13 pages, 8 figures. A new appendix "Conventional approach" has been included, detailing the Bardeen-Pines approach, alpha^2F(omega), lambda, mu, mu* and Tc calculated with the McMillan expression
Superconductivity, the lossless flow of electric current, occurs typically at very low temperatures. A possible exception is highly pressurized hydrogen, for which room temperature superconductivity has been predicted. However, as a result of various approximations used, conflicting theoretical predictions exist for the temperatures where superconductivity is expected to occur in highly pressurized hydrogen. Here we avoid those approximations and exploit the ``jellium'' model proposed in 1966 by De Gennes, where superconductivity involves the combination of Coulomb repulsion between the electrons and Coulomb attraction between the protons and the electrons. We confirm that metallic hydrogen should indeed exhibit superconductivity, but this is limited to temperatures far below previous estimates. We also find that the superconducting order develops over an energy range significantly exceeding the characteristic phonon energy, and that the phase of the order parameter flips 180 degrees at the characteristic phonon energy above and below the Fermi energy.
Two-dimensional transition metal carbides and nitrides (MXenes) are an emerging class of atomically-thin superconductors, whose characteristics are highly prone to tailoring by surface functionalization. Here we explore the use of hydrogen adatoms to enhance phonon-mediated superconductivity in MXenes, based on first-principles calculations combined with Eliashberg theory. We first demonstrate the stability of three different structural models of hydrogenated Mo- and W-based MXenes. Particularly high critical temperatures of over 30 K are obtained for hydrogenated Mo$_2$N and W$_2$N. Several m…
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 d…
Unique to certain unconventional superconductors is the coexistence of magnetism and superconductivity. We have previously found ferromagnetism and superconductivity in hydrogenated graphitic materials. Herein we present similar as well as completely new findings this time applicable to hydrogenated graphite foils. As the strength of the magnetic field is increased, the temperature-dependent magnetization shows several important transitions. From a Neel paramagnetic-antiferromagnetic transition, to a ferromagnetic superconductor state, to an orbital paramagnetic glass high-temperature supercon…
High-critical-temperature (Tc) superconductivity at 48 K is reported for hydrogen-doped SmFeAsO epitaxial films on MgO single-crystal substrates. The key processes are pulsed laser deposition to grow undoped SmFeAsO epitaxial films and subsequent topotactic chemical reaction using CaH2 powders under evacuated silica-glass ampule atmosphere. Based on this post-deposition thermal annealing treatment that we have developed, a maximum hydrogen concentration x = ~0.35 was realized in SmFeAs(O1-xHx). Disordered hydrogen-substitution at O sites is experimentally confirmed directly by atomic-scale mic…
Superconductive H3S synthesized from H2S is very poorly crystallized, and has excess sulfur as impurity (3H2S -> 2H3S + S). The phase transition process undergoes in sulfur excess condition, which might cause hydrogen deficiency. The influence of hydrogen deficiency is not clear. Therefore investigation on the superconductivity in H3S with no hydrogen deficiency is demanded. Two groups performed synthesis of H3S from elemental sulfur and hydrogen (direct synthesis) and their results have shown that no hydrogen deficiency is caused when the direct synthesis is performed under hydrogen excessive…
We present detailed studies of the superconductivity in high-pressure H3S. X-ray diffraction measurements show that cubic Im-3m H3S was synthesized from elemental sulfur and hydrogen donor ammonia borane (NH3BH3). Our electrical transport measurements confirm superconductivity with a transition temperature Tc = 197 K at 153 GPa. From the analysis of both the normal state resistivity and the slope of the critical field, we conclude that the superconductivity is described by clean-limit behaviour. A significant broadening of the resistive transition in finite magnetic field is found, as expected…
We have shown that adiabatic electronic structure of superconducting phase of sulphur hydride at 200 GPa is unstable toward vibration motion of H-atoms. Theoretical study indicates that in coupling to H-vibrations, system undergoes transition from adiabatic into stabilised anti-adiabatic multi-gap superconducting state at temperature which can reach 203 K.
We investigate the role of specific phonon mode symmetries for the room temperature superconductivity in atomic hydrogen under large pressure. Using anisotropic Migdal-Eliashberg theory with ab initio input from density functional theory, we show that the $E_u$ phonon modes are the dominant driving force for obtaining such high critical temperatures. When going from 400 to 600 GPa, we find an increased transition temperature, however, the total electron-phonon coupling strength is counterintuitively reduced. Our analysis reveals that this is due to an enhanced contribution to the coupling stre…
The recently synthesized hydrogen boride monolayer in the Cmmm phase is a promising super-conductor due to its similarity to MgB2 and the large hydrogen content in its structure. Making use of first-principles calculations based on density functional theory, we study its electronic, vibrational,and superconducting properties and conclude that, despite the expectations, hydrogen boride does not have a sizable superconducting critical temperature. The presence of hydrogen in the system alters the boron-boron bonding, weakening the electron-phonon interaction. We have studied the effect of enhanc…
In a short review-article we first discuss the results, which are mainly devoted to the generalizations of the famous Kohn-Luttinger mechanism of superconductivity in purely repulsive fermion systems at low electron densities. In the context of repulsive-U Hubbard model and Shubin-Vonsovsky model we consider briefly the superconducting phase diagrams and the symmetries of the order parameter in novel strongly correlated electron systems including idealized monolayer and bilayer graphene. We stress that purely repulsive fermion systems are mainly the subject of unconventional low-temperature su…
Roles of paramagnetic and diamagnetic pair-breaking effects in superconductivity in electric-field-induced surface metallic state are studied by Bogoliubov-de Gennes equation, when magnetic fields are applied parallel to the surface. The multi-gap states of sub-bands are related to the depth dependence and the magnetic field dependence of superconductivity. In the Fermi-energy density of states and the spin density, sub-band contributions successively appear from higher-level sub-bands with increasing magnetic fields. The characteristic magnetic field dependence may be a key feature to identif…
Room temperature superconductivity has been achieved under high pressure in an organically derived carbonaceous sulfur hydride with a critical superconducting transition temperature (Tc) of 288 kelvin. This development is part of a new class of dense, hydrogen rich materials with remarkably high critical temperatures. Metal superhydrides are a subclass of these materials that provide a different and potentially more promising route to very high Tc superconductivity. The most promising binary metal superhydrides contain alkaline or rare earth elements, and recent experimental observations of La…
Hydrogen-rich superhydrides are promising high-Tc superconductors, with superconductivity experimentally observed near room temperature, as shown in recently discovered lanthanide superhydrides at very high pressures, e.g. LaH10 at 170 GPa and CeH9 at 150 GPa. Superconductivity is believed to be closely related with the high vibrational modes of the bound hydrogen ions. Here we study the limit of extreme pressures (above 200 GPa) where lanthanide hydrides with large hydrogen content have been reported. We focus on LaH16 and CeH16, two prototype candidates for achieving a large electronic contr…
Electrons confined to two dimensions display an unexpected diversity of behaviors as they are cooled to absolute zero. Noninteracting electrons are predicted to eventually "localize" into an insulating ground state, and it has long been supposed that electron correlations stabilize only one other phase: superconductivity. However, many two-dimensional (2D) superconducting materials have shown surprising evidence for metallic behavior, where the electrical resistivity saturates in the zero-temperature limit, the nature of this unexpected metallic state remains under intense scrutiny. We report …
The first-principle method of mathematical modeling was used to calculate the structural, electronic, phonon, and other characteristics of the normal metallic phase of hydrogen at a pressure of 500 GPa. It has been shown that metal hydrogen having a lattice symmetry I41 / AMD cell is a stable phase under a high pressure hydrostatic compression. The resulting structure is a locally stable one with respect to the phonon spectrum.
We present a new technique for measuring the critical temperature Tc in the high pressure, high Tc electron-phonon-driven superconducting hydrides. This technique does not require connecting leads to the sample. In the multiphonon region of the absorption spectrum, the reflectance mirrors the temperature variation of the superconducting order parameter. For an appropriately chosen value of photon energy of order twice the gap plus 1.5 times the maximum phonon energy, the temperature dependence of the reflectance varies much more rapidly below T=Tc than above. It increases with increasing tempe…
The method of mathematical modeling was used for the calculation of the structural, electronic, phonon, and other characteristics of various normal phases of phosphorus hydrides with stoichiometry PHk. It was shown that the di-phosphine may form 2D lattice of the metallic hydrogen, stabilized by phosphorus atoms under high hydrostatic compressive pressure. The resulting structure with the elements of H-P-H is a locally stable one in the phonon spectrum (or metastable). The properties of di-phosphine with the properties of similar structures such as thesulphur hydrides were compared.
We report the observation of conventional superconductivity at the highest temperature yet attained without mechanical compression, around 54 kelvin in palladium-hydride and 60 kelvin in palladium-deuteride. The remarkable increase in Tc compared to the previously known value was achieved by rapidly cooling the hydride and deuteride after loading with hydrogen or deuterium at elevated temperature. Our results encourage hope that conventional superconductivity under ambient conditions will be discovered in materials with very high hydrogen density, as predicted more than a decade ago.
Superconductivity and short range order in metallic glasses Fe$_{x}$Ni$_{1-x}$Zr$_{2}$
在非晶超导体中，超导和涡旋钉扎特性与长程序的缺乏密切相关。因此，超导性和涡旋相的研究可以探测潜在的微观结构和材料的秩序。这是从电阻和局部磁化测量在超导状态下的Fe $_{x}$ Ni $_{1-x}$ Zr $_{2}$金属玻璃与$0\leq x \leq 0.6$。首先，我们介绍了典型的超导性能，如临界温度和磁场，以及它们与铁含量的依赖关系。然后，观察到的特殊的顺时针磁滞回线，宽的双阶跃转变和大的磁化强度波动含有大量的Fe的玻璃进行了分析，揭示了在短程有序与Fe含量的变化。
Hydrogen compounds are peculiar as the quantum nature of the proton can crucially affect their structural and physical properties. A remarkable example are the high-pressure phases of H$_2$O, where quantum proton fluctuations favor the symmetrization of the H bond and lower by 30 GPa the boundary between the asymmetric structure and the symmetric one. Here we show that an analogous quantum symmetrization occurs in the recently discovered sulfur hydride superconductor with the record superconducting critical temperature $T_c=203$ K at 155 GPa. In this system, according to classical theory, supe…
The uniquely characteristic macrostructures of binary hydrogen-clathrate compounds $M$H$_\textrm{n}$ formed at high pressure, a cage of hydrogens surrounding a central-atom host, is theoretically predicted in various studies to include structurally stable phonon-mediated superconductors. High superconductive transition temperatures $T$$_\textrm{C}$ have thus far been measured for syntheses with $M$ = La, Y, and Th. In compressed LaH$_\textrm{10}$, independent studies report $T$$_\textrm{C}$ of 250 K and over 260 K, a maximum in $T$$_\textrm{C}$ with pressure $P$, and normal-state resistance sc…
We present a first-principles implementation of the stochastic path-integral approach proposed by Liu et al. [H. Liu, Y. Yuan, D. Liu, X.-Z. Li, and J. Shi, Phys. Rev. Research 2, 013340 (2020)] for estimating the superconducting transition temperature ($T_c$) of a liquid. The implementation is based on the all-electron projector-augmented-wave (PAW) method. We generalize Liu et al.'s formalism to accommodate the pseudo-description of electron states in the PAW method. A formula for constructing the overlap operator of the PAW method is proposed to eliminate errors due to the incompleteness of…
The electron and phonon spectra, as well as the density of electron and phonon states of the stable orthorhombic structure of hydrogen sulfide (SH2) at pressures 100-180 GPa have been calculated. It is found that the set of parallel planes of hydrogen atoms is formed at pressure ~175 GPa as a result of structural changes in the unit cell of the crystal under pressure. There should be complete concentration of hydrogen atoms in these planes. As a result the electron properties of the system acquire a quasi-two-dimensional character. The features of in phase and antiphase oscillations of hydroge…
Recently BCS superconductivity at 203 K has been discovery in a highly compressed hydrogen sulfide. We use first-principles calculations to systematically examine the effects of partially substituting the chalcogen atoms on the superconductivity of hydrogen chalcogenides under high pressures. We find detailed trends of how the critical temperature changes with increasing the V-, VI- or VII-substitution rate, which highlight the key roles played by low atomic mass and by strong covalent metallicity. In particular, a possible record high critical temperature of 280 K is predicted in a stable H3S…
Lately, there has been much interest in high temperature superconductors, and more recently hydrogen-based superconductors. This work offers a simple model which explains the behavior of the superconducting gap based on BCS theory, and reproduces most effects seen in experiments, including the isotope effect and T_c enhancement as a function of pressure. We show that this is due to a combination of the factors appearing in the gap equation: the matrix element between the proton states, and the level splitting of the proton.
We have systematically searched for the ground state structures of bismuth hydrides based on evolutionary algorithm method and particle swarm optimization algorithm method. Given only rich-hydrogen region, except for BiH$_{3}$, other hydrides (BiH, BiH$_{2}$, BiH$_{4}$, BiH$_{5}$, BiH$_{6}$) have been predicted to be stable with pressurization. With the increase of hydrogen content, hydrogen exists in bismuth hydrides with the different forms and presents the characteristics of ionicity. Under high pressure, the remarkable structural feature is the emergence of H$_{2}$ units in BiH$_{2}$, BiH$…
Making use of first-principles calculations, we analyze the effect of quantum ionic fluctuations and lattice anharmonicity on the crystal structure and superconductivity of P63/mmc ScH6 in the 100-160 GPa pressure range within the stochastic self-consistent harmonic approximation. We predict a strong correction to the crystal structure, the phonon spectra, and the superconducting critical temperatures, which have been estimated in previous calculations without considering ionic fluctuations on the crystal structure and assuming the harmonic approximation for the lattice dynamics. Quantum ionic…
Superconducting layered transition metal dichalcogenides (TMDs) stand out among other superconductors due to the tunable nature of the superconducting transition, coexistence with other collective electronic excitations (charge density waves) and strong intrinsic spin-orbit coupling. Molybdenum disulphide (MoS2) is the most studied representative of this family of materials, especially since the recent demonstration of the possibility to tune its critical temperature, Tc, by electric-field doping. However, just one of its polymorphs, band-insulator 2H-MoS2, has so far been explored for its pot…
Light-element compounds hold great promise of high critical temperature superconductivity judging from the theoretical perspective. Hydrogen-rich material, benzene, is such a kind of candidate but also an organic compound. A series of first-principles calculations are performed on the electronic structures, dynamics properties, and electron-phonon interactions of solid benzene at high pressures. Benzene is found to be dynamically stable in the pressure range of 180 - 200 GPa and to exhibit superconductivity with a maximum transition temperature of 20 K at 195 GPa. The phonon modes of carbon at…
The 1111-type iron-based superconductor LnFeAsO1-xFx (Ln stands for lanthanide) is the first material with a Tc above 50 K, other than cuprate superconductors. Electron doping into LaFeAsO by H, rather than F, revealed a double-dome-shaped Tc-x diagram, with a first dome (SC1, 0.05<x<0.20) and a second dome (SC2, 0.2<x<0.5). Here, we report the Tc for the whole hydrogen-doping range in LaFeAsO1-xHx under pressures of up to 19 GPa. Tc rises to 52 K at 6 GPa for the Tc-valley composition between the two Tc domes. This is the first instance of the Tc exceeding 50 K in La-1111-type iron-based supe…
A possibility of high, room-temperature superconductivity was predicted for metallic hydrogen in the 1960s. However, metallization and superconductivity of hydrogen are yet to be unambiguously demonstrated in the laboratory and may require pressures as high as 5 million atmospheres. Rare earth based "superhydrides" such as LaH10 can be considered a close approximation of metallic hydrogen even though they form at moderately lower pressures. In superhydrides the predominance of H-H metallic bonds and high superconducting transition temperatures bear the hallmarks of metallic hydrogen. Still, ex…
A mechanism of superconductivity is proposed for the Kondo lattice which has semi-metallic conduction bands with electron and hole Fermi surfaces. At high temperatures, the $f$ electron's localized spins/pseudospins are fluctuating between electron and hole Fermi surfaces to seek for a partner to couple with. This system tries to resolve this frustration at low temperatures and chooses to construct a quantum mechanically entangled state composed of the Kondo singlet with electron surface and that with hole surface, to break the U(1) gauge symmetry. The corresponding order parameter is given by…
The recently synthesized air-insensitive hydrogen doped KCr$_3$As$_3$ superconductor has aroused great research interests. This material has, for the first time in the research area of the quasi-one-dimensional Cr-based superconductivity (SC), realized a tunability through charge doping, which will potentially significantly push the development of this area. Here based on the band structure from first-principle calculations, we construct a six-band tight-binding (TB) model equipped with multi-orbital Hubbard interactions, and adopt the random-phase-approximation approach to study the hydrogen-…
