Search

In recent years, metal hydride research has become one of the driving forces of the high-pressure community, as it is believed to hold the key to superconductivity close to ambient temperature. While numerous novel metal hydride compounds have been reported and extensively investigated for their superconducting properties, little attention has been focused on the atomic and electronic states of hydrogen, the main ingredient in these novel compounds. Here, we present combined $^{1}H$- and $^{139}La$-NMR data on lanthanum superhydrides, $LaH_{x}$, ($x = 10.2 - 11.1$), synthesized after laser heating at pressures above 160 GPa. Strikingly, we found hydrogen to be in a highly diffusive state at room temperature, with diffusion coefficients in the order of $10^{-6}~cm^2s^{-1}$. We found that this diffusive state of hydrogen results in a dynamic de-hydrogenation of the sample over the course of several weeks, approaching a composition similar to its precursor materials. Quantitative measurements demonstrate that the synthesized superhydrides continuously decompose over time. Transport measurements underline this conclusion as superconducting critical temperatures were found to decrease significantly over time as well. This observation sheds new light on formerly unanswered questions on the long-term stability of metal superhydrides.

High-temperature superconductivity has been observed in binary hydrides such as LaH10 at pressures above 150 GPa. Hydrogen cage structures have been identified as a common motif beneficial for high critical temperatures Tc. Efforts are now focused on finding hydride high-temperature superconductors at lower pressures. We present evidence for high-temperature superconductivity in binary La4H23 with A15-type structure featuring hydrogen cages at a pressure of P = 95 GPa. We synthesise La4H23 from a lanthanum film capped with a palladium catalyst promoting the dissociation of hydrogen. In resistance measurements, we observe superconductivity with a transition temperature Tc = 90 K. In X-ray diffraction on the same sample, we identify the A15-type cubic body centred structure of the lanthanum sublattice. From comparison with earlier XRD and structure prediction studies, we identify this phase with La4H23. Our study reinforces the concept of hydrogen cages for high-temperature superconductivity., Comment: 18 Pages

Superconductivity often emerges as a dome around a quantum critical point (QCP) where long-range order is suppressed to zero temperature. So far, this has been mostly studied in magnetically ordered materials. By contrast, the interplay between charge order and superconductivity at a QCP is not fully understood. Here, we present resistance measurements proving that a dome of superconductivity surrounds the charge-density-wave (CDW) QCP in pristine samples of 1$T$-TiSe$_2$ tuned with hydrostatic pressure. Furthermore, we use quantum oscillation measurements to show that the superconductivity sets in at a Lifshitz transition in the electronic band structure. We use density functional theory to identify the Fermi pockets enabling superconductivity: large electron and hole pockets connected by the CDW wave vector $\vec{Q}$ which emerge upon partial suppression of the zero-pressure CDW gap. Hence, we conclude that superconductivity is of interband type enabled by the presence of hole and electron bands connected by the CDW $\vec{Q}$ vector. Earlier calculations show that interband interactions are repulsive, which suggests that unconventional s$_{\pm}$ superconductivity is realised in TiSe$_2$ - similar to the iron pnictides. These results highlight the importance of Lifshitz transitions in realising unconventional superconductivity and help understand its interaction with CDW order in numerous materials., Comment: 21 pages, 5 figures

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 for superconductors. We identify a linear temperature-over-field scaling of the resistance at the superconducting transition which is not described by existing theories.

Electronic nematicity in correlated metals often occurs alongside another instability such as magnetism. As a result, the question remains whether nematicity alone can drive unconventional superconductivity or anomalous (quantum critical) transport in such systems. In FeSe, nematicity emerges in isolation, providing a unique opportunity to address this question. Studies to date, however, have proved inconclusive; while signatures of nematic criticality are observed upon sulfur substitution, they appear to be quenched under the application of pressure due to the emergent magnetism. Here, we study the temperature and pressure dependence of the low-temperature resistivity of FeSe$_{1-x}$S$_{x}$ crystals at $x$ values just beyond the nematic quantum critical point. Two distinct components to the resistivity are revealed; one whose magnitude falls with increasing pressure and one which grows upon approaching the magnetic state at higher pressures. These findings indicate that nematic and magnetic critical fluctuations in FeSe$_{1-x}$S$_{x}$ are completely decoupled, in marked contrast to other Fe-based superconductors, and that nematic fluctuations alone may be responsible for the transport signatures of quantum criticality found in FeSe$_{1-x}$S$_{x}$ at ambient pressure.

We present electrical resistance measurements of elemental yttrium on bulk and film samples, and both exhibit superconductivity at very high pressures. We show that the pressure dependence of the superconducting transition temperature above 100 GPa is in good agreement with the predicted Fddd phase by Chen et al. [Phys. Rev. lett. 109, 157004 (2012)]. This result together with a new Rietveld refinement made on X-ray data at 123 GPa from Samudrala et al. [J. Phys. Condens. Matter 24, 362201 (2012)] offer strong evidence that the atomic structure of yttrium above 100 GPa is orthorhombic Fddd. Furthermore, our process of evaporating yttrium film directly on a diamond anvil is expected to be a valuable asset for future synthesis of new superhydride superconductors.

The evolution of the charge carrier concentrations and mobilities are examined across the charge-density-wave (CDW) transition in TiSe2. Combined quantum oscillation and magnetotransport measurements show that a small electron pocket dominates the electronic properties at low temperatures whilst an electron and hole pocket contribute at room temperature. At the CDW transition, an abrupt Fermi surface reconstruction and a minimum in the electron and hole mobilities are extracted from two-band and Kohler analysis of magnetotransport measurements. The minimum in the mobilities is associated with the overseen role of scattering from the softening CDW mode. With the carrier concentrations and dynamics dominated by the CDW and the associated bosonic mode, our results highlight TiSe2 as a prototypical system to study the Fermi surface reconstruction at a density-wave transition., Comment: 15 pages, 3 figures, including supplementary information

Layered $\alpha$-RuCl3 has been discussed as a proximate Kitaev spin liquid compound. Raman and THz spectroscopy of magnetic excitations confirm that the low-temperature antiferromagnetic ordered phase features a broad Raman continuum, together with two magnon-like excitations at 2.7 and 3.6 meV, respectively. The continuum strength is maximized as long-range order is suppressed by an external magnetic field. The state above the field-induced quantum phase transition around 7.5 T is characterized by a gapped multi-particle continuum out of which a two-particle bound state emerges, together with a well-defined single-particle excitation at lower energy. Exact diagonalization calculations demonstrate that Kitaev and off-diagonal exchange terms in the Fleury-Loudon operator are crucial for the occurrence of these features in the Raman spectra. Our study firmly establishes the partially-polarized quantum disordered character of the high-field phase.

The recent discovery of a non-magnetic nematic quantum critical point (QCP) in the iron chalcogenide family FeSe$_{1-x}$S$_{x}$ has raised the prospect of investigating, in isolation, the role of nematicity on the electronic properties of correlated metals. Here we report a detailed study of the normal state transverse magnetoresistance (MR) in FeSe$_{1-x}$S$_{x}$ for a series of S concentrations spanning the nematic QCP. For all temperatures and \textit{x}-values studied, the MR can be decomposed into two distinct components: one that varies quadratically in magnetic field strength $\mu_{0}\textit{H}$ and one that follows precisely the quadrature scaling form recently reported in metals at or close to a QCP and characterized by a \textit{H}-linear MR over an extended field range. The two components evolve systematically with both temperature and S-substitution in a manner that is determined by their proximity to the nematic QCP. This study thus reveals unambiguously the coexistence of two independent charge sectors in a quantum critical system. Moreover, the quantum critical component of the MR is found to be less sensitive to disorder than the quadratic (orbital) MR, suggesting that detection of the latter in previous MR studies of metals near a QCP may have been obscured., Comment: 19 pages (including Supplemental Material), 12 figures

A polarized electronic Raman scattering study reveals the emergence of symmetry dependence in the electronic Raman response of single crystalline URu$_{2}$Si$_{2}$ below the Kondo crossover scale $T_K\sim100K$. In particular, the development of a coherent Kondo pseudo-gap predominantly in the E$_g$ channel highlights strong anisotropy in the Kondo physics in URu$_{2}$Si$_{2}$ that has previously been neglected in theoretical models of this system. A calculation of the Raman vertices demonstrates that the strongest Raman vertex does indeed develop within the E$_g$ channel for interband transitions and reaches a maximum along the diagonals of the Brillouin zone, implying a d-wave-like geometry for the Kondo pseudo-gap. Below the hidden order phase transition at $T_{HO}= 17.5K$, the magnitude of the pseudo-gap is found to be enhanced. Moreover, the anisotropy of the pseudo-gap is similar in form to that proposed for the chiral d-wave (E$_g$) superconducting state that appears below $T_c=1.5K$.

The iron-based high temperature superconductors share a number of similarities with their copper-based counterparts, such as reduced dimensionality, proximity to states of competing order, and a critical role for 3d electron orbitals. Their respective temperature-doping phase diagrams also contain certain commonalities that have led to claims that the metallic and superconducting properties of both families are governed by their proximity to a quantum critical point (QCP) located inside the superconducting dome. In this review, we critically examine these claims and highlight significant differences in the bulk physical properties of both systems. While there is now a large body of evidence supporting the presence of a (magnetic) QCP in the iron pnictides, the situation in the cuprates is much less apparent, at least for the end point of the pseudogap phase. We argue that the opening of the normal state pseudogap in cuprates, so often tied to a putative QCP, arises from a momentum-dependent breakdown of quasiparticle coherence that sets in at much higher doping levels but which is driven by the proximity to the Mott insulating state at half filling. Finally, we present a new scenario for the cuprates in which this loss of quasiparticle integrity and its evolution with momentum, temperature and doping plays a key role in shaping the resultant phase diagram., Comment: This key issues review is dedicated to the memory of Dr. John Loram whose pioneering measurements, analysis and ideas inspired much of its content

We have performed Raman scattering measurements on URu$_2$Si$_2$ single crystals on a large energy range up to $\sim$ 1300 cm$^{-1}$ and in all the Raman active symmetries as a function of temperature down to 15 K. A large excitation, active only in the E$_{g}$ symmetry, is reported. It has been assigned to a crystal electric field excitation on the Uranium site. We discuss how this constrains the crystal electric field scheme of the Uranium ions. Furthermore, three excitations in the A$_{1g}$ symmetry are observed. They have been associated to double Raman phonon processes consistently with ab initio calculations of the phonons dispersion.

Polymer translocation is a promising strategy for the next-generation DNA sequencing technologies. The use of biological and synthetic nano-pores, however, still suffers from serious drawbacks. In particular, the width of the membrane layer can accommodate several bases at the same time, making difficult accurate sequencing applications. More recently, the use of graphene membranes has paved the way to new sequencing capabilities, with the possibility to measure transverse currents, among other advances. The reduced thickness of these new membranes poses new questions on the effect of deformability and vibrations of the membrane on the translocation process, two features which are not taken into account in the well-established theoretical frameworks. Here, we make a first step forward in this direction. We report numerical simulation work on a model system simple enough to allow gathering significant insight on the effect of these features on the average translocation time, with appropriate statistical significance. We have found that the interplay between thermal fluctuations and the deformability properties of the nano-pore play a crucial role in determining the process. We conclude by discussing new directions for further work.

Optical spectroscopy has been combined with computational and theoretical techniques to show how the spin dynamics in the model multiferroic BiFeO3 responds to the application of hydrostatic pressure and its corresponding series of structural phase transitions from R3c to the Pnma phases. As pressure increases, multiple spin excitations associated with non-collinear cycloidal magnetism collapse into two excitations, which show jump discontinuities at some of the ensuing crystal phase transitions. Effective Hamiltonian approach provides information on the electrical polarization and structural changes of the oxygen octahedra through the successive structural phases. The extracted parameters are then used in a Ginzburg-Landau model to reproduce the evolution with pressure of the spin waves excitations observed at low energy and we demonstrate that the structural phases and the magnetic anisotropy drive and control the spin excitations., Comment: 5 pages, 4 figures

We measured the polarized optical conductivity of URu$_2$Si$_2$ from room temperature down to 5 K, covering the Kondo state, the coherent Kondo liquid regime, and the hidden-order phase. The normal state is characterized by an anisotropic behavior between the ab plane and c axis responses. The ab plane optical conductivity is strongly influenced by the formation of the coherent Kondo liquid: a sharp Drude peak develops and a hybridization gap at 12 meV leads to a spectral weight transfer to mid-infrared energies. The c axis conductivity has a different behavior: the Drude peak already exists at 300 K and no particular anomaly or gap signature appears in the coherent Kondo liquid regime. When entering the hidden-order state, both polarizations see a dramatic decrease in the Drude spectral weight and scattering rate, compatible with a loss of about 50 % of the carriers at the Fermi level. At the same time a density-wave like gap appears along both polarizations at about 6.5 meV at 5 K. This gap closes respecting a mean field thermal evolution in the ab plane. Along the c axis it remains roughly constant and it "fills up" rather than closing., Comment: 10 pages, 7 figures

We report a comprehensive investigation of the lattice dynamics of URu$_2$Si$_2$ as a function of temperature using Raman scattering, optical conductivity and inelastic neutron scattering measurements as well as theoretical {\it ab initio} calculations. The main effects on the optical phonon modes are related to Kondo physics. The B$_{1g}$ ($\Gamma_3$ symmetry) phonon mode slightly softens below $\sim$100~K, in connection with the previously reported softening of the elastic constant, $C_{11}-C_{12}$, of the same symmetry, both observations suggesting a B$_{1g}$ symmetry-breaking instability in the Kondo regime. Through optical conductivity, we detect clear signatures of strong electron-phonon coupling, with temperature dependent spectral weight and Fano line shape of some phonon modes. Surprisingly, the line shapes of two phonon modes, E$_u$(1) and A$_{2u}$(2), show opposite temperature dependencies. The A$_{2u}$(2) mode loses its Fano shape below 150 K, whereas the E$_u$(1) mode acquires it below 100~K, in the Kondo cross-over regime. This may point out to momentum-dependent Kondo physics. By inelastic neutron scattering measurements, we have drawn the full dispersion of the phonon modes between 300~K and 2~K. No remarkable temperature dependence has been obtained including through the hidden order transition. {\it Ab initio} calculations with the spin-orbit coupling are in good agreement with the data except for a few low energy branches with propagation in the (a,b) plane.

We have performed polarized electronic Raman scattering on URu2Si2 single crystals at low temperature down to 8 K in the hidden order state and under magnetic field up to 10 T. The hidden order state is characterized by a sharp excitation at 1.7 meV and a gap in the electronic continuum below 6.8 meV. Both Raman signatures are of pure A2g symmetry. By comparing the behavior of the Raman sharp excitation and the neutron resonance at Q0=(0,0,1), we provide new evidence, constrained by selection rules of the two probes, that the hidden order state breaks the translational symmetry along the c axis such that Gamma and Z points fold on top of each other. The observation of these distinct Raman features with a peculiar A2g symmetry as a signature of the hidden order phase places strong constraints on current theories of the hidden order in URu2Si2., Comment: To be published in Physical Review Letter, Supplemental Material included, main manuscript: 4 pages, 3 figures; new version of "A2g signatures of the Hidden Order State of URu2Si2"

We report neutron diffraction experiments performed in the tetragonal antiferromagnetic heavy fermion system CeRhIn$_{5-x}$Sn$_{x}$ in its ($x$, $T$) phase diagram up to the vicinity of the critical concentration $x_c$ $\approx$ 0.40, where long range magnetic order is suppressed. The propagation vector of the magnetic structure is found to be $\bf{k_{IC}}$=(1/2, 1/2, $k_l$) with $k_l$ increasing from $k_l$=0.298 to $k_l$=0.410 when $x$ increases from $x$=0 to $x$=0.26. Surprisingly, for $x$=0.30, the order has changed drastically and a commensurate antiferromagnetism with $\bf{k_{C}}$=(1/2, 1/2, 0) is found. This concentration is located in the proximity of the quantum critical point where superconductivity is expected., Comment: 5 pages, 5 figures, submitted to Phys. Rev. B

We discuss recent results on the heavy fermion superconductor CeRhIn$_5$ which presents ideal conditions to study the strong coupling between the suppression of antiferromagnetic order and the appearance of unconventional superconductivity. The appearance of superconductivity as function of pressure is strongly connected to the suppression of the magnetic order. Under magnetic field, the re-entrance of magnetic order inside the superconducting state shows that antiferromagnetism nucleates in the vortex cores. The suppression of antiferromagnetism in CeRhIn$_5$ by Sn doping is compared to that under hydrostatic pressure., Comment: 6 pages, 8 figures, to be published in Proc. Int. Conf. Heavy Electrons (ICHE2010) J. Phys. Soc. Jpn. 80 (2011)