Absence of superconductivity in iron polyhydrides at high pressures

Recently, C. M. Pépin et al. [Science 357, 382 (2017)] reported the formation of several new iron polyhydrides FeHx at pressures in the megabar range and spotted FeH5, which forms above 130 GPa, as a potential high-Tc superconductor because of an alleged layer of dense metallic hydrogen. Shortly after, two studies by A. Majumdar et al. [Phys. Rev. B 96, 201107 (2017)] and A. G. Kvashnin et al. [J. Phys. Chem. C 122, 4731 (2018)] based on ab initio Migdal-Eliashberg theory seemed to independently confirm such a conjecture. We conversely find, on the same theoretical-numerical basis, that neither FeH5 nor its precursor, FeH3, shows any conventional superconductivity and explain why this is the case. We also show that superconductivity may be attained by transition-metal polyhydrides in the FeH3 structure type by adding more electrons to partially fill one of the Fe-H hybrid bands (as, e.g., in NiH3). Critical temperatures, however, will remain low because the d-metal bonding, and not the metallic hydrogen, dominates the behavior of electrons and phonons involved in the superconducting pairing in these compounds

The road to room-temperature conventional superconductivity

It is a honor to write a contribution on this memorial for Sandro Massidda. For both of us, at different stages of our life, Sandro was first and foremost a friend. We both admired his humble, playful and profound approach to life and physics. In this contribution we describe the route which permitted to meet a long-standing challenge in solid state physics, i.e. room temperature superconductivity. In less than 20 years the Tc of conventional superconductors, which in the last century had been widely believed to be limited to 25 K, was raised from 40 K in MgB2 to 265 K in LaH10. This discovery was enabled by the development and application of computational methods for superconductors, a field in which Sandro Massidda played a major role.Comment: Viewpoint submitted for JPCM Sandro Massidda's memoria

Electron-phonon interaction in Graphite Intercalation Compounds

Motivated by the recent discovery of superconductivity in Ca- and Yb-intercalated graphite (CaC$_{6}$ and YbC$_{6}$) and from the ongoing debate on the nature and role of the interlayer state in this class of compounds, in this work we critically study the electron-phonon properties of a simple model based on primitive graphite. We show that this model captures an essential feature of the electron-phonon properties of the Graphite Intercalation Compounds (GICs), namely, the existence of a strong dormant electron-phonon interaction between interlayer and $\pi ^{\ast}$ electrons, for which we provide a simple geometrical explanation in terms of NMTO Wannier-like functions. Our findings correct the oversimplified view that nearly-free-electron states cannot interact with the surrounding lattice, and explain the empirical correlation between the filling of the interlayer band and the occurrence of superconductivity in Graphite-Intercalation Compounds.Comment: 13 pages, 12 figures, submitted to Phys. Rev.

Pair-distribution functions of the two-dimensional electron gas

Based on its known exact properties and a new set of extensive fixed-node reptation quantum Monte Carlo simulations (both with and without backflow correlations, which in this case turn out to yield negligible improvements), we propose a new analytical representation of (i) the spin-summed pair-distribution function and (ii) the spin-resolved potential energy of the ideal two-dimensional interacting electron gas for a wide range of electron densities and spin polarization, plus (iii) the spin-resolved pair-distribution function of the unpolarized gas. These formulae provide an accurate reference for quantities previously not available in analytic form, and may be relevant to semiconductor heterostructures, metal-insulator transitions and quantum dots both directly, in terms of phase diagram and spin susceptibility, and indirectly, as key ingredients for the construction of new two-dimensional spin density functionals, beyond the local approximation.Comment: 12 pages, 10 figures; misprints correcte

Electrons and phonons in the ternary alloy CaAl2−x_{2-x}Six_x} as a function of composition

We report a detailed first-principles study of the structural, electronic and vibrational properties of the superconducting C$_{32}$ phase of the ternary alloy CaAl$_{2-x}$Si$_x$, both in the experimental range $0.6 \leq x \leq 1.2$, for which the alloy has been synthesised, and in the theoretical limits of high aluminium and high silicon concentration. Our results indicate that, in the experimental range, the dependence of the electronic bands on composition is well described by a rigid-band model, which breaks down outside this range. Such a breakdown, in the (theoretical) limit of high aluminium concentration, is connected to the appearance of vibrational instabilities, and results in important differences between CaAl$_2$ and MgB$_2$. Unlike MgB$_2$, the interlayer band and the out-of-plane phonons play a major role on the stability and superconductivity of CaAlSi and related C$_{32}$ intermetallic compounds

Local-spin-density functional for multideterminant density functional theory

Based on exact limits and quantum Monte Carlo simulations, we obtain, at any density and spin polarization, an accurate estimate for the energy of a modified homogeneous electron gas where electrons repel each other only with a long-range coulombic tail. This allows us to construct an analytic local-spin-density exchange-correlation functional appropriate to new, multideterminantal versions of the density functional theory, where quantum chemistry and approximate exchange-correlation functionals are combined to optimally describe both long- and short-range electron correlations.Comment: revised version, ti appear in PR

A local density functional for the short-range part of the electron-electron interaction

Motivated by recent suggestions --to split the electron-electron interaction into a short-range part, to be treated within the density functional theory, and a long-range part, to be handled by other techniques-- we compute, with a diffusion Monte Carlo method, the ground-state energy of a uniform electron gas with a modified, short-range-only electron-electron interaction \erfc(\mu r)/r, for different values of the cutoff parameter $\mu$ and of the electron density. After deriving some exact limits, we propose an analytic representation of the correlation energy which accurately fits our Monte Carlo data and also includes, by construction, these exact limits, thus providing a reliable ``short-range local-density functional''.Comment: 7 pages, 3 figure

Correlation energy, pair-distribution functions and static structure factors of jellium

We discuss and clarify a simple and accurate interpolation scheme for the spin-resolved electron static structure factor (and corresponding pair correlation function) of the 3D unpolarized homogeneous electron gas which, along with some analytic properties of the spin-resolved pair-correlation functions, we have just published. We compare our results with the very recent spin-resolved scheme by Schmidt et al., and focus our attention on the spin-resolved correlation energies and the high-density limit of the correlation functions.Comment: 8 pages, 3 figures. Proceedings of the conference on Statistical Mechanics and Strongly Correlated Systems (Bachelet, Parisi & Vulpiani Eds.) to appear as a special issue of Physica A (Elsevier, Amsterdam 2000

Correlation energy and spin polarization in the 2D electron gas

The ground state energy of the two--dimensional uniform electron gas has been calculated with fixed--node diffusion Monte Carlo, including backflow correlations, for a wide range of electron densities as a function of spin polarization. We give a simple analytic representation of the correlation energy which fits the density and polarization dependence of the simulation data and includes several known high- and low-density limits. This parametrization provides a reliable local spin density energy functional for two-dimensional systems and an estimate for the spin susceptibility. Within the proposed model for the correlation energy, a weakly first--order polarization transition occurs shortly before Wigner crystallization as the density is lowered.Comment: Minor typos corrected, see erratum: Phys. Rev. Lett. 91, 109902(E) (2003