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Register a new userHydrogen-induced high-temperature superconductivity in two-dimensional materials: Example of hydrogenated monolayer MgB$_2$
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Hydrogen-based compounds under ultra-high 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. We demonstrate here that the intrinsic advantages of hydrogen for phonon-mediated superconductivity can be exploited in a completely different system, namely two-dimensional (2D) materials. We find that hydrogen adatoms can strongly enhance superconductivity in 2D materials due to flatband states originating from atomic-like hydrogen orbitals, with a resulting high density of states, and due to the emergence of high-frequency hydrogen-related phonon modes that boost the electron-phonon coupling. As a concrete example, we investigate 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 the coupling between them. 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.
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According to the crystal structure of MgB$_{2}$ and band structure calculations quasi-two-dimensional (2D) boron planes are responsible for the superconductivity. We report on critical fields and resistance measurements of 30 nm thick MgB$_{2}$ films grown on MgO single crystalline substrate. A linear temperature dependence of the parallel and perpendicular upper critical fields indicate a 3D-like penetration of magnetic field into the sample. Resistivity measurements, in contrast, yield a temperature dependence of fluctuation conductivity above T$_{c}$ which agrees with the Aslamazov-Larkin theory of fluctuations in 2D superconductors. We consider this finding as an experimental evidence of two-dimensional nucleation of superconductivity in MgB$_{2}$.
Starting from first principles, we show the formation and evolution of superconducting gaps in MgB$_2$ at its ultrathin limit. Atomically thin MgB$_2$ is distinctly different from bulk MgB$_2$ in that surface states become comparable in electronic density to the bulk-like $sigma$- and $pi$-bands. Combining the ab initio electron-phonon coupling with the anisotropic Eliashberg equations, we show that monolayer MgB$_2$ develops three distinct superconducting gaps, on completely separate parts of the Fermi surface due to the emergent surface contribution. These gaps hybridize nontrivially with every extra monolayer added to the film, owing to the opening of additional coupling channels. Furthermore, we reveal that the three-gap superconductivity in monolayer MgB$_2$ is robust over the entire temperature range that stretches up to a considerably high critical temperature of 20 K. The latter can be boosted to $>$50 K under biaxial tensile strain of $sim$ 4%, which is an enhancement stronger than in any other graphene-related superconductor known to date.
The magnetic field dependent critical current density $j_c(B)$ of a MgB$_2$ bulk sample has been obtained by means of magnetization hysteresis measurements. The $j_c(B)$ curves at different temperatures demonstrate a crossover from single vortex pinning to small-bundle vortex pinning, when the field is larger than the crossover field $B_{sb}$. The temperature dependence of the crossover field $B_{sb}(T)$ is in agreement with a model of randomly distributed weak pinning centers via the spatial fluctuations of the transition temperature ($delta T_c$-pinning), while pinning due to the mean free path fluctuations ($delta l$-pinning) is not observed.
Insight into why superconductivity in pristine and doped monolayer graphene seems strongly suppressed has been central for the recent years various creative approaches to realize superconductivity in graphene and graphene-like systems. We provide further insight by studying electron-phonon coupling and superconductivity in doped monolayer graphene and hexagonal boron nitride based on intrinsic phonon modes. Solving the graphene gap equation using a detailed model for the effective attraction based on electron tight binding and phonon force constant models, the various system parameters can be tuned at will. Consistent with results in the literature, we find slight gap modulations along the Fermi surface, and the high energy phonon modes are shown to be the most significant for the superconductivity instability. The Coulomb interaction plays a major role in suppressing superconductivity at realistic dopings. Motivated by the direct onset of a large density of states at the Fermi surface for small charge dopings in hexagonal boron nitride, we also calculate the dimensionless electron-phonon coupling strength there, but the comparatively large density of states cannot immediately be capitalized on, and the charge doping necessary to obtain significant electron-phonon coupling is similar to the value in graphene.
Despite growing interest in them, highly crystalline two-dimensional superconductors derived from exfoliated layered materials are few. Employing the anisotropic Migdal-Eliashberg formalism based on {it ab initio} calculations, we find monolayer NiTe$_{2}$ to be an intrinsic superconductor with a $T_{text c}sim$5.7~K, although the bulk crystal is not known to superconduct. Remarkably, bilayer NiTe$_{2}$ intercalated with lithium is found to display two-gap superconductivity with a critical temperature $T_{text{c}}sim 11.3$~K and superconducting gap of $sim$3.1~meV, arising from a synergy of electronic and phononic effects. The comparatively high $T_text{c}$, substrate independence and proximity tunability will make these superconductors ideal platforms for exploring intriguing correlation effects and quantum criticality associated two-dimensional superconductivity.
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