Hydrogen-Induced High-Temperature Superconductivity in Two-Dimensional Materials: The Example of Hydrogenated Monolayer MgB_{2}.

Hydrogen-based compounds under ultrahigh pressure, such as the polyhydrides H_{3}S and LaH_{10}, superconduct through the conventional electron-phonon coupling mechanism to attain the record critical temperatures known to date. Here we exploit the intrinsic advantages of hydrogen to strongly enhance phonon-mediated superconductivity in a completely different system, namely, a two-dimensional material with hydrogen adatoms. We find that van Hove singularities in the electronic structure, originating from atomiclike hydrogen states, lead to a strong increase of the electronic density of states at the Fermi level, and thus of the electron-phonon coupling. Additionally, the emergence of high-frequency hydrogen-related phonon modes in this system boosts the electron-phonon coupling further. As a concrete example, we demonstrate the effect of hydrogen adatoms on the superconducting properties of monolayer MgB_{2}, by solving the fully anisotropic Eliashberg equations, in conjunction with a first-principles description of the electronic and vibrational states, and their coupling. We show that hydrogenation leads to a high critical temperature of 67 K, which can be boosted to over 100 K by biaxial tensile strain.

Free surfaces recast superconductivity in few-monolayer MgB2: Combined first-principles and ARPES demonstration.

Two-dimensional materials are known to harbour properties very different from those of their bulk counterparts. Recent years have seen the rise of atomically thin superconductors, with a caveat that superconductivity is strongly depleted unless enhanced by specific substrates, intercalants or adatoms. Surprisingly, the role in superconductivity of electronic states originating from simple free surfaces of two-dimensional materials has remained elusive to date. Here, based on first-principles calculations, anisotropic Eliashberg theory, and angle-resolved photoemission spectroscopy (ARPES), we show that surface states in few-monolayer MgB2 make a major contribution to the superconducting gap spectrum and density of states, clearly distinct from the widely known, bulk-like σ- and π-gaps. As a proof of principle, we predict and measure the gap opening on the magnesium-based surface band up to a critical temperature as high as ~30 K for merely six monolayers thick MgB2. These findings establish free surfaces as an unavoidable ingredient in understanding and further tailoring of superconductivity in atomically thin materials.