In aligned graphene/h-BN, we demonstrate that pressure induces a substantial enhancement of the moiré potential strength, evidenced by the suppression of the first valence bandwidth and the near-doubling of the primary band gap. Moreover, we report the first observation of a tertiary gap emerging above 6.4 GPa, verifying theoretical predictions. Our results establish hydrostatic pressure as a universal parameter to reshape moiré band structures. By enabling quantum transport studies at previously inaccessible pressure regimes, this Letter expands the accessible parameter space for exploring correlated phases in moiré systems.