Underdoped YBa2Cu3O6 Research Articles

The in- and out-of-plane magnetisation of highly underdoped YBa2Cu3O6+x single crystals

Previously we have shown how measurements of static magnetic susceptibility χc(T) of YBa2Cu3O6+x single crystals for magnetic fields applied along the c-axis, and χab(T) for fields in the ab-plane, can give useful information about their thermodynamic properties which are still being hotly debated. SQUID magnetometry above the superconducting (s/c) transition temperature Tc is used for larger crystals, while piezolever torque magnetometry gives χc(T)-χab(T) for tiny crystals. Here we present new data for more heavily under-doped crystals with hole concentrations per CuO2 plane, p =0.058 to 0.073. We again find that the T-dependent anisotropy well above Tc arises from the pseudogap and the g-factor anisotropy, while at lower T there are Gaussian s/c fluctuations with a strong cut-off. This is possibly a different region where neutron scattering studies give evidence for competition between incommensurate magnetic short-range order and superconductivity. We have studied crystals with three values of x, measuring χc(T) and χab(T) immediately after fixing x by quenching on to a copper block and again after allowing sufficient time at room temperature for the Cu-O chains to order. Thus, we report data for three pairs of underdoped (UD) crystals with Tc ranging from 13 to 36 K, namely UD13 and UD20, UD15 and UD30, UD23 and UD36. As found previously for polycrystalline samples, ordering the Cu-O chains increases Tc and substantially reduces the Curie term. These are isotropic, in contrast to the Pauli-like susceptibility from the CuO2 planes where there is g factor anisotropy, and this allows us to make a powerful novel analysis. At higher T, χc(T)- χab(T) varies as a + bT where the bT term arises from the pseudogap. At lower T, deviations from this behaviour are analysed in terms of 2D or 3D Gaussian s/c fluctuations to obtain in-plane coherence lengths and upper critical fields as T→0.

Normal-state charge transport in YBa2Cu3O6.67 under uniaxial stress

To provide a foundation for theoretical models of high-temperature superconductivity, experimental research has sought to establish correspondences between macroscopic transport coefficients on the one hand, and atomic-scale correlation functions measured by spectroscopic and scattering probes on the other hand. This research avenue has been confounded by the gradual onset of electronic ordering phenomena and of the corresponding transport anomalies. We report measurements of the uniaxial-stress dependence of the normal-state resistivity and Hall coefficient of the underdoped high-temperature superconductor YBa2Cu3O6.67. We observe a remarkable correspondence between the differential stress responses of the transport coefficients and resonant X-ray diffraction features indicative of charge ordering, which parallels the phenomenology of classical charge-density-wave compounds. However, our observations imply that static charge order is not responsible for a sign reversal of the Hall coefficient, and suggest that the interplay with liquid-like, dynamical charge correlations is essential for the prominent transport anomalies in the underdoped cuprates.

Hidden magnetic texture in the pseudogap phase of high-Tc YBa2Cu3O6.6

Despite decades of intense research, the enigmatic pseudo-gap (PG) phase of superconducting cuprates remains unsolved. In the last 15 years, various symmetry breaking states were discovered in the PG phase, including an intra-unit cell (IUC) magnetism, which preserves the lattice translational (LT) symmetry but breaks the time-reversal and parity symmetries, and an additional incipient charge density wave breaking the LT symmetry. However, none of these states can (alone) account for the partial gapping of the Fermi surface. Here we report a hidden LT-breaking magnetism using polarized neutron diffraction. Our measurements reveal magnetic correlations, in two different underdoped YBa2Cu3O6.6 single crystals that set in at the PG onset temperature with (i) a planar propagation wave vector (π, 0) ≡ (0, π), yielding a doubling or quadrupling of the magnetic unit cell and (ii) magnetic moments mainly pointing perpendicular to the CuO2 layers. The LT-breaking magnetism is at short-range suggesting the formation of clusters of 5–6 unit cells. Together with the previously reported IUC magnetism, it yields a hidden magnetic texture of the CuO2 unit cells hosting loop currents, forming large supercells that may be helpful for elucidating the PG puzzle.

Restored strange metal phase through suppression of charge density waves in underdoped YBa2Cu3O7-δ.

The normal state of optimally doped cuprates is dominated by the “strange metal” phase that shows a linear temperature (T) dependence of the resistivity persisting down to the lowest T. For underdoped cuprates, this behavior is lost below the pseudogap temperature T*, where charge density waves (CDWs), together with other intertwined local orders, characterize the ground state. We found that the T-linear resistivity of highly strained, ultrathin, underdoped YBa2Cu3O7–δ films is restored when the CDW amplitude, detected by resonant inelastic x-ray scattering, is suppressed. This observation suggests an intimate connection between the onset of CDWs and the departure from T-linear resistivity in underdoped cuprates. Our results illustrate the potential of using strain control to manipulate the ground state of quantum materials.

Emergent charge order from correlated electron-phonon physics in cuprates

Charge-density wave order is now understood to be a widespread feature of underdoped cuprate high-temperature superconductors, although its origins remain unclear. While experiments suggest that the charge-ordering wavevector is determined by Fermi-surface nesting, the relevant sections of the Fermi surface are featureless and provide no clue as to the underlying mechanism. Here, focusing on underdoped YBa2Cu3O6+x, we propose that charge-density waves form from the incipient softening of a bond-buckling phonon. The momentum dependence of its coupling to itinerant electrons favourably selects the wavevector found in experiments. But, it requires quasiparticle renormalization by strong electronic correlations to enable a unique enhancement of the charge susceptibility near the B1g-phonon selected wavevector. The B1g phonon frequency softens by a few percent, and finite-range charge-density wave correlations will form locally, if nucleated by defects or dopant disorder. These results suggest that underdoped cuprates cannot be understood in the context of strong electronic correlations alone.

Infrared spectroscopy study of the in-plane response of YBa2Cu3O6.6 in magnetic fields up to 30 Tesla

With Terahertz and Infrared spectroscopy we studied the in-plane response of an underdoped YBa2Cu3O6.6 single crystal with Tc=58(1) K in high magnetic fields up to B=30 Tesla applied along the c-axis. Our goal was to investigate the field-induced suppression of superconductivity and to observe the signatures of the three dimensional (3d) incommensurate copper charge density wave (Cu-CDW) which was previously shown to develop at such high magnetic fields. Our study confirms that a B-field in excess of 20 Tesla gives rise to a full suppression of the macroscopic response of the superconducting condensate. However, it reveals surprisingly weak signatures of the 3d Cu-CDW at high magnetic fields. At 30 Tesla there is only a weak reduction of the spectral weight of the Drude-response (by about 3%) that is accompanied by an enhancement of two narrow electronic modes around 90 and 240 cm-1, that are interpreted in terms of pinned phase modes of the CDW along the a- and b-direction, respectively, and of the so-called mid-infrared (MIR) band. The pinned phased modes and the MIR band are strong features already without magnetic field which suggests that prominent but short-ranged and slowly fluctuating (compared to the picosecond IR-time scale) CDW correlations exist all along, i.e., even at zero magnetic field.

Stabilization of three-dimensional charge order in YBa2Cu3O6+x via epitaxial growth

Incommensurate charge order (CO) has been identified as the leading competitor of high-temperature superconductivity in all major families of layered copper oxides, but the perplexing variety of CO states in different cuprates has confounded investigations of its impact on the transport and thermodynamic properties. The three-dimensional (3D) CO observed in YBa2Cu3O6+x in high magnetic fields is of particular interest, because quantum transport measurements have revealed detailed information about the corresponding Fermi surface. Here we use resonant X-ray scattering to demonstrate 3D-CO in underdoped YBa2Cu3O6+x films grown epitaxially on SrTiO3 in the absence of magnetic fields. The resonance profiles indicate that Cu sites in the charge-reservoir layers participate in the CO state, and thus efficiently transmit CO correlations between adjacent CuO2 bilayer units. The results offer fresh perspectives for experiments elucidating the influence of 3D-CO on the electronic properties of cuprates without the need to apply high magnetic fields.

Optically induced lattice deformations, electronic structure changes, and enhanced superconductivity in YBa2Cu3O6.48.

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa2Cu3O6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO2 planes. The empty chain Cu dy2-z2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these results, we calculate changes in the soft x-ray absorption spectra at the Cu L-edge. Femtosecond x-ray pulses from a free electron laser are used to probe changes in absorption at two photon energies along this spectrum and provide data consistent with these predictions.

Fermi liquid behavior of the in-plane resistivity in the pseudogap state of YBa2Cu4O8

Our knowledge of the ground state of underdoped hole-doped cuprates has evolved considerably over the last few years. There is now compelling evidence that, inside the pseudogap phase, charge order breaks translational symmetry leading to a reconstructed Fermi surface made of small pockets. Quantum oscillations [Doiron-Leyraud N, et al. (2007) Nature 447(7144):565-568], optical conductivity [Mirzaei SI, et al. (2013) Proc Natl Acad Sci USA 110(15):5774-5778], and the validity of Wiedemann-Franz law [Grissonnache G, et al. (2016) Phys Rev B 93:064513] point to a Fermi liquid regime at low temperature in the underdoped regime. However, the observation of a quadratic temperature dependence in the electrical resistivity at low temperatures, the hallmark of a Fermi liquid regime, is still missing. Here, we report magnetoresistance measurements in the magnetic-field-induced normal state of underdoped YBa2Cu4O8 that are consistent with a T2 resistivity extending down to 1.5 K. The magnitude of the T2 coefficient, however, is much smaller than expected for a single pocket of the mass and size observed in quantum oscillations, implying that the reconstructed Fermi surface must consist of at least one additional pocket.

Metal-insulator transitions and magnetic susceptibility in doped cuprate compounds

Results are presented from a theoretical study of the possibility of hole carrier localization and metal-insulator transitions which show up in the temperature dependences of the magnetic susceptibility χ(T) of doped copper-oxide (cuprate) compounds. The criteria for metal-insulator transitions owing to strong hole-lattice interactions and the formation of very narrow polaron bands in these materials with reduced doping level x are analyzed. It is shown that these kinds of metal-insulator transitions occur in underdoped La2-xSrxCuO4 and YBa2Cu3O6+x cuprates (i.e., for x ranging from 0.04 to 0.12). The characteristic temperature dependences χ(T) of the HTSC cuprates are found for different doping levels. These results are in good agreement with experimental data on metal-insulator transitions and the magnetic susceptibility of the HTSC cuprates.

Pseudogap of Ortho-III YBa2Cu3O7−x from Cu EPR investigation

The temperature dependences of g factors of underdoped YBa2Cu3O7−x (Tc ≈ 86.5 K) indicate that the pseudogap onset temperature T∗ (≈190 K) coincides with the phase boundary established by resistivity, Nernst effect, neutron diffraction and ultrasound measurements in YBCO phase diagram. The obtained empirical relationship between g factors and pseudogap is appropriate for the entire charactering temperature range of Ortho-III YBCO. The EPR signals are ascribed to the localized Cu2+(1) sites based on the quantitative calculations of the g factors by involving the local structures of the paramagnetic copper (1) sites. The present work provides another potential spectroscopic probe for the pseudogap in underdoped high Tc superconductors and the origin of EPR and related mechanisms in YBCO which are still controversial.

Magnetic field controlled charge density wave coupling in underdoped YBa2Cu3O6+x

The application of magnetic fields to layered cuprates suppresses their high-temperature superconducting behaviour and reveals competing ground states. In widely studied underdoped YBa2Cu3O6+x (YBCO), the microscopic nature of field-induced electronic and structural changes at low temperatures remains unclear. Here we report an X-ray study of the high-field charge density wave (CDW) in YBCO. For hole dopings ∼0.123, we find that a field (B∼10 T) induces additional CDW correlations along the CuO chain (b-direction) only, leading to a three-dimensional (3D) ordered state along this direction at B∼15 T. The CDW signal along the a-direction is also enhanced by field, but does not develop an additional pattern of correlations. Magnetic field modifies the coupling between the CuO2 bilayers in the YBCO structure, and causes the sudden appearance of the 3D CDW order. The mirror symmetry of individual bilayers is broken by the CDW at low and high fields, allowing Fermi surface reconstruction, as recently suggested.

Absence of Magnetic Field Dependence of the Anomalous Bond-Stretching Phonon in YBa2Cu3O6.6

Superlattice diffraction peaks have been recently observed in underdoped YBa2Cu3O6.6. They have been interpreted to originate from a charge density wave (CDW) formation. It is believed that strong phonon anomalies previously observed near the same wavevectors are related to the CDW. Competition with superconductivity is a salient feature of the CDW peaks. We investigated if the same is true of anomalous bond-stretching phonons around 60 meV by measuring the spectrum of this phonon at 10 K with and without an applied magnetic field of 10 T. Applying the field had no effect on the phonon within the experimental uncertainty.

The microscopic structure of charge density waves in underdoped YBa2Cu3O6.54 revealed by X-ray diffraction.

Charge density wave (CDW) order appears throughout the underdoped high-temperature cuprate superconductors, but the underlying symmetry breaking and the origin of the CDW remain unclear. We use X-ray diffraction to determine the microscopic structure of the CDWs in an archetypical cuprate YBa2Cu3O6.54 at its superconducting transition temperature ∼60 K. We find that the CDWs in this material break the mirror symmetry of the CuO2 bilayers. The ionic displacements in the CDWs have two components, which are perpendicular and parallel to the CuO2 planes, and are out of phase with each other. The planar oxygen atoms have the largest displacements, perpendicular to the CuO2 planes. Our results allow many electronic properties of the underdoped cuprates to be understood. For instance, the CDWs will lead to local variations in the electronic structure, giving an explicit explanation of density-wave states with broken symmetry observed in scanning tunnelling microscopy and soft X-ray measurements.

Influence of the Fermi Surface Morphology on the Magnetic Field-Driven Vortex Lattice Structure Transitions in YBa2Cu3O7−δ: δ = 0, 0.15

We report small-angle neutron scattering measurements of the vortex lattice (VL) structure in single crystals of the lightly underdoped cuprate superconductor YBa2Cu3O6.85. At 2 K, and for fields of up to 16 T applied parallel to the crystal c-axis, we observe a sequence of field-driven and first-order transitions between different VL structures. By rotating the field away from the c-axis, we observe each structure transition to shift to either higher or lower field dependent on whether the field is rotated towards the [100] or [010] direction. We use this latter observation to argue that the Fermi surface morphology must play a key role in the mechanisms that drive the VL structure transitions. Furthermore, we show this interpretation is compatible with analogous results obtained previously on lightly overdoped YBa2Cu3O7. In that material, it has long-been suggested that the high field VL structure transition is driven by the nodal gap anisotropy. In contrast, the results and discussion presented here bring into question the role, if any, of a nodal gap anisotropy on the VL structure transitions in both YBa2Cu3O6.85 and YBa2Cu3O7.

Femtosecond x rays link melting of charge-density wave correlations and light-enhanced coherent transport inYBa2Cu3O6.6

We use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge density wave correlations in underdoped YBa2Cu3O6.6. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

A revision of the fishtail effect in YBa2Cu3O7−δ crystals and its connection with vortex dynamics

The fishtail magnetization observed in many type II superconductors has been investigated since the earliest nineties and associated with different phase transitions and dynamic crossovers in complex vortex matter. In systems without a sharp order–disorder phase transition, the fishtail has been related with a crossover from elastic to plastic vortex creep regimes. In this paper we perform a critical revision of this accepted picture. We show that, in slightly underdoped YBa2Cu3O7−δ single crystals, there is a clear correlation between the fishtail magnetization and the Peak Effect observed in ac experiments with the associated history effects. We propose that both features are originated in the same dynamic crossover, between two plastic creep regimes. The proposed picture can also apply to other system, as those belonging to same families of iron-based pnictides.

Controlling the near-surface superfluid density in underdoped YBa2Cu3O(6+x) by photo-illumination.

The interaction with light weakens the superconducting ground state in classical superconductors. The situation in cuprate superconductors is more complicated: illumination increases the charge carrier density, a photo-induced effect that persists below room temperature. Furthermore, systematic investigations in underdoped YBa2Cu3O6+x (YBCO) have shown an enhanced critical temperature Tc. Until now, studies of photo-persistent conductivity (PPC) have been limited to investigations of structural and transport properties, as well as the onset of superconductivity. Here we show how changes in the magnetic screening profile of YBCO in the Meissner state due to PPC can be determined on a nanometer scale utilizing low-energy muons. The data obtained reveal a strongly increased superfluid density within the first few tens of nanometers from the sample surface. Our findings suggest a non-trivial modification of the near-surface band structure and give direct evidence that the superfluid density of YBCO can be controlled by light illumination.

Competing charge, spin, and superconducting orders in underdopedYBa2Cu3Oy

To explore the doping dependence of the recently discovered charge density wave (CDW) order in YBa2Cu3Oy, we present a bulk-sensitive high-energy x-ray study for several oxygen concentrations, including strongly underdoped YBa2Cu3O6.44. Combined with previous data around the so-called 1/8 doping, we show that bulk CDW order exists at least for hole concentrations (p) in the CuO2 planes of 0.078 <~ p <~ 0.132. This implies that CDW order exists in close vicinity to the quantum critical point for spin density wave (SDW) order. In contrast to the pseudogap temperature T*, the onset temperature of CDW order decreases with underdoping to T_CDW ~ 90K in YBa2Cu3O6.44. Together with a weakened order parameter this suggests a competition between CDW and SDW orders. In addition, the CDW order in YBa2Cu3O6.44 shows the same type of competition with superconductivity as a function of temperature and magnetic field as samples closer to p = 1/8. At low p the CDW incommensurability continues the previously reported linear increasing trend with underdoping. In the entire doping range the in-plane correlation length of the CDW order in b-axis direction depends only very weakly on the hole concentration, and appears independent of the type and correlation length of the oxygen-chain order. The onset temperature of the CDW order is remarkably close to a temperature T^\dagger that marks the maximum of 1/(T_1T) in planar 63^Cu NQR/NMR experiments, potentially indicating a response of the spin dynamics to the formation of the CDW. Our discussion of these findings includes a detailed comparison to the charge stripe order in La2-xBaxCuO4.

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 can be studied using applied magnetic fields that are sufficiently strong to suppress long-range superconductivity at low temperatures. Proposals in which the normal ground state is characterized 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 as 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 nodes, and also 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.