Oxygen dynamics in epitaxial YBa2Cu3O7-δ thin films

We have investigated epitaxial YBCO films by Perturbed γγ-Angular Correlation Spectroscopy (PAC) using ¹¹¹In probe atoms. The probes substitute on the yttrium lattice site and hyperfine parameters have been determined unambiguously. Excellent agreement is achieved with full potential electric field gradient (efg) calculations. Good reproducibility has been achieved by our preparation method allowing us to study the influence of oxygen motion on the structural orthorhombic to tetragonal phase transition. This revised version was published online in August 2006 with corrections to the Cover Date.     

Epitaxial growth of solution deposited YBa2Cu3O7-δ films

The solution deposition of YBa2Cu3O7- (Y123) high temperature superconducting thin films was studied. The films were prepared from a polymer-containing precursor onto SrTiO3 (001) and LaAlO3 (001) substrates and mineralized at high temperatures. The process depended on details of the film preparation in a delicate fashion, resulting either in superconducting or non-superconducting thin films. To elucidate this difference in conductivity, scanning electron microscopy and several X-ray diffraction techniques were used to characterize the resulting Y123 layers. Both the morphology of the film and the percentage of non-superconducting minority components are likely to be the origin of the difference in the conductance behavior at low temperatures.     

Screw dislocation mediated growth of sputtered and laser-ablated YBa2Cu3O7-δ films

By imaging the as-grown surfaces of sputtered and laserablated YBa₂Cu₃O_7– films with scanning tunneling microscopy (STM), we have directly observed spiral-shaped growth terraces which emanate from screw dislocations. The density of screw dislocations was observed to decrease with increasing growth temperature and substrate misorientation. The surface structures observed by STM together with cross-sectional transmission electron microscope (TEM) images provide insights into the mechanisms of crystal growth operative during the formation of YBa₂Cu₃O_7– films grown using these two widespread techniques.     

Pinning potential in thick PrBa2Cu3Ox/YBa2Cu3O7−δ quasi-multilayers

Using Pulsed Laser Deposition we have fabricated thick quasi-multilayers composed of incomplete layers of PrBa₂Cu₃O_x (PrBCO) nano-dots and layers of YBa₂Cu₃O_7?δ (YBCO). The number of such sequences was between 2 and 6, with the thickness of individual YBCO layers between 565 and 885 nm, and total thickness between 1.13 and 5.31 μm. For the thinner quasi-multilayer, DC magnetization studies showed an increase in the critical current density J_c at all fields in comparison with a pure YBCO reference sample, while the thicker samples showed an increased J_c only in high fields. We have also investigated the frequency dependence of J_c from AC susceptibility studies and found that the pinning potential is well described by a logarithmic dependence on current density. Pinning potentials in PrBCO/YBCO quasi-multilayers also proved to be higher than in the reference sample at high fields. From angle-dependent transport measurements we have found indications of strong pinning centres induced by the (PrBCO) nano-dots, both isotropic and c-axis correlated.     

An investigation of the PrBa2Cu3O7-δ system

Members of the PrBa₂Cu₃O_7– system possessing the orthorhombic structure over a wide range of oxygen stoichiometry (=–0.5 to +0.5) have been prepared and characterized. Similar compositions with a tetragonal structure have also been prepared. None of the oxides is superconducting, independent of the structure or stoichiometry. Praseodymium seems to be present to a small extent in the 4+ state in oxygen-excess (negative ) samples. Orthorhombic PrBa₂Cu₃O_7– samples show the presence of twins suggesting that twins arise from orthorhombicity and have no relation to the superconductivity. A neutron diffraction study of a near-stoichiometric sample has shown a disordered orthorhombic structure with 72% occupancy of the 01 (chain) sites and with no interchange between Pr and Ba sites.Contribution No. 503 from the Solid State and Structural Chemistry Unit     

Structural transition of secondary phase oxide nanorods in epitaxial YBa2Cu3O7−δ films on vicinal substrates

A theoretical study of a structural transition of secondary phase oxide nanorods in epitaxial YBa₂Cu₃O_7?δ films on vicinal SrTiO₃ substrates is presented. Two possible types of film/substrate interface are considered, with one assuming complete coherence, while the other is defective as manifested by the presence of antiphase grain boundaries. Only in the former case does the increase of the vicinal angle of the substrate lead to a substantial change of the strain field in the film, resulting in a transition of the nanorod orientation from the normal to the in-plane direction of the film. The calculated threshold vicinal angle for the onset of the transition and lattice deformation of the YBa₂Cu₃O_7?δ film due to the inclusion of the nanorods is in very good agreement with experimental observations. This result sheds lights on the understanding of the role of the film/substrate lattice mismatch in controlling self-assembly of dopant nanostructures in matrix films.     

Correlation betweenJ c and screw dislocation density in sputtered YBa2Cu3O7-δ films

Electric transport properties of sputtered YBa₂Cu₃O_7– films were studied as a function of screw dislocation density, ranging from 5·10⁷ cm^–2 to 1.3·10⁹ cm^–2 as determined at the film surface. A correlation was found between the number of screw dislocations and the critical current density (J _c ). Films with higher screw dislocation densities have higher critical current densities and a slower drop ofJ _c as a function of applied magnetic fieldH.     

Observation of the early stages of growth and the formation of growth spirals in epitaxial YBa2Cu3O7-δ thin films by AFM

Ultrathin epitaxial films of YBa₂Cu₃O_7– on SrTiO₃ prepared by Direct Current (DC) sputtering and pulsed laser deposition were imaged by Atomic Force Microscopy (AFM) to follow the different stages of growth of the thin films. Series of films with thicknesses between 1.2 nm and 12 nm (1–10 monolayers of YBa₂Cu₃O_7–) were prepared under identical conditions, optimized with respect to electrical and structural properties, to obtain information on the mechanisms responsible for the formation of growth spirals which are commonly observed in films having a thickness of several 10 nm or more. It could be shown that few layers are formed by a layered growth mode where material is attached laterally to 2D islands which are only one c-axis unit cell in height. In a later stage of growth when about 8–10 layers have been formed, the growth process changes to a mode which is mediated by growth spirals. This could be directly monitored in the AFM images where different defect structures like vertically sheared growth fronts and dendrite-like terraces of stacked islands as well as the resulting growth spirals could be identified.     

Features of the twin structure of YBa2Cu3O7−x epitaxial films

X-ray diffraction is used to investigate YBa₂Cu₃O_7?x (YBCO) films on NdGaO₃(110) and a ${{(100)CeO_2 } \mathord{\left/ {\vphantom {{(100)CeO_2 } {(1\bar 102)}}} \right. \kern-0em} {(1\bar 102)}}Al_2 O_3 $ heterostructure. Symmetric, asymmetric, and axial geometries for θ and θ/2θ scans are used to obtain diffraction spectra from different crystallographic planes. The orientational and quantitative twinning characteristics of the films are determined. While the crystallographic parameters of these two types of film (the films are c-axis oriented with c=11.67 Å) are similar, there are differences in the twin structure. In particular, the features of the NdGaO₃ structure lead to the appearance of an angle differing from 90° (90.20°) between the possible (110) and θ/2θ twin planes in a YBCO film and a different number of twin components in each system of twins. It is concluded from an analysis of the broadening of reflections, which are sensitive to twinning, that there is not twinning in a 60% film of YBCO on Al₂O₃ with a CeO₂ buffer layer.     

Femtosecond dynamics and transport of optically excited electrons in epitaxial Cu films on Si(111)-7×7

Time-resolved two-photon photoemission spectroscopy is used to study ultrafast electron dynamics of epitaxial Cu films grown in situ on a Si(111)-7×7 substrate with 6 to 44 nm thickness. For excitation with femtosecond laser pulses at h=2.35 eV a pronounced increase of the electron relaxation rates is observed with increasing film thickness and even further in comparison to bulk data. This is attributed to an enhanced energy dissipation in thicker films due to transport of excited carriers into the bulk. PACS 73.50.Gr; 73.90.+f; 78.47.+p; 79.60.-i     

Micromechanical model for self-organized secondary phase oxide nanorod arrays in epitaxial YBa2Cu3O7−δ films

A micromechanical model based on the theory of elasticity has been developed to study the configuration of self-assembled secondary phase oxide nanostructures in high-temperature superconducting YBa₂Cu₃O_7?δ films. With the calculated equilibrium strain and elastic energy of the impurity doped film, a phase diagram of lattice mismatches vs. elastic constants of the dopant was obtained that predicts the energetically preferred orientation of secondary phase nanorods. The calculation of the nanorod orientation and the film lattice deformation has yielded excellent agreement with experimental measurements.     

Transient photoimpedance response of YBa2Cu3O7−0δ epitaxial films in the mixed state

This paper reports on an investigation of transient photoimpedance response to radiation, in other words, real-time variations of the impedance induced by femtosecond optical pulses in superconducting films transferred to the mixed state by an external magnetic field applied parallel to the c-axis. When the films were in a state characterized by the absence of dc resistivity, the response amplitude increased with the magnetic field faster than expected owing to the contribution of magnetic vortices to the impedance of a superconductor with s-wave pairing of electrons. It turned out that the effect is due to a growth in the effective density of quasiparticle states in the mixed state of a d-wave superconductor. In the absence of magnetic field, however, the response amplitude was higher at lower temperatures, which contradicts the predictions of both models. Possible reasons for this feature in the response as a function of temperature are discussed. Zh. éksp. Teor. Fiz. 116, 1035–1047 (September 1999)     

Local electronic structure of Cu2O,CuO and YBa2Cu3O7−δ

Cu 3d and O 2p electronic states of Cu₂O, CuO, and the highT _c compound YBa₂Cu₃O_7– have been probed by means of high resolution x-ray emission spectroscopy (XES). The CuL and OK XES bands are compared in detail with recently reported x-ray photoelectron and ultraviolet photoelectron spectroscopy (XPS and UPS) measurements and densities of states obtained by local density functional (LDF) theory. The XES data show that the hybridization between Cu 3d and O 2p states is completely modified in CuO and YBa₂Cu₃O_7–, whered-d correlation energy is large, as compared to LDF predictions. Such is not the case for Cu₂O where agreement between theory and experiment is good.The Cu 3d states are found to be highly localized in YBa₂Cu₃O_7– (though less so than in CuO). The O 2p states lie at lower binding energies than in the simpler oxides and are mainly situated above the Cu 3d states. The respective positions of the centre of gravity of the OK emission bands on an x-ray energy scale indicate that the oxygen sites are less well screened by the O 2p states in the highT _c compound. This provides indirect evidence for the presence ofd-like states at the oxygen sites.     

Electronic structure and optical spectra of YBa2Cu3O7−δ thin films in the infrared and UV region

Optical reflectance of YBa₂Cu₃O_7- thin films grown by laser ablation is measured within photon energies of 0.1 eV to 3.5 eV at room temperature. The spectra can be fit congruently with the anisotropic dielectric constants which take account of the intraband free carrier transition and interband transition. The anisotropic plasma frequencies are simulated to be _pl=2.18 eV and _ch=2.80 eV contributed from free carriers on the plane and in the chain, respectively. The interband transition occurs near 2.5 eV and is pertinent to a rather broad line width.     

Misfit stresses in YBa2Cu3O7−x films

Misfit and thermoelastic stresses in HTSC layers 1-2-3 grown on various substrates are, analyzed with the use of ultrasonic measurements of Young's moduli inYBa ₂ Cu ₃ O _7−x . It is shown that the misfit stress gives the main contribution to the formation of the HTSC layer strain. Military Academy of Strategic Rocket Forces. Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 4, pp. 87–90, April, 2000.     

Raman study of the 90° grain boundaries in YBa2Cu3O7−δ thin films

YBa₂Cu₃O_7−δ (YBCO) films containing two different types of 90° grain boundaries were fabricated on the same substrates. Raman spectra from several parts of the basal-plane-faced tilt (TL) grain boundaries were measured and compared with those from the twist (TW) grain boundaries. The Raman results show that I(500)/I(340), the relative intensity of the A_1g mode near 500 cm⁻¹ with respect to that of the B_1g mode near 340 cm⁻¹, is suppressed in the TL boundaries, relative to the TW boundaries. The results can be interpreted to mean that the stress is stronger in the TL boundaries than in the TW boundaries. This may offer an alternative explanation for the weak-link behavior of the step-edge Josephson junctions.     

Production of thick YBa2Cu3O7-δ films on sapphire with a cerium oxide sublayer

The feasibility of producing high-quality films of the high-temperature superconducting material YBa₂Cu₃O_7-δ with thicknesses up to 2.6 μm by dc magnetron sputtering is demonstrated. It is found that inclusions consisting of CuO and YBa₂Cu₃O₈ coexist with the growing film and are “sinks” for defects, nonstoichiometric atoms, and mechanical stresses. X-ray diffraction and Rutherford backscattering studies show that the structural perfection of the films increases as the thickness is increased in the proposed production regime. Zh. Tekh. Fiz. 69, 132–136 (September 1999)     

Fluctuation-induced conductivity in melt-textured Pr-doped YBa2Cu3O7-δ composite superconductor

In this study, the effects of thermal fluctuations on the electrical conductivity in melt-textured YBa₂Cu₃O_7-δ, Y_0.95Pr_0.05Ba₂Cu₃O_7-δ and (YBa₂Cu₃O_7-δ)_0.95–(PrBa₂Cu₃O_7-δ)_0.05 composite superconductor were considered. The composite superconductor samples were prepared through the top seeding method using melt-textured NdBa₂Cu₃O_7-d seeds. The resistivity measurements were performed with a low-frequency, low-current AC technique in order to extract the temperature derivative and analyze the influence of the praseodymium ion on the normal superconductor transition and consequently on the fluctuation regimes. The results show that the resistive transition is a two-step process. In the normal phase, above the critical temperature, Gaussian and critical fluctuation regimes were identified, while below the critical temperature, in the regime near the approach to the zero-resistance state, the fluctuation conductivity diverges as expected in a paracoherent-coherent transition.     

Fluctuation-enhanced conductivity and magnetoconductivity of high-quality YBa2Cu3O7−δ crystals

We present measurements of the in-plane resistivity _ab of YBa₂Cu₃O_7– single crystals withT _c 92 K and _ab (100 K)50 cm. The temperature dependence of the fluctuation conductivity and of the magnetoconductivity aboveT _c is analyzed in terms of direct and indirect fluctuation contributions for layered superconductors. The combination of fluctuation conductivity and magnetoconductivity allows to determine both coherence lengths _ab (0) and _c (0) as well as the phase-relaxation time of the pairs in an unequivocal manner. Evidence for clean limit type-II superconductivity in our crystals is given by large values of the mean free pathl _{ab ab} (0).Dedicated to Prof. Dr. F. Hund on the occasion of his 95th birthday     

Thermal and magnetic properties of some YBa2Cu3O7−δ samples

Thermal and magnetic measurements have been performed on several YBa₂Cu₃O_7−δ compounds, some ones showing a large content of high T_c (93 K) superconducting phase. A jump in the specific heat ΔCp, is well evidenced at the transition allowing a determination of the ratio ΔCp/T_c ≅ 23 ± 5. mJ/ (mole Cu)K². In addition, an estimation of the γ value (≅ 11 mJ/(mole Cu). K²) has been drawn from the determination of the electronic entropy at T_c. The samples have been characterized by susceptibility, magnetization and resistivity experiments. The critical field slopes at T_c were found to be dHc₁/dT ≅ 17 Oe/K and dHc₂/dT ≅ 20 kOe/K. The results are discussed in the framework of the Ginzburg-Landau theory.