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The search for room temperature superconductivity has accelerated dramatically in the last few years driven largely by theoretical predictions that first indicated alloying dense hydrogen with other elements could produce conventional phonon-mediated superconductivity at very high temperatures and at accessible pressures, and more recently, with the success of structure search methods that have identified specific candidates and pressure-temperature (P-T) conditions for synthesis. These theoretical advances have prompted improvements in experimental techniques to test these predictions. As a result, experimental studies of simple binary hydrides under pressure have yielded high critical superconducting transition temperatures (Tc), of 260 K in LaH10, close to the commonly accepted threshold for room temperature, 293 K, at pressures near 180 GPa. We successfully synthesized a metallic La-based superhydride from La metal and ammonia borane, NH3BH3, and find a multi-step transition with a Tc of 294 K for the highest onset. When subjected to subsequent thermal excursions to higher temperatures that promoted a chemical reaction to what we believe is a ternary or higher order system, the transition temperature was driven to higher temperatures. Although the reaction does not appear to be complete, the onset temperature was pushed from 294 K to 556 K before the experiments had to be terminated. The results provide evidence for hot superconductivity well above room temperature, in line with recent predictions for a higher order hydride under pressure., Comment: 30 pages including 6 figures ( with 2 side by side figures)

Topological semimetals generally contain heavy elements. Using density-functional theoretic calculations, we predict that three dense lithium polymorphs in the pressure range 200--360 GPa display nontrivial semimetallic electronic structure. Specifically, these high-pressure phases exhibit Fermi pockets which are degenerate over a loop in $\boldsymbol{k}$-space, around which an encircling $\bm k$-space path is threaded by $\pm \pi$ Berry phase. Accordingly, these dense lithium phases are topological nodal loop semimetals involving a single light element., Comment: 6 pages,6 figures

We suggest, and demonstrate, a systematic approach to the study of cuprate superconductors, namely, progressive change of ion size in order to systematically alter the interaction strength and other key parameters. R(Ba,Sr)$_2$Cu$_3$O$_y$ (R={La, ... Lu,Y}) is such a system where potentially obscuring structural changes are minimal. We thereby systematically alter both dielectric and magnetic properties. Dielectric fluctuation is characterized by ionic polarizability while magnetic fluctuation is characterized by exchange interactions measurable by Raman scattering. The range of transition temperatures is 70 to 107 K and we find that these correlate only with the dielectric properties, a behavior which persists with external pressure. The ultimate significance may remain to be proven but it highlights the role of dielectric screening in the cuprates and adds support to a previously proposed novel pairing mechanism involving exchange of quantized waves of electronic polarization., Comment: Manuscript: 5 pages, 4 figures. Supplemental material included (9 pages, 5 figures)

We investigate the ground-state properties of a collection of \textit{N} non-interacting electrons in a macroscopic volume $\Omega$ also containing a crystalline array of \textit{N} spheres of radius $r_c$ each taken as largely impenetrable to electrons and with proximity of neighboring excluding regions playing a key physical role. The sole parameter of this quantum system is the ratio $r_c/r_s$, where $r_s$ is the Wigner- Seitz radius. Two lattices (FCC and BCC) are selected to illustrate the behavior of the system as a function of $r_c/r_s$. As this ratio increases valence electrons localize in the interstitial regions and the relative band-width $\epsilon_F/\epsilon_F^0$ is found to decrease monotonically for both. The system is motivated by the behavior of the alkali metals at significant compression. It accounts for band narrowing, leads to electronic densities with interstitially centered maxima, and can be taken as a model which clearly may be improved upon by perturbation and other methods., Comment: 11 pages, 5 figures

We introduce a diagrammatic quantum field formalism for the evaluation of normalized expectation values of operators, and suitable for systems with localized electrons. It is used to develop a convergent series expansion for the energy in powers of overlap integrals of single-particle orbitals. This method gives intuitive and practical rules for writing down the expansion to arbitrary order of overlap, and can be applied to any spin configuration and to any dimension. Its applicability for systems with well localized electrons has been illustrated with examples, including the two-dimensional Wigner crystal and spin-singlets in the low-density electron gas., Comment: 13 pages, 0 figures

Non-classical response to rotation is a hallmark of quantum ordered states such as superconductors and superfluids. The rotational responses of all currently known single-component "super" states of matter (superconductors, superfluids and supersolids) are largely described by two fundamental principles and fall into two categories according to whether the systems are composed of charged or neutral particles: the London law relating the angular velocity to a subsequently established magnetic field and the Onsager-Feynman quantization of superfluid velocity. These laws are theoretically shown to be violated in a two-component superconductor such as the projected liquid metallic states of hydrogen and deuterium at high pressures. The rotational responses of liquid metallic hydrogen or deuterium identify them as a new class of dissipationless states; they also directly point to a particular experimental route for verification of their existence., Comment: Nature Physics in print. This is an early version of the paper. The final version will be posted 6 months after its publication Nature Physics, according to the journal policy

We present a general method based on nonlinear response theory to obtain effective interactions between ions in an electron gas which can also be applied to other systems where an adiabatic separation of time-scales is possible. Nonlinear contributions to the interatomic potential are expressed in terms of physically meaningful quantities, giving insight in the physical properties of the system. The method is applied to various test cases and is found to improve the standard linear and quadratic response approaches. It also reduces the discrepancies previously observed between perturbation theory and density-functional theory results for the proton-proton pair potentials in metallic environments., Comment: 16 pages, 8 figures. v2: some added references, and a few minor modifications. To appear in Phys. Rev. B

Dissipationless quantum states, such as superconductivity and superfluidity, have attracted interest for almost a century. A variety of systems exhibit these macroscopic quantum phenomena, ranging from superconducting electrons in metals to superfluid liquids, atomic vapours, and even large nuclei. It was recently suggested that liquid metallic hydrogen could form two new unusual dissipationless quantum states, namely the metallic superfluid and the superconducting superfluid. Liquid metallic hydrogen is projected to occur only at an extremely high pressure of about 400 GPa, while pressures on hydrogen of 320 GPa having already been reported. The issue to be adressed is if this state could be experimentally observable in principle. We propose four experimental probes for detecting it., Comment: in print in Phys. Rev. Lett

Although hydrogen is the simplest of atoms, it does not form the simplest of solids or liquids. Quantum effects in these phases are considerable (a consequence of the light proton mass) and they have a demonstrable and often puzzling influence on many physical properties, including spatial order. To date, the structure of dense hydrogen remains experimentally elusive. Recent studies of the melting curve of hydrogen indicate that at high (but experimentally accessible) pressures, compressed hydrogen will adopt a liquid state, even at low temperatures. In reaching this phase, hydrogen is also projected to pass through an insulator-to-metal transition. This raises the possibility of new state of matter: a near ground-state liquid metal, and its ordered states in the quantum domain. Ordered quantum fluids are traditionally categorized as superconductors or superfluids; these respective systems feature dissipationless electrical currents or mass flow. Here we report an analysis based on topological arguments of the projected phase of liquid metallic hydrogen, finding that it may represent a new type of ordered quantum fluid. Specifically, we show that liquid metallic hydrogen cannot be categorized exclusively as a superconductor or superfluid. We predict that, in the presence of a magnetic field, liquid metallic hydrogen will exhibit several phase transitions to ordered states, ranging from superconductors to superfluids., Comment: for a related paper see cond-mat/0410425. A correction to the front page caption appeared in Oct 14 issue of Nature: http://www.nature.com/nature/links/041014/041014-11.html

Spin correlations in an interacting electron liquid are studied in the high-frequency limit and in both two and three dimensions. The third-moment sum rule is evaluated and used to derive exact limiting forms (at both long- and short-wavelengths) for the spin-antisymmetric local-field factor, $\lim_{\omega \to \infty}G_-({\bf q, \omega})$. In two dimensions $\lim_{\omega \to \infty}G_-({\bf q, \omega})$ is found to diverge as $1/q$ at long wavelengths, and the spin-antisymmetric exchange-correlation kernel of time-dependent spin density functional theory diverges as $1/q^2$ in both two and three dimensions. These signal a failure of the local-density approximation, one that can be redressed by alternative approaches., Comment: 5 pages

The structural, electronic, and adhesive properties of Cu/SiO$_2$ interfaces are investigated using first-principles density-functional theory within the local density approximation. Interfaces between fcc Cu and $\alpha$-cristobalite(001) surfaces with different surface stoichiometries are considered. Interfacial properties are found to be sensitive to the choice of the termination, and the oxygen density at the substrate surface is the most important factor influencing the strength of adhesion. For oxygen-rich interfaces, the O atoms at the interface substantially rearrange after the deposition of Cu layers, suggesting the formation of Cu-O bonds. Significant hybridization between Cu$-d$ and O$-p$ states is evident in site-projected density of states at the interface. As oxygen is systematically removed from the interface, less rearrangement is observed, implying weaker adhesion. Computed adhesion energies for each of the interfaces are found to reflect these observed structural and bonding trends, leading to the largest adhesion energy in the oxygen rich cases. The adhesion energy is also calculated between Cu and SiO$_2$ substrates terminated with hydroxyl groups, and adhesion of Cu to these substrates is found to be considerably reduced. This work supports the notion that Cu films can adhere well to hydroxyl-free SiO$_2$ substrates should oxygen be present in sufficient amounts at the interface., Comment: 9 pages, 8 figures, 2 tables

Using density functional theory implemented within the generalized gradient approximation, a new non-magnetic insulating ground state of solid oxygen is proposed and found to be energetically favored at pressures corresponding to the $\epsilon$-phase. The newly-predicted ground state is composed of linear herringbone-type chains of O$_2$ molecules and has {\it Cmcm} symmetry (with an alternative monoclinic cell). Importantly, this phase supports IR-active zone-center phonons, and their computed frequencies are found to be in broad agreement with recent infrared absorption experiments., Comment: 4 pages, 4 figures

We calculate the leading order corrections (in $r_s$) to the static polarization $\Pi^{*}(q,0,)$, with dynamically screened interactions, for the two-dimensional electron gas. The corresponding diagrams all exhibit singular logarithmic behavior in their derivatives at $q=2 k_F$ and provide significant enhancement to the proper polarization particularly at low densities. At a density of $r_s=3$, the contribution from the leading order {\em fluctuational} diagrams exceeds both the zeroth order (Lindhard) response and the self-energy and exchange contributions. We comment on the importance of these diagrams in two-dimensions and make comparisons to an equivalent three-dimensional electron gas; we also consider the impact these finding have on $\Pi^{*}(q,0)$ computed to all orders in perturbation theory.

The dynamic response of an interacting electron system is determined by an extension of the relaxation-time approximation forced to obey local conservation laws for number, momentum and energy. A consequence of these imposed constraints is that the local electron equilibrium distribution must have a space- and time-dependent chemical potential, drift velocity and temperature. Both quantum kinetic and semi-classical arguments are given, and we calculate and analyze the corresponding analytical d-dimensional dielectric function. Dynamical correlation, arising from relaxation effects, is shown to soften the plasmon dispersion of both two- and three-dimensional systems. Finally, we consider the consequences for a hydrodynamic theory of a d-dimensional interacting electron gas, and by incorporating the competition between relaxation and inertial effects we derive generalised hydrodynamic equations applicable to arbitrary frequencies., Comment: Revtex4. 16 pages, 6 figures. Typos have been corrected

Using density functional theory the ground state structural, electronic, and magnetic properties of monatomic lithium and sodium chains with low average density are investigated. A metallic, zigzag ground state structure is predicted but, most interestingly, stable equilibria for chains under tension are predicted to be {\it ferromagnetic}, which can be traced to exchange effects arising from occupation of the second subband as a function of the interatomic distance., Comment: Revised version; 4 pages, 4 figures; to appear in International Journal of Quantum Chemistry (2003)

Using density functional theory the atomic and electronic structure of sodium are predicted to depart substantially from those expected of simple metals for $r_s <$ 2.48 ($p > 130$ GPa). Newly-predicted phases include those with low structural symmetry, semi-metallic electronic properties (including zero-gap semiconducting limiting behavior), unconventional valence charge density distributions, and even those that raise the possibility of superconductivity, all at currently achievable pressures. Important differences emerge between sodium and lithium at high densities, and these are attributable to corresponding differences in their respective cores., Comment: 13 pages; 3 figures

We show that electron-ion structure factors in fluid metallic systems can be well understood from an application of linear response in the electron system, combined with hard-sphere like correlation for the ionic component. In particular, we predict that electron-ion structure factors fall into two general classes, one for high ($Z>3$) and one for low ($Z\leq2$) valence metals, and make suggestions for experiments to test these ideas. In addition, we show how the general success of electronic linear response for most metallic systems stems in part from an intrinsic interference between atomic and electronic length scales which weakens the nonlinear response. The main exception to this is metallic hydrogen., Comment: to appear in J. Non-Crystalline Solids, part of LAM-10 conference proceedings. RevTex, 12 pages, 2 figures

Linear response methods applied to electron systems often display a level of accuracy which is notable when viewed in terms of the strengths of perturbing interactions. Neglect of higher response terms is in fact justifiable in many cases and it can be shown to stem from an intrinsic interference between atomic and electronic length scales. For fluid metallic systems it can be further shown that electron-ion structure (increasingly accessible experimentally) can be understood from an application of linear response in the electron system, combined with hard-sphere like correlation for the ionic component., Comment: 5 pages, 2 figures

The electrical resistivity of liquid hydrogen has been measured at the high dynamic pressures, densities and temperatures that can be achieved with a reverberating shock wave. The resulting data are most naturally interpreted in terms of a continuous transition from a semiconducting to a metallic, largely diatomic fluid, the latter at 140 GPa, (ninefold compression) and 3000 K. While the fluid at these conditions resembles common liquid metals by the scale of its resistivity of 500 micro-ohm-cm, it differs by retaining a strong pairing character, and the precise mechanism by which a metallic state might be attained is still a matter of debate. Some evident possibilities include (i) physics of a largely one-body character, such as a band-overlap transition, (ii) physics of a strong-coupling or many-body character,such as a Mott-Hubbard transition, and (iii) processes in which structural changes are paramount., Comment: 12 pages, RevTeX format. Figures available on request; send mail to: ardlouis@msc.cornell.edu To appear: Philosophical Transaction of the Royal Society A

Density-functional theory is applied to compute the ground-state energies of quantum hard-sphere solids. The modified weighted-density approximation is used to map both the Bose and the Fermi solid onto a corresponding uniform Bose liquid, assuming negligible exchange for the Fermi solid. The required liquid-state input data are obtained from a paired phonon analysis and the Feynman approximation, connecting the static structure factor and the linear response function. The Fermi liquid is treated by the Wu-Feenberg cluster expansion, which approximately accounts for the effects of antisymmetry. Liquid-solid transitions for both systems are obtained with no adjustment of input data. Limited quantitative agreement with simulation indicates a need for further improvement of the liquid-state input through practical alternatives to the Feynman approximation., Comment: IOP-TeX, 21 pages + 7 figures, to appear, J. Phys.: Condens. Matter