Vibron Softening of Solid Hydrogen under Nanoconfinement

The vibron behavior of hydrogen bears significant importance for understanding the phases of solid hydrogen under high pressure. In this work, we reveal an unusual high-pressure behavior of hydrogen confined within nanopores through a combination of experimental measurements and theoretical calculations. The nanoconfined hydrogen molecules retain an hcp lattice up to 170 GPa, yet significant deviations from the vibrational characteristics of bulk hydrogen are observed in the primary vibrons of both Raman and infrared spectra. This lowered vibron peak is linked to the disorder of the hydrogen molecules with longer bonds and enhanced intermolecular interactions at the interface. Further investigation reveals that this nanoscale confinement leads to a considerable decrease in the band gap of solid hydrogen, potentially facilitating band gap closure at considerably lower pressures. Our findings provide crucial insights into the behavior of solid hydrogen under spatial nanoconfinement, paving the way for novel explorations into hydrogen metallization.