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

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

Chemical Hardness, Linear Response, and Pseudopotential Transferability

We propose a systematic method of analyzing pseudopotential transferability based on linear-response properties of the free atom, including self-consistent chemical hardness and polarizability. Our calculation of hardness extends the approach of Teter\cite{teter} not only by including self-consistency, but also by generalizing to non-diagonal hardness matrices, thereby allowing us to test for transferability to non-spherically symmetric environments. We apply the method to study the transferability of norm-conserving pseudopotentials for a variety of elements in the Periodic Table. We find that the self-consistent corrections are frequently significant, and should not be neglected. We prove that the partial-core correction improves the pseudopotential hardness of alkali metals considerably. We propose a quantity to represent the average hardness error and calculate this quantity for many representative elements as a function of pseudopotential cutoff radii. We find that the atomic polarizabilities are usually well reproduced by the norm-conserving pseudopotentials. Our results provide useful guidelines for making optimal choices in the pseudopotential generation procedure.Comment: Revtex (preprint style, 33 pages) + 9 postscript figures A version in two-column article style with embedded figures is available at http://electron.rutgers.edu/~dhv/preprints/index.html#l

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

Tailoring strain in SrTiO3 compound by low energy He+ irradiation

The ability to generate a change of the lattice parameter in a near-surface layer of a controllable thickness by ion implantation of strontium titanate is reported here using low energy He+ ions. The induced strain follows a distribution within a typical near-surface layer of 200 nm as obtained from structural analysis. Due to clamping effect from the underlying layer, only perpendicular expansion is observed. Maximum distortions up to 5-7% are obtained with no evidence of amorphisation at fluences of 1E16 He+ ions/cm2 and ion energies in the range 10-30 keV.Comment: 11 pages, 4 figures, Accepted for publication in Europhysics Letter (http://iopscience.iop.org/0295-5075

Variational finite-difference representation of the kinetic energy operator

A potential disadvantage of real-space-grid electronic structure methods is the lack of a variational principle and the concomitant increase of total energy with grid refinement. We show that the origin of this feature is the systematic underestimation of the kinetic energy by the finite difference representation of the Laplacian operator. We present an alternative representation that provides a rigorous upper bound estimate of the true kinetic energy and we illustrate its properties with a harmonic oscillator potential. For a more realistic application, we study the convergence of the total energy of bulk silicon using a real-space-grid density-functional code and employing both the conventional and the alternative representations of the kinetic energy operator.Comment: 3 pages, 3 figures, 1 table. To appear in Phys. Rev. B. Contribution for the 10th anniversary of the eprint serve