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W. N. Hardy

Publications and source records attributed to W. N. Hardy.

At least 55 records · Page 3Linked to original sources

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

The condensation of an electron superfluid from a conventional metallic state at a critical temperature $T_c$ is described well by the BCS theory. In the underdoped copper-oxides, high-temperature superconductivity condenses instead 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, appearing at a temperature $T_{CDW}$ just above $T_c$. The near coincidence of $T_c$ and $T_{CDW}$, as well the coexistence and competition of CDW and superconducting order below $T_c$, suggests that they 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, $τ_{qp}$, as a function of temperature and magnetic field in underdoped HgBa$_{2}$CuO$_{4+δ}$ (Hg-1201) and YBa$_{2}$Cu$_{3}$O$_{6+x}$ (YBCO) single crystals by ultrafast time-resolved reflectivity. We find that $τ_{qp}(T)$ exhibits a local maximum in a small temperature window near $T_c$ 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 $T_c$ 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.

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Two types of nematicity in the phase diagram of the cuprate superconductor YBa$_2$Cu$_3$O$_y$

Nematicity has emerged as a key feature of cuprate superconductors, but its link to other fundamental properties such as superconductivity, charge order and the pseudogap remains unclear. Here we use measurements of transport anisotropy in YBa$_2$Cu$_3$O$_y$ to distinguish two types of nematicity. The first is associated with short-range charge-density-wave modulations in a doping region near $p = 0.12$. It is detected in the Nernst coefficient, but not in the resistivity. The second type prevails at lower doping, where there are spin modulations but no charge modulations. In this case, the onset of in-plane anisotropy - detected in both the Nernst coefficient and the resistivity - follows a line in the temperature-doping phase diagram that tracks the pseudogap energy. We discuss two possible scenarios for the latter nematicity.

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Change of carrier density at the pseudogap critical point of a cuprate superconductor

The pseudogap is a central puzzle of cuprate superconductors. Its connection to the Mott insulator at low doping $p$ remains ambiguous and its relation to the charge order that reconstructs the Fermi surface at intermediate $p$ is still unclear. Here we use measurements of the Hall coefficient in magnetic fields up to 88 T to show that Fermi-surface reconstruction by charge order in YBa$_2$Cu$_3$O$_y$ ends sharply at a critical doping $p = 0.16$, distinctly lower than the pseudogap critical point at $p^* = 0.19$. This shows that pseudogap and charge order are separate phenomena. We then find that the change of carrier density from $n = 1 + p$ in the conventional metal at high p to $n = p$ at low $p$ - a signature of the lightly doped cuprates - starts at $p^*$. This shows that pseudogap and antiferromagnetic Mott insulator are linked.

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Magnetic field controlled charge density wave coupling in underdoped YBa$_2$Cu$_3$O$_{6+x}$

The application of large magnetic fields ($B \sim B_{c2}$) to layered cuprates suppresses their high temperature superconducting behaviour and reveals competing ground states. In the widely-studied material YBa$_2$Cu$_3$O$_{6+x}$ (YBCO), underdoped ($p \sim 1/8$) samples show signatures of field-induced electronic and structural changes at low temperatures. However, the microscopic nature of the field-induced reconstruction and the high-field state are unclear. Here we report an x-ray study of the high-field charge density wave (CDW) in YBCO, for doping, $0.1 \lesssim p \lesssim 0.13$. For $p \sim 0.123$, we find that a field ($B \sim 10$~T) induces new CDW correlations along the CuO chain ($b$) direction only, leading to a 3-D ordered state along this direction at $B \sim 15$~T. The CDW signal along the $a$-direction is also enhanced by field, but does not develop a new pattern of correlations. We find that field modifies the coupling between the CuO$_2$ bilayers in the YBCO structure, and causes the sudden appearance of 3D CDW order. The mirror symmetry of individual bilayers is broken by the CDW at low and high fields, allowing recently suggested Fermi surface reconstruction.

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The nature of the charge density waves in under-doped YBa$_2$Cu$_3$O$_{6.54}$ revealed by X-ray measurements of the ionic displacements

All underdoped high-temperature cuprate superconductors appear to exhibit charge density wave (CDW) order, but both the underlying symmetry breaking and the origin of the CDW remain unclear. We use X-ray diffraction to determine the microscopic structure of the CDW in an archetypical cuprate YBa$_2$Cu$_3$O$_{6.54}$ at its superconducting transition temperature Tc ~ 60 K. We find that the CDWs present in this material break the mirror symmetry of the CuO2 bilayers. The ionic displacements in a CDW have two components: one perpendicular to the CuO$_2$ planes, and another parallel to these planes, which is out of phase with the first. The largest displacements are those of the planar oxygen atoms and are perpendicular to the CuO$_2$ planes. Our results allow many electronic properties of the underdoped cuprates to be understood. For instance, the CDW will lead to local variations in the doping (or electronic structure) giving an explicit explanation of the appearance of density-wave states with broken symmetry in scanning tunnelling microscopy (STM) and soft X-ray measurements.

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Magnetization of underdoped YBa$_2$Cu$_3$O$_{y}$ above the irreversibility field

Torque magnetization measurements on YBa$_2$Cu$_3$O$_{y}$ (YBCO) at doping $y=6.67$($p=0.12$), in DC fields ($B$) up to 33 T and temperatures down to 4.5 K, show that weak diamagnetism persists above the extrapolated irreversibility field $H_{\rm irr} (T=0) \approx 24$ T. The differential susceptibility $dM/dB$, however, is more rapidly suppressed for $B\gtrsim 16$ T than expected from the properties of the low field superconducting state, and saturates at a low value for fields $B \gtrsim 24$ T. In addition, torque measurements on a $p=0.11$ YBCO crystal in pulsed field up to 65 T and temperatures down to 8 K show similar behaviour, with no additional features at higher fields. We discuss several candidate scenarios to explain these observations: (a) superconductivity survives but is heavily suppressed at high field by competition with CDW order; (b) static superconductivity disappears near 24 T and is followed by a region of fluctuating superconductivity, which causes $dM/dB$ to saturate at high field; (c) the stronger 3D ordered CDW that sets in above 15 T may suppress the normal state spin susceptibility sufficiently to give an apparent diamagnetism of the magnitude observed.

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Thermodynamic signature of a magnetic-field-driven phase transition within the superconducting state of an underdoped high-temperature superconductor

More than a quarter century after the discovery of the high temperature superconductor (HTS) YBa$_2$Cu$_3$O$_{6+δ}$ (YBCO) studies continue to uncover complexity in its phase diagram. In addition to HTS and the pseudogap there is growing evidence for multiple phases with boundaries which are functions of temperature ($T$), doping (p) and magnetic field. Here we report the low temperature electronic specific heat (C$_{elec}$) of YBCO6.47 (p=0.08) up to a magnetic field (H) of 34.5 teslas (T), a poorly understood region of the underdoped H-$T$-p phase space. We observe two regimes: below a characteristic magnetic field H'$\approx$10 T, C$_{elec}/T$ obeys an expected H$^{1/2}$ behavior, however, near H' there is a sharp inflection followed by a linear-in-H behavior. H' rests deep within the superconducting phase and the linear-in-H behavior is observed in the zero resistance regime. In the limit of zero temperature, C$_{elec}/T$ is proportional to the zero-energy electronic density of states. Thus this inflection is evidence of a magnetic-field-driven quantum phase transition.

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Signatures of New $d$-Wave Vortex Physics in Overdoped Tl$_2$Ba$_2$CuO$_{6+x}$ Revealed by TF-$μ^+$SR

The spontaneous expulsion of applied magnetic field, the Meissner effect, is a defining feature of superconductors; in Type-II superconductors above the lower critical field, this screening takes the form of a lattice of magnetic flux vortices. Using implanted spin-1/2 positive muons, one can measure the vortex lattice field distribution through the spin precession and deduce key parameters of the superconducting ground state, and thereby fundamental properties of the superconducting pairing. Muon spin rotation/relaxation ($μ$SR) experiments have indeed revealed much interesting physics in the underdoped cuprates, where superconductivity is closely related to, or coexistent with, disordered or fluctuating magnetic and charge excitations. Such complications should be absent in overdoped cuprates, which are believed to exhibit conventional Fermi liquid behaviour. These first transverse field (TF)-$μ^+$SR experiments on heavily-overdoped single crystals reveal a superfluid density exhibiting a clear inflection point near 0.5$T_c$, with a striking doping-independent scaling. This reflects hitherto unrecognized physics intrinsic to $d$-wave vortices, evidently generic to the cuprates, and may offer fundamentally new insights into their still-mysterious superconductivity.

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Onset field for Fermi-surface reconstruction in the cuprate superconductor YBCO

Quantum oscillations and negative Hall and Seebeck coefficients at low temperature and high magnetic field have shown the Fermi surface of underdoped cuprates to contain a small closed electron pocket. It is thought to result from a reconstruction by charge order, but whether it is the order seen by NMR and ultrasound above a threshold field or the short-range modulations seen by X-ray diffraction in zero field is unclear. Here we use measurements of the thermal Hall conductivity in YBCO to show that Fermi-surface reconstruction occurs only above a sharply defined onset field, equal to the transition field seen in ultrasound. This reveals that electrons do not experience long-range broken translational symmetry in the zero-field ground state, and hence in zero field there is no quantum critical point for the onset of charge order as a function of doping.

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Normal-state nodal electronic structure in underdoped high-Tc copper oxides

An outstanding problem in the field of high-transition-temperature (high Tc) superconductivity is the identification of the normal state out of which superconductivity emerges in the mysterious underdoped regime. The normal state uncomplicated by thermal fluctuations is effectively accessed by the use of applied magnetic fields sufficiently strong to suppress long-range superconductivity at low temperatures. Proposals in which the normal ground state is characterised by small Fermi surface pockets that exist in the absence of symmetry breaking have been superseded by models based on the existence of a superlattice that breaks the translational symmetry of the underlying lattice. Recently, a charge superlattice model that positions a small electron-like Fermi pocket in the vicinity of the nodes (where the superconducting gap is minimum) has been proposed a replacement for the prevalent superlattice models that position the Fermi pocket in the vicinity of the pseudogap at the antinodes (where the superconducting gap is maximum). Although some ingredients of symmetry breaking have been recently revealed by crystallographic studies, their relevance to the electronic structure remains unresolved. Here we report angle-resolved quantum oscillation measurements in the underdoped copper oxide YBa2Cu3O6+x. These measurements reveal a normal ground state comprising electron-like Fermi surface pockets located in the vicinity of the superconducting gap minima (or nodes), and further point to an underlying superlattice structure of low frequency and long wavelength with features in common with the charge order identified recently by complementary spectroscopic techniques.

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Three-Dimensional Charge Density Wave Order in YBa2Cu3O6.67 at High Magnetic Fields

Charge density wave (CDW) correlations have recently been shown to universally exist in cuprate superconductors. However, their nature at high fields inferred from nuclear magnetic resonance is distinct from that measured by x-ray scattering at zero and low fields. Here we combine a pulsed magnet with an x-ray free electron laser to characterize the CDW in YBa2Cu3O6.67 via x-ray scattering in fields up to 28 Tesla. While the zero-field CDW order, which develops below T ~ 150 K, is essentially two-dimensional, at lower temperature and beyond 15 Tesla, another three-dimensionally ordered CDW emerges. The field-induced CDW onsets around the zero-field superconducting transition temperature, yet the incommensurate in-plane ordering vector is field-independent. This implies that the two forms of CDW and high-temperature superconductivity are intimately linked.

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Separation of magnetic and superconducting behaviour in YBCO6.33 (Tc=8.4 K)

Neutron scattering from high-quality YBa2Cu3O6.33 (YBCO6.33) single crystals with a Tc of 8.4 K shows no evidence of a coexistence of superconductivity with long-range antiferromagnetic order at this very low, near-critical doping of p~0.055. However, we find short-range three dimensional spin correlations that develop at temperatures much higher than Tc. Their intensity increases smoothly on cooling and shows no anomaly that might signify a Neel transition. The system remains subcritical with spins correlated over only one and a half unit cells normal to the planes. At low energies the short-range spin response is static on the microvolt scale. The excitations out of this ground state give rise to an overdamped spectrum with a relaxation rate of 3 meV. The transition to the superconducting state below Tc has no effect on the spin correlations. The elastic interplanar spin response extends over a length that grows weakly but fails to diverge as doping is moved towards the superconducting critical point. Any antiferromagnetic critical point likely lies outside the superconducting dome. The observations suggest that conversion from Neel long-range order to a spin glass texture is a prerequisite to formation of paired superconducting charges. We show that while pc =0.052 is a critical doping for superconducting pairing, it is not for spin order.

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The symmetry of charge order in cuprates

Charge-ordered ground states permeate the phenomenology of 3d-based transition metal oxides, and more generally represent a distinctive hallmark of strongly-correlated states of matter. The recent discovery of charge order in various cuprate families fueled new interest into the role played by this incipient broken symmetry within the complex phase diagram of high-Tc superconductors. Here we use resonant X-ray scattering to resolve the main characteristics of the charge-modulated state in two cuprate families: Bi2201 and YBCO. We detect no signatures of spatial modulations along the nodal direction in Bi2201, thus clarifying the inter-unit-cell momentum-structure of charge order. We also resolve the intra-unit-cell symmetry of the charge ordered state, which is revealed to be best represented by a bond-order with modulated charges on the O-2p orbitals and a prominent d-wave character. These results provide insights on the microscopic description of charge order in cuprates, and on its origin and interplay with superconductivity.

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Broken translational and rotational symmetry via charge stripe order in underdoped YBCO

Following the early discovery of stripe-like order in La-based copper-oxide superconductors, charge ordering instabilities were observed in all cuprate families. However, it has proven difficult to distinguish between uni- (stripes) and bi-directional (checkerboard) charge order in Y- and Bi-based materials. Here we use resonant x-ray scattering (RXS) to measure the two-dimensional structure factor in YBCO, in reciprocal space. Our data reveal the presence of charge stripe order, i.e. locally unidirectional density waves, suggesting it as the true microscopic nature of charge modulations in cuprates. At the same time, we find that the well-established competition between charge order and superconductivity is stronger for charge correlations across than along the stripes, which provides additional evidence for the intrinsic unidirectional nature of the charge order.

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Quasiparticle mass enhancement approaching optimal doping in a high-Tc superconductor

In the quest for superconductors with high transition temperatures (T$_\mathrm{c}$s), one emerging motif is that unconventional superconductivity is enhanced by fluctuations of a broken-symmetry phase near a quantum-critical point. While recent experiments have suggested the existence of the requisite broken symmetry phase in the high-T$_\mathrm{c}$ cuprates, the signature of quantum-critical fluctuations in the electronic structure has thus far remained elusive, leaving their importance for high-T$_\mathrm{c}$ superconductivity in question. We use magnetic fields exceeding 90 tesla to access the underlying metallic state of the cuprate YBa2Cu3O6+$_δ$ over an unprecedented range of doping, and magnetic quantum oscillations reveal a strong enhancement in the quasiparticle effective mass toward optimal doping. This mass enhancement is a characteristic signature of quantum criticality, and identifies a quantum-critical point at p$_{crit}$ $\approx$ 0.18. This point also represents the juncture of the vanishing pseudogap energy scale and the disappearance of Kerr rotation, the negative Hall coefficient, and the recently observed charge order, suggesting a mechanism of high-T$_\mathrm{c}$ that is strongest when these definitive experimental signatures of the underdoped cuprates converge at a quantum critical point.

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Incipient charge order observed by NMR in the normal state of YBa2Cu3Oy

The pseudogap regime of high-temperature cuprates harbours diverse manifestations of electronic ordering whose exact nature and universality remain debated. Here, we show that the short-ranged charge order recently reported in the normal state of YBa2Cu3Oy corresponds to a truly static modulation of the charge density. We also show that this modulation impacts on most electronic properties, that it appears jointly with intra-unit-cell nematic, but not magnetic, order, and that it exhibits differences with the charge density wave observed at lower temperatures in high magnetic fields. These observations prove mostly universal, they place new constraints on the origin of the charge density wave and they reveal that the charge modulation is pinned by native defects. Similarities with results in layered metals such as NbSe2, in which defects nucleate halos of incipient charge density wave at temperatures above the ordering transition, raise the possibility that order-parameter fluctuations, but no static order, would be observed in the normal state of most cuprates if disorder were absent.

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Evidence for a small hole pocket in the Fermi surface of underdoped YBa2Cu3Oy

The Fermi surface of a metal is the fundamental basis from which its properties can be understood. In underdoped cuprate superconductors, the Fermi surface undergoes a reconstruction that produces a small electron pocket, but whether there is another, as yet undetected portion to the Fermi surface is unknown. Establishing the complete topology of the Fermi surface is key to identifying the mechanism responsible for its reconstruction. Here we report the discovery of a second Fermi pocket in underdoped YBa2Cu3Oy, detected as a small quantum oscillation frequency in the thermoelectric response and in the c-axis resistance. The field-angle dependence of the frequency demonstrates that it is a distinct Fermi surface and the normal-state thermopower requires it to be a hole pocket. A Fermi surface consisting of one electron pocket and two hole pockets with the measured areas and masses is consistent with a Fermi-surface reconstruction caused by the charge-density-wave order observed in YBa2Cu3Oy, provided other parts of the reconstructed Fermi surface are removed by a separate mechanism, possibly the pseudogap.

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Impact of Quenched Oxygen Disorder on Charge Density Wave Order in YBa$_2$Cu$_3$O$_{6+x}$

The competition between superconductivity and charge density wave (CDW) order in underdoped cuprates has now been widely reported, but the role of disorder in this competition has yet to be fully resolved. A central question is whether disorder sets the length scale of the CDW order, for instance by pinning charge density fluctuations or disrupting an otherwise long range order. Using resonant soft x-ray scattering, we investigate the sensitivity of CDW order in YBa$_2$Cu$_3$O$_{6+x}$ (YBCO) to varying levels of oxygen disorder. We find that quench cooling YBCO$_{6.67}$ (YBCO$_{6.75}$) crystals to destroy their o-V and o-VIII (o-III) chains decreases the intensity of the CDW superlattice peak by a factor of 1.9 (1.3), but has little effect on the CDW correlation length, incommensurability, and temperature dependence. This reveals that while quenched oxygen disorder influences the CDW order parameter, the spatial extent of the CDW order is insensitive to the level of quenched oxygen disorder and may instead be a consequence of competition with superconductivity.

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