Pines' demon observed as a 3D acoustic plasmon in Sr2RuO4.

The characteristic excitation of a metal is its plasmon, which is a quantized collective oscillation of its electron density. In 1956, David Pines predicted that a distinct type of plasmon, dubbed a 'demon', could exist in three-dimensional (3D) metals containing more than one species of charge carrier1. Consisting of out-of-phase movement of electrons in different bands, demons are acoustic, electrically neutral and do not couple to light, so have never been detected in an equilibrium, 3D metal. Nevertheless, demons are believed to be critical for diverse phenomena including phase transitions in mixed-valence semimetals2, optical properties of metal nanoparticles3, soundarons in Weyl semimetals4 and high-temperature superconductivity in, for example, metal hydrides3,5-7. Here, we present evidence for a demon in Sr2RuO4 from momentum-resolved electron energy-loss spectroscopy. Formed of electrons in the ß and γ bands, the demon is gapless with critical momentum qc = 0.08 reciprocal lattice units and room-temperature velocity v = (1.065 ± 0.12) × 105 m s-1 that undergoes a 31% renormalization upon cooling to 30 K because of coupling to the particle-hole continuum. The momentum dependence of the intensity of the demon confirms its neutral character. Our study confirms a 67-year old prediction and indicates that demons may be a pervasive feature of multiband metals.

High-sensitivity heat-capacity measurements on Sr2RuO4 under uniaxial pressure.

A key question regarding the unconventional superconductivity of [Formula: see text] remains whether the order parameter is single- or two-component. Under a hypothesis of two-component superconductivity, uniaxial pressure is expected to lift their degeneracy, resulting in a split transition. The most direct and fundamental probe of a split transition is heat capacity. Here, we report measurement of heat capacity of samples subject to large and highly homogeneous uniaxial pressure. We place an upper limit on the heat-capacity signature of any second transition of a few percent of that of the primary superconducting transition. The normalized jump in heat capacity, [Formula: see text], grows smoothly as a function of uniaxial pressure, favoring order parameters which are allowed to maximize in the same part of the Brillouin zone as the well-studied van Hove singularity. Thanks to the high precision of our measurements, these findings place stringent constraints on theories of the superconductivity of [Formula: see text].

In-Plane Magnetic Penetration Depth in Sr_{2}RuO_{4}: Muon-Spin Rotation and Relaxation Study.

We report on measurements of the in-plane magnetic penetration depth (λ_{ab}) in single crystals of Sr_{2}RuO_{4} down to ≃0.015 K by means of muon-spin rotation-relaxation. The linear temperature dependence of λ_{ab}^{-2} for T≲0.7 K suggests the presence of nodes in the superconducting gap. This statement is further substantiated by observation of the Volovik effect, i.e., the reduction of λ_{ab}^{-2} as a function of the applied magnetic field. The experimental zero-field and zero-temperature value of λ_{ab}=124(3) nm agrees with λ_{ab}≃130 nm, calculated based on results of electronic structure measurements reported in A. Tamai et al. [High-resolution photoemission on Sr_{2}RuO_{4} reveals correlation-enhanced effective spin-orbit coupling and dominantly local self-energies, Phys. Rev. X 9, 021048 (2019)PRXHAE2160-330810.1103/PhysRevX.9.021048]. Our analysis reveals that a simple nodal superconducting energy gap, described by the lowest possible harmonic of a gap function, does not capture the dependence of λ_{ab}^{-2} on T, so the higher angular harmonics of the energy gap function need to be introduced.

Momentum-resolved superconducting energy gaps of Sr2RuO4 from quasiparticle interference imaging.

Sr2RuO4 has long been the focus of intense research interest because of conjectures that it is a correlated topological superconductor. It is the momentum space (k-space) structure of the superconducting energy gap [Formula: see text] on each band i that encodes its unknown superconducting order parameter. However, because the energy scales are so low, it has never been possible to directly measure the [Formula: see text] of Sr2RuO4 Here, we implement Bogoliubov quasiparticle interference (BQPI) imaging, a technique capable of high-precision measurement of multiband [Formula: see text] At T = 90 mK, we visualize a set of Bogoliubov scattering interference wavevectors [Formula: see text] consistent with eight gap nodes/minima that are all closely aligned to the [Formula: see text] crystal lattice directions on both the α and ß bands. Taking these observations in combination with other very recent advances in directional thermal conductivity [E. Hassinger et al., Phys. Rev. X 7, 011032 (2017)], temperature-dependent Knight shift [A. Pustogow et al., Nature 574, 72-75 (2019)], time-reversal symmetry conservation [S. Kashiwaya et al., Phys. Rev B, 100, 094530 (2019)], and theory [A. T. Rømer et al., Phys. Rev. Lett. 123, 247001 (2019); H. S. Roising, T. Scaffidi, F. Flicker, G. F. Lange, S. H. Simon, Phys. Rev. Res. 1, 033108 (2019); and O. Gingras, R. Nourafkan, A. S. Tremblay, M. Côté, Phys. Rev. Lett. 123, 217005 (2019)], the BQPI signature of Sr2RuO4 appears most consistent with [Formula: see text] having [Formula: see text] [Formula: see text] symmetry.

Nanoscale Femtosecond Dynamics of Mott Insulator (Ca0.99Sr0.01)2RuO4.

Ca2RuO4 is a transition-metal oxide that exhibits a Mott insulator-metal transition (IMT) concurrent with a symmetry-preserving Jahn-Teller distortion (JT) at 350 K. The coincidence of these two transitions demonstrates a high level of coupling between the electronic and structural degrees of freedom in Ca2RuO4. Using spectroscopic measurements with nanoscale spatial resolution, we interrogate the interplay of the JT and IMT through the temperature-driven transition. Then, we introduce photoexcitation with subpicosecond temporal resolution to explore the coupling of the JT and IMT via electron-hole injection under ambient conditions. Through the temperature-driven IMT, we observe phase coexistence in the form of a stripe phase existing at the domain wall between macroscopic insulating and metallic domains. Through ultrafast carrier injection, we observe the formation of midgap states via enhanced optical absorption. We propose that these midgap states become trapped by lattice polarons originating from the local perturbation of the JT.

Keldysh Space Control of Charge Dynamics in a Strongly Driven Mott Insulator.

The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca_{2}RuO_{4}. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100-fs pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh crossover from a multiphoton absorption to quantum tunneling dominated pair production regime. Our results provide a procedure to control coherent and nonlinear heating processes in Mott insulators, facilitating the discovery of novel out-of-equilibrium phenomena in strongly correlated systems.

Superconducting Sr2RuO4 Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden-Popper Intergrowth.

Ruddlesden-Popper (RP) phases (An+1BnO3n+1, n = 1, 2,···) have attracted intensive research with diverse functionalities for device applications. However, the realization of a high-quality RP-phase film is hindered by the formation of out-of-phase boundaries (OPBs) that occur at terrace edges, originating from lattice mismatch in the c-axis direction with the A'B'O3 (n = ∞) substrate. Here, using strontium ruthenate RP-phase Sr2RuO4 (n = 1) as a model system, an experimental approach for suppressing OPBs was developed. By tuning the growth parameters, the Sr3Ru2O7 (n = 2) phase was formed in a controlled manner near the film-substrate interface. This higher-order RP-phase then blocked the subsequent formation of OPBs, resulting in nearly defect-free Sr2RuO4 layer at the upper region of the film. Consequently, the Sr2RuO4 thin films exhibited superconductivity up to 1.15 K, which is the highest among Sr2RuO4 films grown by pulsed laser deposition. This work paves the way for synthesizing pristine RP-phase heterostructures and exploring their unique physical properties.

Retraction: In Situ Control of Diamagnetism by Electric Current in Ca_{3}(Ru_{1-x}Ti_{x})_{2}O_{7} [Phys. Rev. Lett. 122, 196602 (2019)].

Retraction of DOI: 10.1103/PhysRevLett.122.196602.

In Situ Control of Diamagnetism by Electric Current in Ca_{3}(Ru_{1-x}Ti_{x})_{2}O_{7}.

Nonequilibrium steady state conditions induced by a dc current can alter the physical properties of strongly correlated electron systems. In this regard, it was recently shown that dc current can trigger novel electronic states, such as current-induced diamagnetism, which cannot be realized in equilibrium conditions. However, reversible control of diamagnetism has not been achieved yet. Here, we demonstrate reversible in situ control between a Mott insulating state and a diamagnetic semimetal-like state by a dc current in the Ti-substituted bilayer ruthenate Ca_{3}(Ru_{1-x}Ti_{x})_{2}O_{7} (x=0.5%). By performing simultaneous magnetic and resistive measurements, we map out the temperature vs current-density phase diagram in the nonequilibrium steady state of this material. The present results open up the possibility of creating novel electronic states in a variety of strongly correlated electron systems under dc current.

Violation of emergent rotational symmetry in the hexagonal Kagome superconductor CsV3Sb5.

Superconductivity is caused by electron pairs that are canonically isotropic, whereas some exotic superconductors are known to exhibit non-trivial anisotropy stemming from unconventional pairings. However, superconductors with hexagonal symmetry, the highest rotational symmetry allowed in crystals, exceptionally have strong constraint that is called emergent rotational symmetry (ERS): anisotropic properties should be very weak especially near the critical temperature Tc even for unconventional pairings such as d-wave states. Here, we investigate superconducting anisotropy of the recently-found hexagonal Kagome superconductor CsV3Sb5, which is known to exhibit various intriguing phenomena originating from its undistorted Kagome lattice formed by vanadium atoms. Based on calorimetry performed under accurate two-axis field-direction control, we discover a combination of six- and two-fold anisotropies in the in-plane upper critical field. Both anisotropies, robust up to very close to Tc, are beyond predictions of standard theories. We infer that this clear ERS violation with nematicity is best explained by multi-component nematic superconducting order parameter in CsV3Sb5 intertwined with symmetry breakings caused by the underlying charge-density-wave order.

First-order superconducting transition of Sr2RuO4.

By means of the magnetocaloric effect, we examine the nature of the superconducting-normal (S-N) transition of Sr(2)RuO(4), a most promising candidate for a spin-triplet superconductor. We provide thermodynamic evidence that the S-N transition of this oxide is of first order below approximately 0.8 K and only for magnetic field directions very close to the conducting plane, in clear contrast to the ordinary type-II superconductors exhibiting second-order S-N transitions. The entropy release across the transition at 0.2 K is 10% of the normal-state entropy. Our result urges an introduction of a new mechanism to break superconductivity by magnetic field.

Extremely large magnetoresistance in the nonmagnetic metal PdCoO2.

Extremely large magnetoresistance is realized in the nonmagnetic layered metal PdCoO(2). In spite of a highly conducting metallic behavior with a simple quasi-two-dimensional hexagonal Fermi surface, the interlayer resistance reaches up to 35,000% for the field along the [11[over ¯]0] direction. Furthermore, the temperature dependence of the resistance becomes nonmetallic for this field direction, while it remains metallic for fields along the [110] direction. Such severe and anisotropic destruction of the interlayer coherence by a magnetic field on a simple Fermi surface is ascribable to orbital motion of carriers on the Fermi surface driven by the Lorentz force, but seems to have been largely overlooked until now.

Quantum oscillations and high carrier mobility in the delafossite PdCoO(2).

We present de Haas-van Alphen and resistivity data on single crystals of the delafossite PdCoO(2). At 295 K we measure an in-plane resistivity of 2.6 µΩ cm, making PdCoO(2) the most conductive oxide known. The low-temperature in-plane resistivity has an activated rather than the usual T(5) temperature dependence, suggesting a gapping of effective scattering that is consistent with phonon drag. Below 10 K, the transport mean free path is ∼20 µm, approximately 10(5) lattice spacings and an astoundingly high value for flux-grown crystals. We discuss the origin of these properties in light of our data.

Edge states of Sr2RuO4 detected by in-plane tunneling spectroscopy.

Tunneling spectroscopy has been performed on Sr(2)RuO(4) searching for the edge states peculiar to topological superconductivity. Conductance spectra exhibit broad humps with three types of peak shape: domelike peak, split peak, and two-step peak. By comparing the experiments with predictions for unconventional superconductivity, these varieties are shown to originate from multiband chiral p-wave symmetry with weak anisotropy of pair amplitude. The broad hump in the conductance spectrum is a direct manifestation of the edge state due to chiral p-wave superconductivity.

Unsplit superconducting and time reversal symmetry breaking transitions in Sr2RuO4 under hydrostatic pressure and disorder.

There is considerable evidence that the superconducting state of Sr2RuO4 breaks time reversal symmetry. In the experiments showing time reversal symmetry breaking, its onset temperature, TTRSB, is generally found to match the critical temperature, Tc, within resolution. In combination with evidence for even parity, this result has led to consideration of a dxz ± idyz order parameter. The degeneracy of the two components of this order parameter is protected by symmetry, yielding TTRSB = Tc, but it has a hard-to-explain horizontal line node at kz = 0. Therefore, s ± id and d ± ig order parameters are also under consideration. These avoid the horizontal line node, but require tuning to obtain TTRSB ≈ Tc. To obtain evidence distinguishing these two possible scenarios (of symmetry-protected versus accidental degeneracy), we employ zero-field muon spin rotation/relaxation to study pure Sr2RuO4 under hydrostatic pressure, and Sr1.98La0.02RuO4 at zero pressure. Both hydrostatic pressure and La substitution alter Tc without lifting the tetragonal lattice symmetry, so if the degeneracy is symmetry-protected, TTRSB should track changes in Tc, while if it is accidental, these transition temperatures should generally separate. We observe TTRSB to track Tc, supporting the hypothesis of dxz ± idyz order.

Low-dimensional structure and magnetism of the quantum antiferromagnet Rb4Cu(MoO4)3 and the structure of Rb4Zn(MoO4)3.

Single crystals of the quantum low-dimensional antiferromagnet Rb(4)Cu(MoO(4))(3) and the nonmagnetic analogue Ru(4)Zn(MoO(4))(3) have been synthesized by a flux-growth method. Detailed structural studies indicate that the Cu(II)-O network separated by a MoO(4) layer has a strongly anisotropic hybridization along the a-axis, forming a quasi-one-dimensional (1-d) chain of Cu(II) S = 1/2 spins. Furthermore, our low-temperature thermodynamic measurements have revealed that a quantum paramagnetic state with Wilson ratio approximately 2 remains stable down to at least 0.1 K, 100 times lower than the intrachain antiferromagnetic coupling scale. The low-temperature magnetic and thermal properties are found to be consistent with theoretical predictions made for a 1-d network of S = 1/2 spins.

Unconventional anomalous hall effect in the metallic triangular-lattice magnet PdCrO2.

We experimentally reveal an unconventional anomalous Hall effect (UAHE) in a quasi-two-dimensional triangular-lattice antiferromagnet PdCrO2. Using high quality single crystals of PdCrO2, we found that the Hall resistivity ρ(xy) deviates from the conventional behavior below T*≃20 K, noticeably lower than T(N)=37.5 K, at which Cr³+ (S=3/2) spins order in a 120° structure. In view of the theoretical expectation that the spin chirality cancels out in the simplest 120° spin structure, we discuss required conditions for the emergence of UAHE within Berry-phase mechanisms.

Uniaxial-strain control of nematic superconductivity in SrxBi2Se3.

Nematic states are characterized by rotational symmetry breaking without translational ordering. Recently, nematic superconductivity, in which the superconducting gap spontaneously lifts the rotational symmetry of the lattice, has been discovered. In nematic superconductivity, multiple superconducting domains with different nematic orientations can exist, and these domains can be controlled by a conjugate external stimulus. Domain engineering is quite common in magnets but has not been achieved in superconductors. Here, we report control of the nematic superconductivity and their domains of SrxBi2Se3, through externally-applied uniaxial stress. The suppression of subdomains indicates that it is the Δ4y state that is most favoured under compression along the basal Bi-Bi bonds. This fact allows us to determine the coupling parameter between the nematicity and lattice distortion. These results provide an inevitable step towards microscopic understanding and future utilization of the unique topological nematic superconductivity.

Evolution of Superconductivity with Sr-Deficiency in Antiperovskite Oxide Sr3-xSnO.

Bulk superconductivity was recently reported in the antiperovskite oxide Sr3-xSnO, with a possibility of hosting topological superconductivity. We investigated the evolution of superconducting properties such as the transition temperature Tc and the size of the diamagnetic signal, as well as normal-state electronic and crystalline properties, with varying the nominal Sr deficiency x0. Polycrystalline Sr3-xSnO was obtained up to x0 = 0:6 with a small amount of SrO impurities. The amount of impurities increases for x0 > 0.6, suggesting phase instability for high deficiency. Mössbauer spectroscopy reveals an unusual Sn4- ionic state in both stoichiometric and deficient samples. By objectively analyzing superconducting diamagnetism data obtained from a large number of samples, we conclude that the optimal x0 lies in the range 0.5 < x0 < 0.6. In all superconducting samples, two superconducting phases appear concurrently that originate from Sr3-xSnO but with varying intensities. These results clarify the Sr deficiency dependence of the normal and superconducting properties of the antiperovskite oxide Sr3-xSnO will ignite future work on this class of materials.

Superconductivity in heavily boron-doped silicon carbide.

The discoveries of superconductivity in heavily boron-doped diamond in 2004 and silicon in 2006 have renewed the interest in the superconducting state of semiconductors. Charge-carrier doping of wide-gap semiconductors leads to a metallic phase from which upon further doping superconductivity can emerge. Recently, we discovered superconductivity in a closely related system: heavily boron-doped silicon carbide. The sample used for that study consisted of cubic and hexagonal SiC phase fractions and hence this led to the question which of them participated in the superconductivity. Here we studied a hexagonal SiC sample, free from cubic SiC phase by means of x-ray diffraction, resistivity, and ac susceptibility.