Enhancement of critical current density of YBa2Cu3O7 − δ thin films by self-assembly of Y2O3 nanoparticulates

YBa₂Cu₃O_7 − δ (YBCO) thin films, possessing high critical current density (J_c), have been synthesized by embedding a homogeneous array of Y₂O₃ non-superconducting nanoclusters/nanoparticles using a pulsed laser deposition technique. The size, interparticle spacing, and density of Y₂O₃ nanoparticles in YBCO thin films were tailored by varying the number of laser pulses in order to determine the optimum size for effective immobilization of vortices. Scanning transmission electron microscopy with atomic number contrast and X-ray diffraction techniques were used to determine the size and structure of the nanoparticles. Both techniques indicate that the Y₂O₃ particles are epitaxial with respect to the surrounding YBCO matrix. The information about pinning of vortices by the nanoparticles was obtained by investigating the behavior of critical current density as a function of temperature and applied field, which in turn determines the vortex density in the sample. The superconducting transition temperature (T_c) of YBCO films with the inclusion of nanoparticles was observed to remain almost the same or decrease marginally (1-2 K) with respect to T_c of pure YBCO films deposited under identical conditions. However, J_cs of YBCO films embedded with self-assembled nanoparticles were found to be significantly higher than that of pure YBCO films. The J_c enhancement was up to five times in high magnetic field, which is a key requirement for practical application of high-T_c materials.     

Study of SrTiO3 thin films grown by sputtering technique for tunnel barriers in quasiparticle injection contacts

High-quality, c-axis oriented YBa₂Cu₃O_7 − x/SrTiO₃/Au (YBCO/STO/Au) planar structures were fabricated in situ by direct current/radiofrequency inverted-cylinder magnetron sputtering on (001) STO oriented substrates. The sandwich-type structures were patterned to transistor dimensions by standard ultraviolet-photolithography and Ar etching. The current transport mechanism in the very thin STO barriers (2-30 nm) was examined by measuring the tunneling G as function of temperature (T), and bias voltage (V). It was found that resonant tunneling and hopping via a small number of localized states (LS) are responsible for electronic conduction in the insulating material. Elastic tunneling was observed for the case of a nominal 2 nm thick STO-barrier with an energy gap Δ ≈ 20 meV in the (001) direction of YBCO. On the other hand, inelastic hopping transport via n-LS dominated for STO barrier thickness d > 2 nm. G of the lowest-order hopping channel (hopping via two LS) exhibits the characteristic T and V dependences: G₂^hop(T) ∝ T^4/3, G₂^hop(V) ∝ V^4/3, respectively. Increasing the thickness of the STO barriers, hopping channels of higher order contribute more and more to the current transport as proven by measuring the T and V dependences. A crossover to variable range hopping behavior has been observed for junctions with thicker barriers (d ≥ 20 nm) in the high-V or high-T regime. By fitting the experimental data to theoretical models, physical parameters of the LS could be determined. For instance, the value of the localization length or radius of the localized state was determined to be ~ 4.6 × 10^− 8 cm which corresponds to the lattice constant of the STO unit cell. A value of ~ 6 × 10¹⁹ (eV)^− 1 cm^− 3 was calculated for the density of LS and the average barrier height was estimated as ~ 0.4 eV.     

Microwave characterization of laser ablated Y1Ba2Cu3O7−x thin films

In the present study we report the measurements of microwave surface resistance (R_s) of YBCO thin films on LaAlO₃ substrate as a function of temperature, thickness and magnetic field by microstrip resonator technique. The T_c(R = 0) of the films is 90 K and J_c > 10⁶ A/cm² at 77 K. The microwave surface resistance has been measured for films of various thicknesses. The value of R_s has been found to be initially decreased with increasing film thickness due to increase in number of defects. A minimum microwave surface resistance has been obtained for film thickness of about 300 nm. The increase of R_s with film thickness above 300 nm is possibly due to degradation of the film microstructure as observed with Atomic Force Microscopy. Temperature dependence of surface resistance has been studied for best quality films. The field induced variations of surface resistance are also investigated by applying dc magnetic field perpendicular to stripline structure and surface of the film. A general linear and square field dependence of R_s at low and high value of fields has been observed with critical field value of 0.4 T which confirms the microwave dissipation induced by flux flow in these resonators at 10 GHz frequency. The hysteresis of R_s in dc field observed for field value above critical field shows the higher value of surface resistance in decreasing field than in increasing field which is in agreement with one state critical model and is a characteristic of homogeneous superconductors.     

Low cost synthesis of high-Tc superconducting films on metallic substrates via ultrasonic spray pyrolysis

Ultrasonic spray pyrolysis technique has been used to deposit both in situ and ex situ high temperature superconducting films (HTSC) of Y₁Ba₂Cu₃O_x(YBCO) and Bi₂Sr₂CaCu₂O_x (BSCCO) compounds over various substrates. Nitrate precursor solutions are used to deposit films of ∼10 μm thickness. Both low temperature spray with substrate temperature T_s < 500 °C and high temperature deposition with T_s = 550-900 °C are carried out. Superconducting properties of these films are observed to vary with various parameters such as concentration of spray solution, deposition temperature and nature of substrate and annealing process. Best quality films show T_c (R = 0) of 89 K and J_c of ∼4 × 10⁴ A/cm² at 77 K and ∼ 10⁵ A/cm² at 20 K. X-ray diffraction pattern reveals that the films are textured along c-axis. Successful attempt has been made to deposit in situ superconducting films over polycrystalline Ag for coated conductor applications. Various deposition and annealing conditions are optimized to control the diffusion of Ag from substrate to film, which otherwise can segregate into the grain boundaries and make the films non-superconducting.     

Tl2Ba2CaCu2O8 thin films on 2 in. LaAlO3(0 0 1) substrates

High quality Tl₂Ba₂CaCu₂O₈ (Tl-2212) superconducting thin films are prepared on both sides of 2 in. LaAlO₃(0 0 1) substrates by off-axis magnetron sputtering and post-annealing process. XRD measurements show that these films possess pure Tl-2212 phase with C-axis perpendicular to the substrate surface. The thickness unhomogeneity of the whole film on the 2 in. wafer is less than 5%. The superconducting transition temperatures T_cs of the films are around 105 K. At zero applied magnetic field, the critical current densities J_cs of the films on both sides of the wafer were measured to be above 2 × 10⁶ A/cm² at 77 K. The microwave surface resistance R_s of film was as low as 350 μΩ at 10 GHz and 77 K. In order to test the suitability of Tl-2212 thin films for passive microwave devices, 3-pole bandpass filters have been fabricated from double-sided Tl-2212 films on LaAlO₃ substrates.     

Epitaxial growth and rectification characteristics of double perovskite oxide La2NiMnO6 films on Nb-SrTiO3 single crystal substrates

High-quality thin films of double perovskite La₂NiMnO₆ (LNMO) were epitaxially grown on Nb-doped SrTiO₃ (NSTO) substrates by pulsed laser deposition. The films were found to undergo a ferromagnetic-to-paramagnetic transition at ~ 280 K, which is consistent with the literature report. In the electrical measurements, typical rectifying behavior was observed in the LNMO/NSTO heterojunction. The diffusion voltage (V_D) increases linearly with temperature (T) during cooling until T = 170 K. At T < 170 K, V_D increases at a higher rate and the V_D-T relationship becomes non-linear. A disordered phase related spin polarization was used to understand such behaviors in the heterojunctions.     

Testing field and annealing temperature dependence of leakage properties in Bi3.25La0.75Ti3O12 thin films

Ferroelectric Bi_3.25La_0.75Ti₃O₁₂ thin films annealed at different temperatures were prepared on Pt/Ti/SiO₂/Si substrates by metalorganic decomposition method. The leakage current behavior and the current conduction mechanism were investigated. For all films, the leakage current density − electric field (J−E) characteristic is confined within a “triangle” in the log (J)− log (E) plane bounded by three limiting curves: Ohm's law (J ∝ E), trap-filled-limit (J ∝ E^a, a > 1), and Child's law (J ∝ E²). At high field region, Bi_3.25La_0.75Ti₃O₁₂ thin films with grains of rod-like show higher leakage current, while films with grains of spherical- or planar-like exhibit lower leakage current.     

High-Quality YBa2Cu3O7−x Films with CeO2/YSZ Buffer Layers on 2-Inch Si Wafers Deposited by Pulsed Laser

The pulsed laser deposition (PLD) process is shown for in situ reproducibly fabricating YBa₂Cu₃O_7?x (YBCO) superconducting films with yttrium-stabilized zirconia (YSZ) and CeO₂ buffer layers, nonsuperconducting crystalline YBa₂Cu₃O_7?x (YBCO*) passivation layer, and silver contact film on 2-inch silicon wafers. Variations of less than ±7% in film thickness have been obtained for this multilayer growth over the whole wafer. The YBCO films on 2-inch silicon wafers have homogeneous superconducting properties with zero resistance temperature T _c0 from 88.4 K to 88.9 K. and critical current density J _c at 77 K and zero field from 2.5 × 10⁶ to 7× 10⁶ A/cm². The YSZ, CeO₂ and YBCO layers grow epitaxially on silicon wafers. Full widths at half maximum (FWHMs) of (113) reflections of 40 nm thick YBCO layer from φ-scan patterns are only 1.71° and 1.85° corresponding to the center and edge of the wafer, respectively. These results are very promising for developing high-quality high-T _c superconducting devices on large-area silicon wafers.     

Electrical conduction mechanisms of metal nanoclusters embedded in an amorphous Al2O3 matrix

We present the synthesis and electrical characterization of amorphous nanocomposite layers made of metallic nanoclusters embedded in an alumina matrix (nc-Co:Al₂O₃). The nanostructured materials were fabricated using a pulsed laser deposition (PLD)-derived method based on a nano-cluster generator coupled with a conventional PLD system for host medium co-deposition. The films were subjected to a detailed structural study carried out using high-resolution transmission electron microscopy and atomic force microscopy. The clusters inserted in the alumina matrix are metallic, well crystallized and possess an fcc structure with an average diameter centered at ∼ 2 nm. Dielectric constant and electrical conduction mechanisms of nc-Co:Al₂O₃ layers integrated in metal-insulator-metal capacitive structures were studied for different doping levels and for a broad temperature range (303-473 K). It was concluded that the dielectric constant in the films depends on the doping levels while the major electrical conduction mechanisms are best described by the space charge limited currents formalism, in which the current density J on an applied voltage V follow a power-law dependence (J ∼ Vⁿ) at applied voltages higher than ∼ 2 V. Such composite may find immediate applications as dielectric layers with controlled discharging conduction paths in Radio Frequency-Micro-Electro-Mechanical Systems capacitive structures.     

Structural and electrical properties of BiFeO3 thin films by solution deposition and microwave annealing

Lead-free polycrystalline BiFeO₃ (BFO) thin films were developed using a chemical solution deposition method to deposit the films and the multi-mode 2.45 GHz microwave furnace to optimize the annealing condition of the films. Phase-pure BFO films were obtained at 500 °C-600 °C for 1-5 min with a heating rate of 10 °C/min. The film by microwave annealing (MW) at 550 °C for 5 min exhibited a (012)-preferred orientation with a dense morphology of grain size ~ 294 nm. Its dielectric constant of 96.2, low leakage current density of 2.466 × 10^− 6 A/cm², polarization (2P_r) and coercive field (2E_c) of 0.931 μC/cm² and 57.37 kV/cm, respectively, were improved compared to those by conventional annealing (CA) at the same annealing conditions.     

Reproducibility of transition temperature and critical current density of thin films of YBa2Cu3O7 on (100) LaAlO3

Submicrometer epitaxial films of YBa₂Cu₃O₇(YBCO) on (100) LaAlO₃ were made by coevaporation and furnace annealing. Samples from more than a dozen runs are used in this study. The zero resistance transition temperature (T _c) is high (89 or 90 K) if the film composition is phase pure (Ba/Y=2, Cu/Y=3) or if it is enriched in Ba and Cu. For these compositions the critical current density (J _c) at 77 K has an average value of 2×10⁵ A cm^–2, with a tendency for decreasingJ _c with increasing film thickness (0.2 to 0.8m). Variations inJ _c are not correlated with deviations from ideal stoichiometry. Steeper slopes of the resistance-temperature curves above 100 K and lower values of the room-temperature resistivity are associated with high values ofJ _c. If the film composition is enriched in Y relative to Ba and Cu,T _c decreases by several degrees.     

Superconducting properties of internal-tin route Nb3Sn wires with radially arranged filaments : Development that realizes high Jc and low hysteresis loss

An internal-tin route Nb₃Sn superconducting wire that has both remarkably low hysteresis loss (Q_h) and high critical current density (J_c) was developed according to a new design idea. The wire was constructed by arranging the filaments in a radial layout, enlarging the outer filaments along the radial direction, narrowing the filament spacing in the radial direction intentionally and enlarging the filament spacing in tangential direction. Thus, the electromagnetic coupling among the filaments in tangential direction due to the bridging and/or proximity effect was suppressed without decreasing the volume fraction of Nb. As a result, excellent properties such as J_c(12 T) = 1.15 × 10³ A/mm² and Q_h = 301 mJ/cm³ (for 1 cycle of B = ±3 T) were obtained. We also evaluated the transition temperature (T_c) and upper critical field (B_c2) of the wire. The values for T_c and B_c2 were 17.3 K and 24.1 T, respectively, which were much better than those of usual internal-tin route wires. Moreover, electron probe micro-analyses confirmed that the good T_c and B_c2 were the result of the qualitative improvement of the Nb₃Sn compound based on the effects of arranging the Nb filaments radially, increasing the ratio of Sn-to-Nb and shortening the diffusion length for Sn. This wire is promising for use with conduction-cooled high-field magnets, in which there is a need to decrease the load of the cryocooler, and also for the strands of fusion coils.     

Epitaxial growth and exchange coupling of spinel ferrimagnet Ni0.3Zn0.7Fe2O4 on multiferroic BiFeO3

Thin films of the zinc nickel ferrite, Zn_0.7Ni_0.3Fe₂O₄ (ZNFO), were deposited by the RF magnetron sputtering on a number of substrates, including (001) oriented single crystals of LaAlO₃ (LAO) and SrTiO₃ (STO), polycrystalline Pt/Si, and epitaxial films of BiFeO₃ (BFO) and LaNiO₃ (LNO). Except for the films on Pt/Si, the ZNFO films grown on other substrates were epitaxial and their magnetic properties were affected by the heteroepitaxy induced strains. Typically, the coercivity (H_c) was increased with the strain, i.e. H_c varied from 31 Oe for the 150 nm thick polycrystalline films grown on Pt/Si, to 55 Oe and 155 Oe for the 20 nm thick epitaxial films grown on BFO and LAO, respectively. The saturation magnetization of the epitaxial films was reduced accordingly to about 470 emu/cm³ from 986 emu/cm³ in the polycrystalline films. The all-oxide architecture allowed field-annealing to perform at the temperature above the Neel temperature of BFO (~ 370 °C), after which clear exchange bias was observed.     

High-temperature anomalies of dielectric constant in TiO2 thin films

Anatase and rutile TiO₂ thin films were prepared by chemical vapor deposition with precursors Ti(OPrⁱ)₄ and Ti(dpm)₂(OPrⁱ)₂ (dpm = 2,2,6,6-tetramethylheptane-3,5-dione and Prⁱ = isopropyl), respectively. The dielectric properties of TiO₂ thin films have been studied in 20-1100 K temperature range in air, in controlled Ar/O₂ atmospheres, and in vacuum with silicon-based metal-insulator-semiconductor Au/TiO₂/Si capacitors. High-temperature (T_c ∼ 980 K) anomalous behavior of dielectric constant was observed in both anatase and rutile TiO₂ thin films.     

Properties of La-substituted Na0.5Bi4.5Ti4O15 ferroelectric thin films

Ferroelectric Na_0.5La_0.5Bi₄Ti₄O₁₅ (NaLaBTi) thin films were prepared by a chemical solution deposition method. The NaLaBTi thin films annealed at 750 °C under oxygen atmosphere were randomly oriented polycrystalline. Electrical properties of the NaLaBTi thin films were compared to Na_0.5Bi_4.5Ti₄O₁₅ thin films and better properties were observed in the NaLaBTi thin films. Remnant polarization (2P_r) and coercive electric field (2E_c) were 43 µC/cm² and 204 kV/cm at an applied electric field of 478 kV/cm, respectively. Leakage current density was 1.95 × 10^− 6 A/cm² at 100 kV/cm. Dielectric constant and dielectric loss were 805 and 0.05 at 1 kHz, respectively. Switchable polarization was suppressed by 15% after 1.44 × 10¹⁰ switching cycles.     

Combination of Ag Substrate Decoration with Introduction of?BaZrO3 Nano-Inclusions for?Enhancing Critical Current Density of?YBa2Cu3O7 Films

The combination of two methods: Ag substrate decoration and introduction of BZO nano-inclusions has been used in a pulsed laser deposition (PLD) method to increase the critical density (J _c ) of YBCO films. The films were deposited on single crystal SrTiO₃ (STO) substrates decorated with various architecture of Ag nano-dots. We have studied the diameter and density of Ag nano-dots and their influence on J _c of BZO-added YBCO films. We found that 15 laser pulses on the Ag target gives an optimum result in increasing J _c in comparison with BZO-doped YBCO films of the same thickness in self-field and low applied magnetic fields. A higher number of laser pulses on the Ag target led to increasing critical current density in high applied magnetic fields only (above 2 T). We have studied films of the thickness from 0.4 ??m to 3.8 ??m and found that the highest J _c at all applied fields investigated is achieved for a 1.2 ??m thick film. The transmission electron microscopy clearly shows BZO nano-rods that provide strong c-axis pinning centres in the films.     

Ag and O ion irradiation induced improvement in dielectric properties of the Ba(Co1/3Nb2/3)O3 thin films

We present the preliminary results of temperature and frequency dependent dielectric measurements on Ba(Co_1/3Nb_2/3)O₃ (BCN) thin films. These films were prepared on indium tin oxide (ITO) coated glass substrates by the pulse laser deposition (PLD) technique. It exhibits single-phase hexagonal symmetry. These films were irradiated with Ag¹⁵⁺ (200 MeV) and O⁷⁺ (100 MeV) beams at the fluence 1 × 10¹¹, 1 × 10¹², and 1 × 10¹³ ions/cm². On irradiating these films, its dielectric constant (?′) and dielectric loss (tan δ) parameters improve compared to un-irradiated film. Compared to O⁷⁺ irradiation induced point/cluster defects Ag¹⁵⁺ induced columnar defects are more effective in reducing/pinning trapped charges within grains. The present paper highlights the role of swift heavy ion irradiation in engineering the dielectric properties of conductive samples to enable them to be useful for microwave device applications.     

Structural and superconducting properties of Bi1.7Pb0.4Sr2 − xYbxCa1.1Cu2.1Oy system

The structural, electrical and superconducting properties of Bi_1.7Pb_0.4Sr_2 − xYb_xCa_1.1Cu_2.1O_y system has been studied for different Yb concentrations. The samples are prepared by solid state synthesis in the polycrystalline bulk form. Structural analysis by X-ray diffraction, microstructural examination by SEM and measurements of electrical and superconducting properties have been conducted to study the effects of Yb substitution at Sr site. The critical temperature (T_C) and critical current density (J_C) are found to increase drastically with Yb substitution. Maximum values of T_C and J_C are observed for x = 0.3 and x = 0.2 respectively. The increase in T_C and J_C is explained due to the substitution effect of Yb³⁺ in place of Sr²⁺ and consequent change in the hole concentration in the CuO₂ planes. Above the optimum levels T_C and J_C begin to reduce due to secondary phase formation. A metal-insulator transition originating from the change of carrier concentration is found to occur at higher doping level (x > 0.5).     

Pechini sol-gel deposition and luminescent properties of SrLa1−xRExGa3O7 (RE = Eu, Tb) phosphor films

SrLa_1−xRE_xGa₃O₇ (RE = Eu³⁺, Tb³⁺) phosphor films were deposited on quartz glass substrates by a simple Pechini sol-gel method. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), atomic force microscopy, field-emission scanning electron microscopy, photoluminescence spectra, and lifetimes were used to characterize the resulting films. The results of XRD indicated that the films began to crystallize at 700 °C and crystallized fully at 900 °C. The results of FT-IR spectra were in agreement with those of XRD. Uniform and crack-free films annealed at 900 °C were obtained with average grain size of 80 nm, root mean square roughness of 46 nm and thickness of 130 nm. The RE ions showed their characteristic emission in crystalline SrLa_1−xRE_xGa₃O₇ films, i.e., Eu³⁺⁵D₀-⁷F_J (J = 0, 1, 2, 3, 4), Tb³⁺⁵D₄-⁷F_J (J = 6, 5, 4, 3) emissions, respectively. The optimum concentrations (x) of Eu³⁺ and Tb³⁺ were determined to be 50, and 80 mol% in SrLa_1−xRE_xGa₃O₇ films, respectively.     

Optically induced changes and long-term relaxations of resistivity and critical temperature in He irradiated YBa2Cu3Ox

Thin films of YBa₂Cu₃O_x with superconducting critical temperatures (T_c) ranging from 58 K to 72 K were prepared by pulsed-laser deposition and subsequent irradiation with 75 keV He⁺ ions. Optical excitation of the films with a He-Ne laser resulted in a small resistivity reduction, when the experiment was carried out a short period of time after the ion irradiation. The value of T_c was essentially unchanged by the optical treatment. Further light excitation experiments did not show a significant effect on the resistivity of the samples. We conclude that ion-irradiated metallic YBa₂Cu₃O_x does not exhibit the persistent photoconductivity observed in oxygen-depleted samples with comparable critical temperatures. On the other hand we have observed a long-term relaxation of T_c towards larger values that takes place even when the samples are kept in the dark. Our results indicate that T_c may increase after ion irradiation to an asmptotic value about 20% over the initial value on a typical time scale of years. This observation may be important for possible applications of light-ion irradiated YBa₂Cu₃O_x.