Local inversion-symmetry breaking in a bismuthate high-Tc superconductor.

The doped perovskite BaBiO3 exhibits a maximum superconducting transition temperature (Tc) of 34 K and was the first high-Tc oxide to be discovered, yet pivotal questions regarding the nature of both the metallic and superconducting states remain unresolved. Although it is generally thought that superconductivity in the bismuthates is of the conventional s-wave type, the pairing mechanism is still debated, with strong electron-phonon coupling and bismuth valence or bond disproportionation possibly playing a role. Here we use diffuse x-ray scattering and Monte Carlo modeling to study the local structure of Ba1-xKxBiO3 across its insulator-metal boundary. We find no evidence for either long- or short-range disproportionation, which resolves a major conundrum, as disproportionation and the related polaronic effects are likely not relevant for the metallic and superconducting states. Instead, we uncover nanoscale structural correlations that break inversion symmetry, with far-reaching implications for the electronic physics. This unexpected finding furthermore establishes that the bismuthates belong to the broader classes of materials with hidden spin-orbit coupling and a tendency towards inversion-breaking displacements.

Unconventional short-range structural fluctuations in cuprate superconductors.

The interplay between structural and electronic degrees of freedom in complex materials is the subject of extensive debate in physics and materials science. Particularly interesting questions pertain to the nature and extent of pre-transitional short-range order in diverse systems ranging from shape-memory alloys to unconventional superconductors, and how this microstructure affects macroscopic properties. Here we use neutron and X-ray diffuse scattering to uncover universal structural fluctuations in La2-xSrxCuO4 and Tl2Ba2CuO6+δ, two cuprate superconductors with distinct point disorder effects and with optimal superconducting transition temperatures that differ by more than a factor of two. The fluctuations are present in wide doping and temperature ranges, including compositions that maintain high average structural symmetry, and they exhibit unusual, yet simple scaling behaviour. The scaling regime is robust and universal, similar to the well-known critical fluctuations close to second-order phase transitions, but with a distinctly different physical origin. We relate this behaviour to pre-transitional phenomena in a broad class of systems with structural and magnetic transitions, and propose an explanation based on rare structural fluctuations caused by intrinsic nanoscale inhomogeneity. We also uncover parallels with superconducting fluctuations, which indicates that the underlying inhomogeneity plays an important role in cuprate physics.

Uniaxial Strain Control of Bulk Ferromagnetism in Rare-Earth Titanates.

The perovskite rare-earth titanates are model Mott insulators with magnetic ground states that are very sensitive to structural distortions. These distortions couple strongly to the orbital degrees of freedom and, in principle, it should be possible to tune the superexchange and the magnetic transition with strain. We investigate the representative system (Y,La,Ca)TiO_{3}, which exhibits low crystallographic symmetry and no structural instabilities. From magnetic susceptibility measurements of the Curie temperature, we demonstrate direct, reversible, and continuous control of ferromagnetism by influencing the TiO_{6} octahedral tilts and rotations with uniaxial strain. The relative change in T_{C} as a function of strain is well described by ab initio calculations, which provides detailed understanding of the complex interactions among structural, orbital, and magnetic properties in rare-earth titanates. The demonstrated manipulation of octahedral distortions opens up far-reaching possibilities for investigations of electron-lattice coupling, competing ground states, and magnetic quantum phase transitions in a wide range of quantum materials.

Enhanced superconductivity and ferroelectric quantum criticality in plastically deformed strontium titanate.

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach using irreversible, plastic deformation of single crystals. We show that compressive plastic deformation induces low-dimensional superconductivity well above the superconducting transition temperature (Tc) of undeformed SrTiO3, with evidence of possible superconducting correlations at temperatures two orders of magnitude above the bulk Tc. The enhanced superconductivity is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe deformation-induced signatures of quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order using Raman scattering. Our results suggest that strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence Tc, consistent with a theory of superconductivity enhanced by soft polar fluctuations. Our results demonstrate the potential of plastic deformation and dislocation engineering for the manipulation of electronic properties of quantum materials.

Diagonal nematicity in the pseudogap phase of HgBa2CuO4+δ.

The pseudogap phenomenon in the cuprates is arguably the most mysterious puzzle in the field of high-temperature superconductivity. The tetragonal cuprate HgBa2CuO4+δ, with only one CuO2 layer per primitive cell, is an ideal system to tackle this puzzle. Here, we measure the magnetic susceptibility anisotropy within the CuO2 plane with exceptionally high-precision magnetic torque experiments. Our key finding is that a distinct two-fold in-plane anisotropy sets in below the pseudogap temperature T*, which provides thermodynamic evidence for a nematic phase transition with broken four-fold symmetry. Surprisingly, the nematic director orients along the diagonal direction of the CuO2 square lattice, in sharp contrast to the bond nematicity along the Cu-O-Cu direction. Another remarkable feature is that the enhancement of the diagonal nematicity with decreasing temperature is suppressed around the temperature at which short-range charge-density-wave formation occurs. Our result suggests a competing relationship between diagonal nematic and charge-density-wave order in HgBa2CuO4+δ.

Universal superconducting precursor in three classes of unconventional superconductors.

A pivotal challenge posed by unconventional superconductors is to unravel how superconductivity emerges upon cooling from the generally complex normal state. Here, we use nonlinear magnetic response, a probe that is uniquely sensitive to the superconducting precursor, to uncover remarkable universal behaviour in three distinct classes of oxide superconductors: strontium titanate, strontium ruthenate, and the cuprate high-Tc materials. We find unusual exponential temperature dependence of the diamagnetic response above the transition temperature Tc, with a characteristic temperature scale that strongly varies with Tc. We correlate this scale with the sensitivity of Tc to local stress and show that it is influenced by intentionally-induced structural disorder. The universal behaviour is therefore caused by intrinsic, self-organized structural inhomogeneity, inherent to the oxides' perovskite-based structure. The prevalence of such inhomogeneity has far-reaching implications for the interpretation of electronic properties of perovskite-related oxides in general.

Signatures of Enhanced Superconducting Phase Coherence in Optimally Doped Bi_{2}Sr_{2}Y_{0.08}Ca_{0.92}Cu_{2}O_{8+δ} Driven by Midinfrared Pulse Excitations.

Optimally doped cuprate are characterized by the presence of superconducting fluctuations in a relatively large temperature region above the critical transition temperature. We reveal here that the effect of thermal disorder, which decreases the condensate phase coherence at equilibrium, can be dynamically contrasted by photoexcitation with ultrashort midinfrared pulses. In particular, our findings reveal that light pulses with photon energy comparable to the amplitude of the superconducting gap and polarized in plane along the copper-copper direction can dynamically enhance the optical response associated with the onset of superconductivity. We propose that this effect can be rationalized by an effective d-wave BCS model, which reveals that midinfrared pulses result in a transient increase of the phase coherence.

Unusual behavior of cuprates explained by heterogeneous charge localization.

The discovery of high-temperature superconductivity in cuprates ranks among the major scientific milestones of the past half century, yet pivotal questions regarding the complex phase diagram of these materials remain unanswered. Generally thought of as doped charge-transfer insulators, these complex oxides exhibit pseudogap, strange-metal, superconducting, and Fermi liquid behavior with increasing hole-dopant concentration. Motivated by recent experimental observations, here we introduce a phenomenological model wherein exactly one hole per planar copper-oxygen unit is delocalized with increasing doping and temperature. The model is percolative in nature, with parameters that are highly consistent with experiments. It comprehensively captures key unconventional experimental results, including the temperature and the doping dependence of the pseudogap phenomenon, the strange-metal linear temperature dependence of the planar resistivity, and the doping dependence of the superfluid density. The success and simplicity of the model greatly demystify the cuprate phase diagram and point to a local superconducting pairing mechanism.

Hole pocket-driven superconductivity and its universal features in the electron-doped cuprates.

After three decades of intensive research attention, the emergence of superconductivity in cuprates remains an unsolved puzzle. One major challenge has been to arrive at a satisfactory understanding of the unusual metallic "normal state" from which the superconducting state emerges upon cooling. A second challenge has been to achieve a unified understanding of hole- and electron-doped compounds. Here, we report detailed magnetoresistance measurements for the archetypal electron-doped cuprate Nd2-x Ce x CuO4+δ that, in combination with previous data, provide crucial links between the normal and superconducting states and between the electron- and hole-doped parts of the phase diagram. The characteristics of the normal state (magnetoresistance, quantum oscillations, and Hall coefficient) and those of the superconducting state (superfluid density and upper critical field) consistently indicate two-band (electron and hole) features and point to hole pocket-driven superconductivity in these nominally electron-doped materials. We show that the approximate Uemura scaling between the superconducting transition temperature and the superfluid density found for hole-doped cuprates also holds for the small hole component of the superfluid density in electron-doped cuprates.

Hidden Fermi-liquid Charge Transport in the Antiferromagnetic Phase of the Electron-Doped Cuprate Superconductors.

Systematic analysis of the planar resistivity, Hall effect, and cotangent of the Hall angle for the electron-doped cuprates reveals underlying Fermi-liquid behavior even deep in the antiferromagnetic part of the phase diagram. The transport scattering rate exhibits a quadratic temperature dependence, and is nearly independent of doping and compound and carrier type (electrons versus holes), and hence is universal. Our analysis moreover indicates that the material-specific resistivity upturn at low temperatures and low doping has the same origin in both electron- and hole-doped cuprates.

Single reconstructed Fermi surface pocket in an underdoped single-layer cuprate superconductor.

The observation of a reconstructed Fermi surface via quantum oscillations in hole-doped cuprates opened a path towards identifying broken symmetry states in the pseudogap regime. However, such an identification has remained inconclusive due to the multi-frequency quantum oscillation spectra and complications accounting for bilayer effects in most studies. We overcome these impediments with high-resolution measurements on the structurally simpler cuprate HgBa2CuO4+δ (Hg1201), which features one CuO2 plane per primitive unit cell. We find only a single oscillatory component with no signatures of magnetic breakdown tunnelling to additional orbits. Therefore, the Fermi surface comprises a single quasi-two-dimensional pocket. Quantitative modelling of these results indicates that a biaxial charge density wave within each CuO2 plane is responsible for the reconstruction and rules out criss-crossed charge stripes between layers as a viable alternative in Hg1201. Lastly, we determine that the characteristic gap between reconstructed pockets is a significant fraction of the pseudogap energy.

The rate of quasiparticle recombination probes the onset of coherence in cuprate superconductors.

In the underdoped copper-oxides, high-temperature superconductivity condenses from a nonconventional metallic "pseudogap" phase that exhibits a variety of non-Fermi liquid properties. Recently, it has become clear that a charge density wave (CDW) phase exists within the pseudogap regime. This CDW coexists and competes with superconductivity (SC) below the transition temperature Tc, suggesting that these two orders are intimately related. Here we show that the condensation of the superfluid from this unconventional precursor is reflected in deviations from the predictions of BSC theory regarding the recombination rate of quasiparticles. We report a detailed investigation of the quasiparticle (QP) recombination lifetime, τqp, as a function of temperature and magnetic field in underdoped HgBa2CuO(4+δ) (Hg-1201) and YBa2Cu3O(6+x) (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that τqp(T) exhibits a local maximum in a small temperature window near Tc that is prominent in underdoped samples with coexisting charge order and vanishes with application of a small magnetic field. We explain this unusual, non-BCS behavior by positing that Tc marks a transition from phase-fluctuating SC/CDW composite order above to a SC/CDW condensate below. Our results suggest that the superfluid in underdoped cuprates is a condensate of coherently-mixed particle-particle and particle-hole pairs.

Commensurate antiferromagnetic excitations as a signature of the pseudogap in the tetragonal high-Tc cuprate HgBa2CuO(4+δ).

Antiferromagnetic correlations have been argued to be the cause of the d-wave superconductivity and the pseudogap phenomena exhibited by the cuprates. Although the antiferromagnetic response in the pseudogap state has been reported for a number of compounds, there exists no information for structurally simple HgBa2CuO(4+δ). Here we report neutron-scattering results for HgBa2CuO(4+δ) (superconducting transition temperature Tc≈71 K, pseudogap temperature T*≈305 K) that demonstrate the absence of the two most prominent features of the magnetic excitation spectrum of the cuprates: the X-shaped 'hourglass' response and the resonance mode in the superconducting state. Instead, the response is Y-shaped, gapped and significantly enhanced below T*, and hence a prominent signature of the pseudogap state.

Hourglass Dispersion and Resonance of Magnetic Excitations in the Superconducting State of the Single-Layer Cuprate HgBa_{2}CuO_{4+δ} Near Optimal Doping.

We use neutron scattering to study magnetic excitations near the antiferromagnetic wave vector in the underdoped single-layer cuprate HgBa_{2}CuO_{4+δ} (superconducting transition temperature T_{c}≈88 K, pseudogap temperature T^{*}≈220 K). The response is distinctly enhanced below T^{*} and exhibits a Y-shaped dispersion in the pseudogap state, whereas the superconducting state features an X-shaped (hourglass) dispersion and a further resonancelike enhancement. A large spin gap of about 40 meV is observed in both states. This phenomenology is reminiscent of that exhibited by bilayer cuprates. The resonance spectral weight, irrespective of doping and compound, scales linearly with the putative binding energy of a spin exciton described by an itinerant-spin formalism.

Charge order and its connection with Fermi-liquid charge transport in a pristine high-T(c) cuprate.

Electronic inhomogeneity appears to be an inherent characteristic of the enigmatic cuprate superconductors. Here we report the observation of charge-density-wave correlations in the model cuprate superconductor HgBa2CuO(4+δ) (T(c)=72 K) via bulk Cu L3-edge-resonant X-ray scattering. At the measured hole-doping level, both the short-range charge modulations and Fermi-liquid transport appear below the same temperature of about 200 K. Our result points to a unifying picture in which these two phenomena are preceded at the higher pseudogap temperature by q=0 magnetic order and the build-up of significant dynamic antiferromagnetic correlations. The magnitude of the charge modulation wave vector is consistent with the size of the electron pocket implied by quantum oscillation and Hall effect measurements for HgBa2CuO(4+δ) and with corresponding results for YBa2Cu3O(6+δ), which indicates that charge-density-wave correlations are universally responsible for the low-temperature quantum oscillation phenomenon.

In-plane magnetoresistance obeys Kohler's rule in the pseudogap phase of cuprate superconductors.

We report in-plane resistivity (ρ) and transverse magnetoresistance (MR) measurements for underdoped HgBa(2)CuO(4+δ) (Hg1201). Contrary to the long-standing view that Kohler's rule is strongly violated in underdoped cuprates, we find that it is in fact satisfied in the pseudogap phase of Hg1201. The transverse MR shows a quadratic field dependence, δρ/ρ(0)=aH(2), with a(T)∝T(-4). In combination with the observed ρ∝T(2) dependence, this is consistent with a single Fermi-liquid quasiparticle scattering rate. We show that this behavior is typically masked in cuprates with lower structural symmetry or strong disorder effects.

High-energy anomaly in the angle-resolved photoemission spectra of Nd(2-x)Ce(x)CuO4: evidence for a matrix element effect.

We use polarization-dependent angle-resolved photoemission spectroscopy (ARPES) to study the high-energy anomaly (HEA) in the dispersion of Nd(2-x)Ce(x)CuO4, x=0.123. We find that at particular photon energies the anomalous, waterfall-like dispersion gives way to a broad, continuous band. This suggests that the HEA is a matrix element effect: it arises due to a suppression of the intensity of the broadened quasiparticle band in a narrow momentum range. We confirm this interpretation experimentally, by showing that the HEA appears when the matrix element is suppressed deliberately by changing the light polarization. Calculations of the matrix element using atomic wave functions and simulation of the ARPES intensity with one-step model calculations provide further evidence for this scenario. The possibility to detect the full quasiparticle dispersion further allows us to extract the high-energy self-energy function near the center and at the edge of the Brillouin zone.

Photo-enhanced antinodal conductivity in the pseudogap state of high-Tc cuprates.

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe, we are able to track the dynamics of the dielectric function and unveil an anomalous decrease in the scattering rate of the charge carriers in a pseudogap-like region of the temperature (T) and hole-doping (p) phase diagram. In this region, delimited by a well-defined T*neq(p) line, the photoexcitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasiparticles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between nodal quasiparticles and antinodal excitations.

Doping-dependent photon scattering resonance in the model high-temperature superconductor HgBa2CuO4+δ revealed by Raman scattering and optical ellipsometry.

We study the model high-temperature superconductor HgBa(2)CuO(4+δ) with electronic Raman scattering and optical ellipsometry over a wide doping range. The dependence of the resonant Raman cross section on the incident photon energy changes drastically as a function of doping, in a manner that corresponds to a rearrangement of the interband optical transitions seen with ellipsometry. This doping-dependent Raman resonance allows us to reconcile the apparent discrepancy between Raman and x-ray detection of magnetic fluctuations in superconducting cuprates. Intriguingly, the strongest variation occurs across the doping level where the antinodal superconducting gap appears to reach its maximum.

Absence of static loop-current magnetism at the apical oxygen site in HgBa2CuO4+δ from NMR.

The simple structure of HgBa(2)CuO(4+δ) (Hg1201) is ideal among cuprates for study of the pseudogap phase as a broken symmetry state. We have performed (17)O nuclear magnetic resonance on an underdoped Hg1201 crystal with a transition temperature of 74 K to look for circulating loop currents proposed theoretically and inferred from neutron scattering. The narrow spectra preclude static local fields in the pseudogap phase at the apical site, suggesting that the moments observed with neutrons are fluctuating. The nuclear magnetic resonance frequency shifts are consistent with a dipolar field from the Cu(2+) site.