Investigation of Planckian behavior in a high-conductivity oxide: PdCrO2.

The layered delafossite metal PdCrO[Formula: see text] is a natural heterostructure of highly conductive Pd layers Kondo coupled to localized spins in the adjacent Mott insulating CrO[Formula: see text] layers. At high temperatures, T, it has a T-linear resistivity which is not seen in the isostructural but nonmagnetic PdCoO[Formula: see text]. The strength of the Kondo coupling is known, as-grown crystals are extremely high purity and the Fermi surface is both very simple and experimentally known. It is therefore an ideal material platform in which to investigate "Planckian metal" physics. We do this by means of controlled introduction of point disorder, measurement of the thermal conductivity and Lorenz ratio, and studying the sources of its high-temperature entropy. The T-linear resistivity is seen to be due mainly to elastic scattering and to arise from a sum of several scattering mechanisms. Remarkably, this sum leads to a scattering rate within 10[Formula: see text] of the Planckian value of k[Formula: see text]T/[Formula: see text].

Low-symmetry nonlocal transport in microstructured squares of delafossite metals.

Intense work studying the ballistic regime of electron transport in two-dimensional systems based on semiconductors and graphene had been thought to have established most of the key experimental facts of the field. In recent years, however, additional forms of ballistic transport have become accessible in the quasi-two-dimensional delafossite metals, whose Fermi wavelength is a factor of 100 shorter than those typically studied in the previous work and whose Fermi surfaces are nearly hexagonal in shape and therefore strongly faceted. This has some profound consequences for results obtained from the classic ballistic transport experiment of studying bend and Hall resistances in mesoscopic squares fabricated from delafossite single crystals. We observe pronounced anisotropies in bend resistances and even a Hall voltage that is strongly asymmetric in magnetic field. Although some of our observations are nonintuitive at first sight, we show that they can be understood within a nonlocal Landauer-Büttiker analysis tailored to the symmetries of the square/hexagonal geometries of our combined device/Fermi surface system. Signatures of nonlocal transport can be resolved for squares of linear dimension of nearly 100 µm, approximately a factor of 15 larger than the bulk mean free path of the crystal from which the device was fabricated.

Parity Transition of Spin-Singlet Superconductivity Using Sublattice Degrees of Freedom.

Recently, a superconducting (SC) transition from low-field (LF) to high-field (HF) SC states was reported in CeRh_{2}As_{2}, indicating the existence of multiple SC states. It has been theoretically noted that the existence of two Ce sites in the unit cell, the so-called sublattice degrees of freedom owing to the local inversion symmetry breaking at the Ce sites, can lead to the appearance of multiple SC phases even under an interaction inducing spin-singlet superconductivity. CeRh_{2}As_{2} is considered as the first example of multiple SC phases owing to this sublattice degree of freedom. However, microscopic information about the SC states has not yet been reported. In this study, we measured the SC spin susceptibility at two crystallographically inequivalent As sites using nuclear magnetic resonance for various magnetic fields. Our experimental results strongly indicate a spin-singlet state in both SC phases. In addition, the antiferromagnetic phase, which appears within the SC phase, only coexists with the LF SC phase; there is no sign of magnetic ordering in the HF SC phase. The present Letter reveals unique SC properties originating from the locally noncentrosymmetric characteristics.

Observation of Antiferromagnetic Order as Odd-Parity Multipoles inside the Superconducting Phase in CeRh_{2}As_{2}.

Spatial inversion symmetry in crystal structures is closely related to the superconducting (SC) and magnetic properties of materials. Recently, several theoretical proposals that predict various interesting phenomena caused by the breaking of the local inversion symmetry have been presented. However, experimental validation has not yet progressed owing to the lack of model materials. Here we present evidence for antiferromagnetic (AFM) order in CeRh_{2}As_{2} (SC transition temperature T_{SC}∼0.37 K), wherein the Ce site breaks the local inversion symmetry. The evidence is based on the observation of different extents of broadening of the nuclear quadrupole resonance spectrum at two crystallographically inequivalent As sites. This AFM ordering breaks the inversion symmetry of this system, resulting in the activation of an odd-parity magnetic multipole. Moreover, the onset of antiferromagnetism T_{N} within an SC phase, with T_{N}

Itinerant ferromagnetism of the Pd-terminated polar surface of PdCoO2.

The ability to modulate the collective properties of correlated electron systems at their interfaces and surfaces underpins the burgeoning field of "designer" quantum materials. Here, we show how an electronic reconstruction driven by surface polarity mediates a Stoner-like magnetic instability to itinerant ferromagnetism at the Pd-terminated surface of the nonmagnetic delafossite oxide metal PdCoO2 Combining angle-resolved photoemission spectroscopy and density-functional theory calculations, we show how this leads to a rich multiband surface electronic structure. We find similar surface state dispersions in PdCrO2, suggesting surface ferromagnetism persists in this sister compound despite its bulk antiferromagnetic order.

Orbital selective Fermi surface shifts and mechanism of high T(c) superconductivity in correlated AFeAs (A=Li, Na).

Based on the dynamical mean field theory and angle resolved photoemission spectroscopy, we have investigated the mechanism of high T(c) superconductivity in stoichiometric LiFeAs. The calculated spectrum is in excellent agreement with the measured angle resolved photoemission spectroscopy. The Fermi surface (FS) nesting, which is predicted in the conventional density functional theory method, is suppressed due to the orbital-dependent correlation effect within the dynamical mean field theory method. We have shown that such marginal breakdown of the FS nesting is an essential condition to the spin-fluctuation mediated superconductivity, while the good FS nesting in NaFeAs induces a spin density wave ground state. Our results indicate that a fully charge self-consistent description of the correlation effect is crucial in the description of the FS nesting-driven instabilities.

Directional ballistic transport in the two-dimensional metal PdCoO2.

In an idealized infinite crystal, the material properties are constrained by the symmetries of the unit cell. The point-group symmetry is broken by the sample shape of any finite crystal, but this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from an anisotropic Fermi surface are needed. Here we show how a strongly facetted Fermi surface and the long quasiparticle mean free path present in microstructures of PdCoO2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. We fabricate bar-shaped transport devices narrower than the mean free path from single crystals using focused ion beam milling, such that the ballistic charge carriers at low temperatures frequently collide with both of the side walls that define the channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and a transverse voltage appears in zero magnetic field. Using ballistic Monte Carlo simulations and a numerical solution of the Boltzmann equation, we identify the orientation of the narrow channel as the source of symmetry breaking.

Quasiparticle interference and quantum confinement in a correlated Rashba spin-split 2D electron liquid.

Exploiting inversion symmetry breaking (ISB) in systems with strong spin-orbit coupling promises control of spin through electric fields-crucial to achieve miniaturization in spintronic devices. Delivering on this promise requires a two-dimensional electron gas with a spin precession length shorter than the spin coherence length and a large spin splitting so that spin manipulation can be achieved over length scales of nanometers. Recently, the transition metal oxide terminations of delafossite oxides were found to exhibit a large Rashba spin splitting dominated by ISB. In this limit, the Fermi surface exhibits the same spin texture as for weak ISB, but the orbital texture is completely different, raising questions about the effect on quasiparticle scattering. We demonstrate that the spin-orbital selection rules relevant for conventional Rashba system are obeyed as true spin selection rules in this correlated electron liquid and determine its spin coherence length from quasiparticle interference imaging.

h/e oscillations in interlayer transport of delafossites.

Microstructures can be carefully designed to reveal the quantum phase of the wave-like nature of electrons in a metal. Here, we report phase-coherent oscillations of out-of-plane magnetoresistance in the layered delafossites PdCoO2 and PtCoO2 The oscillation period is equivalent to that determined by the magnetic flux quantum, h/e, threading an area defined by the atomic interlayer separation and the sample width, where h is Planck's constant and e is the charge of an electron. The phase of the electron wave function appears robust over length scales exceeding 10 micrometers and persisting up to temperatures of T > 50 kelvin. We show that the experimental signal stems from a periodic field modulation of the out-of-plane hopping. These results demonstrate extraordinary single-particle quantum coherence lengths in delafossites.

Evidence for coexistence of superconductivity and magnetism in single crystals of Co-doped SrFe(2)As(2).

In order to investigate whether magnetism and superconductivity coexist in Co-doped SrFe(2)As(2), we have prepared single crystals of SrFe(2-x)Co(x)As(2), x = 0 and 0.4, and characterized them via x-ray diffraction, electrical resistivity in zero and applied field up to 9 T as well as at ambient and applied pressure up to 1.6 GPa, and magnetic susceptibility. At x = 0.4, there is both magnetic and resistive evidence for a spin density wave transition at 120 K, while T(c) = 19.5 K-indicating coexistent magnetism and superconductivity. A discussion of how these results compare with reported results, both in SrFe(2-x)Co(x)As(2) and in other doped 122 compounds, is given.

Interactions in the bond-frustrated helimagnet ZnCr2Se4 investigated by NMR.

The zero field 53Cr nuclear magnetic resonance was measured at low temperatures to investigate the interactions in the bond-frustrated S = 3/2 Heisenberg helimagnet ZnCr2Se4. A quadratic decrease of the sublattice magnetization was determined from the temperature dependence of the isotropic hyperfine field. We calculated the magnetization using linear spin wave theory for the incommensurate spiral spin order and compared this outcome with experimental results to estimate the coupling constants. The hyperfine fields at Cr and Se ions provide evidences that the spin polarization of Cr ions is transferred to neighboring Se ions due to the covalent bonding between them, resulting in reduced magnetic moment in the Cr ion. This observation indicates that the Jahn-Teller effect, which leads to distortion inducing spin-lattice coupling, is not completely missing in ZnCr2Se4.

Super-geometric electron focusing on the hexagonal Fermi surface of PdCoO2.

Geometric electron optics may be implemented in solids when electron transport is ballistic on the length scale of a device. Currently, this is realized mainly in 2D materials characterized by circular Fermi surfaces. Here we demonstrate that the nearly perfectly hexagonal Fermi surface of PdCoO2 gives rise to highly directional ballistic transport. We probe this directional ballistic regime in a single crystal of PdCoO2 by use of focused ion beam (FIB) micro-machining, defining crystalline ballistic circuits with features as small as 250 nm. The peculiar hexagonal Fermi surface naturally leads to enhanced electron self-focusing effects in a magnetic field compared to circular Fermi surfaces. This super-geometric focusing can be quantitatively predicted for arbitrary device geometry, based on the hexagonal cyclotron orbits appearing in this material. These results suggest a novel class of ballistic electronic devices exploiting the unique transport characteristics of strongly faceted Fermi surfaces.

In Situ Modification of a Delafossite-Type PdCoO2 Bulk Single Crystal for Reversible Hydrogen Sorption and Fast Hydrogen Evolution.

The observation of extraordinarily high conductivity in delafossite-type PdCoO2 is of great current interest, and there is some evidence that electrons behave like a fluid when flowing in bulk crystals of PdCoO2. Thus, this material is an ideal platform for the study of the electron transfer processes in heterogeneous reactions. Here, we report the use of bulk single-crystal PdCoO2 as a promising electrocatalyst for hydrogen evolution reactions (HERs). An overpotential of only 31 mV results in a current density of 10 mA cm-2, accompanied by high long-term stability. We have precisely determined that the crystal surface structure is modified after electrochemical activation with the formation of strained Pd nanoclusters in the surface layer. These nanoclusters exhibit reversible hydrogen sorption and desorption, creating more active sites for hydrogen access. The bulk PdCoO2 single crystal with ultrahigh conductivity, which acts as a natural substrate for the Pd nanoclusters, provides a high-speed channel for electron transfer.

Manifestation of magnetic quantum fluctuations in the dielectric properties of a multiferroic.

Insulating magnets can display novel signatures of quantum fluctuations as similar to the case of metallic magnets. However, their weak spin-lattice coupling has made such observations challenging. Here we find that antiferromagnetic (AF) quantum fluctuations manifest in the dielectric properties of multiferroic Ba2CoGe2O7, where a ferroelectric polarization develops concomitant to an AF ordering. Upon application of a magnetic field (H), dielectric constant shows a characteristic power-law dependence near absolute zero temperature and close to the critical field Hc=37.1 T due to enhanced AF quantum fluctuations. When H>Hc, the dielectric constant shows the temperature-dependent anomalies that reflect a crossover from a field-tuned quantum critical to a gapped spin-polarized state. We uncover theoretically that a linear relation between AF susceptibility and dielectric constant stems from the generic magnetoelectric coupling and directly explains the experimental findings, opening a new pathway for studying quantum criticality in condensed matter.