Metal Borohydrides as high-TcT_{c} ambient pressure superconductors

The extreme pressures required to stabilize the recently discovered superhydrides represent a major obstacle to their practical application. In this paper, we propose a novel route to attain high-temperature superconductivity in hydrides at ambient pressure, by doping commercial metal borohydrides. Using first-principles calculations based on Density Functional Theory and Migdal-Eliashberg theory, we demonstrate that in Ca(BH$_4$)$_2$ a moderate hole doping of 0.03 holes per formula unit, obtained through a partial replacement of Ca with monovalent K, is sufficient to achieve $T_c$'s as high as 110 K. The high-$T_c$ arises because of the strong electron-phonon coupling between the B-H $\sigma$ molecular orbitals and bond-stretching phonons. Using a random sampling of large supercells to estimate the local effects of doping, we show that the required doping can be achieved without significant disruption of the electronic structure and at moderate energetic cost. Given the wide commercial availability of metal borohydrides, the ideas presented here can find prompt experimental confirmation. If successful, the synthesis of high-$T_c$ doped borohydrides will represent a formidable advancement towards technological exploitation of conventional superconductors.Comment: 6 pages, 5 figures, submitted to APS. Supplemental material will be available upon publicatio

HEX: High-pressure Elemental Xstals, a complete Database

This paper introduces the HEX (High-pressure Elemental Xstals) database, a complete database of the ground-state crystal structures of the first 57 elements of the periodic table, from H to La, at 0, 100, 200 and 300 GPa. HEX aims to provide a unified reference for high-pressure research, by compiling all available experimental information on elements at high pressure, and complementing it with the results of accurate evolutionary crystal structure prediction runs based on Density Functional Theory. Besides offering a much-needed reference, our work also serves as a benchmark of the accuracy of current ab-initio methods for crystal structure prediction. We find that, in 98 % of the cases in which experimental information is available, ab-initio crystal structure prediction yields structures which either coincide or are degenerate in enthalpy to within 300 K with experimental ones. The main manuscript contains synthetic tables and figures, while the Crystallographic Information File (cif) for all structures will be available on a figshare online repository when the paper will be published.Comment: 22 pages, 3 figures, 10 table

A database of high-pressure crystal structures from hydrogen to lanthanum

This paper introduces the HEX (High-pressure Elemental Xstals) database, a complete database of the ground-state crystal structures of the first 57 elements of the periodic table, from H to La, at 0, 100, 200 and 300 GPa. HEX aims to provide a unified reference for high-pressure research, by compiling all available experimental information on elements at high pressure, and complementing it with the results of accurate evolutionary crystal structure prediction runs based on Density Functional Theory. Besides offering a much-needed reference, our work also serves as a benchmark of the accuracy of current ab-initio methods for crystal structure prediction. We find that, in 98% of the cases in which experimental information is available, ab-initio crystal structure prediction yields structures which either coincide or are degenerate in enthalpy to within 300 K with experimental ones. The main manuscript contains synthetic tables and figures, while the Crystallographic Information File (cif) for all structures can be downloaded from the related figshare online repository

Absence of electron-phonon-mediated superconductivity in hydrogen-intercalated nickelates

A recent experiment [X. Ding et al., Nature (London) 615, 50 (2023)] indicates that superconductivity in nickelates is restricted to a narrow window of hydrogen concentration, 0.22 < x < 0.28 in Nd0.8Sr0.2NiO2Hx. This reported necessity of hydrogen suggests that it plays a crucial role for superconductivity, as it does in the vast field of hydride superconductors. Using density-functional theory and its extensions, we explore the effect of topotactic hydrogen on the electronic structure and phonon-mediated superconductivity in nickelate superconductors. Our calculations show that the electron-phonon coupling in hydrogen-intercalated nickelates is not strong enough to drive the electron pairing, and thus cannot explain the reported superconductivity

NbTi: a nontrivial puzzle for the conventional theory of superconductivity

We present the first $ab$-$initio$ study of superconductivity in NbTi, the workhorse for many applications. Despite its apparent simplicity, NbTi turns out to be a major challenge for computational superconductivity. In fact, anharmonic effects are crucial to obtain dynamically stable phonons for the ordered bcc phase, unstable at the harmonic level, and beyond-Morel Anderson effects in the Coulomb interaction reduce the Tc by more than 20%. Lattice disorder causes an additional large discrepancy in $T_c$ compared to experiment. Our results imply that a quantitative description of technologically-relevant superconductors requires methodological developments beyond the current standards.Comment: 6 pages, 3 figures, 1 tabl

Unconventional superconductivity without doping: infinite-layer nickelates under pressure

High-temperature unconventional superconductivity quite generically emerges from doping a strongly correlated parent compound, often (close to) an antiferromagnetic insulator. The recently developed dynamical vertex approximation is a state-of-the-art technique that has quantitatively predicted the superconducting dome of nickelates. Here, we apply it to study the effect of pressure in the infinite-layer nickelate Sr$_x$Pr$_ {1-x}$NiO$_2$. We reproduce the increase of the critical temperature ($T_c$) under pressure found in experiment up to 12 GPa. According to our results, $T_c$ can be further increased with higher pressures. Even without Sr-doping the parent compound, PrNiO$_2$, will become a high-temperature superconductor thanks to a strongly enhanced self-doping of the \nidxsqysq{} orbital under pressure. With a maximal \Tc{} of 100\,K around 100\,GPa, nickelate superconductors can reach that of the best cuprates.Comment: Main text: 6 pages, 4 figures. Supplementary information: 18 pages, 16 figure

Pb10−xCux(PO4)6O: a Mott or charge transfer insulator in need of further doping for (super)conductivity

We briefly review the status quo of research on the putative superconductor Pb9Cu(PO4)6O also known as LK-99. Further, we provide ab initio derived tight-binding parameters for a two- and five-band model, and solve these in dynamical-mean-field theory. The interaction-to-bandwidth ratio makes LK-99 a Mott or charge transfer insulator. Electron or hole doping (which is different from substituting Pb by Cu and thus differs from LK-99) is required to make it metallic and potentially superconducting