A method for the direct observation of the early stages of growth of superconducting films by transmission electron microscopy (TEM) is reported. The technique uses well‐characterized, single‐crystal TEM foils as substrates for the deposition process. Ultrathin films of YBa2Cu3O6+x (YBCO) were prepared by pulsed laser deposition from stoichiometric bulk samples directly onto (001) oriented MgO thin‐foil substrates. Observation of the film by TEM is possible without any post‐deposition specimen preparation. The epitactic nature of the film growth is shown by analysis of the moire fringe pattern and by selected area diffraction. In addition to an interconnected film, copper oxide particles and stoichiometric ablated clusters were observed.

Observation of the early stages of growth of superconducting thin films by transmission electron microscopy

Complex metal oxides, including ferroelectric, ferrimagnetic and superconducting ceramics, have a variety of technologically useful properties that can be exploited for a number of applications. Fabrication of complex metal oxide ceramics with specific properties requires high-purity powders with controlled chemical compositions, size distributions, and morphologies. Powders with these characteristics can be produced by aerosol processes in which fine particles are generated in gaseous flow systems. The particles can also be deposited from the gas phase onto surfaces to form films. This paper will discuss the use of aerosol processes for the generation of complex metal oxide powders. A review of aerosol processes will be presented first, followed by a discussion of the methods used for the generation of superconducting ceramic powders. Examples include the production of YBa2Cu3O7, La1.85Sr0.15CuO4, and Tl-Ca-Ba-Cu-O powders and films. Emphasis will be placed on defining the conditions required for the generation of chemically homogeneous particles with controlled morphologies.

Generation of complex Metal Oxides by Aerosol Processes: Superconducting ceramic particles and films

The composition of pulsed-ultraviolet-laser-deposited Y-Ba-Cu-O films was examined as a function of position across the substrate, laser fluence, laser spot size, substrate temperature, target conditioning, oxygen pressure and target-substrate distance. Laser fluence, laser spot size, and substrate temperature were found to have little effect on composition within the range investigated. Ablation from a fresh target surface results in films enriched in copper and barium, both of which decrease in concentration until a steady state condition is achieved. Oxygen pressure and target-substrate distance have a significant effect on film composition. In vacuum, copper and barium are slightly concentrated at the center of deposition. With the introduction of an oxygen background pressure, scattering results in copper and barium depletion in the deposition center, an effect which increases with increasing target-substrate distance. A balancing of these two effects results in stoichiometric deposition.

Composition variations in pulsed-laser-deposited Y-Ba-Cu-O thin films as a function of deposition parameters

We present experimental results of photoablated product and kinetic energy (KE) distributions from the ultraviolet laser ablation of a sintered YBa2Cu3O6+x wafer at the laser wavelengths 351, 248, and 193 nm. Data is presented which spans the laser fluence range beginning at the threshold for species ejection (50 mJ/cm2) to nearly that required for the formation of an above surface plasma (800 mJ/cm2). The goal of this experiment was to measure changes in the photophysical process as the incident laser fluence was increased above the threshold value. Our results show, that near the laser threshold fluence, the photoejected products consist of small atomic and oxide species. An unforeseen result for the UV laser wavelengths used, is the lack of CuO+/CuO and free oxygen (O+/O, O+2/O2) in the mass spectrum. In addition, the product distributions are dependent on the laser wavelength. Measured also, at laser threshold fluence, are the nascent photoejected cation kinetic energy distribution. Here our results s...

Laser photodecomposition of sintered YBa2Cu3O6+x: Ejected species population distributions and initial kinetic energies for the laser ablation wavelengths 351, 248, and 193 nm

A study of the interaction of pulsed coherent radiation from a Nd:YAG laser (wavelength 1064 nm) with solid targets used in the deposition of YBa2Cu3O7−x superconducting thin films is presented. Electron microscopy, time-of-flight mass spectroscopy, laser induced fluorescence spectroscopy, precise target weight loss measurements, and wet chemical analysis of collected films were employed. The photon-target interaction, the gas phase ablated particle beam, and the collected film were each probed. Conclusions concerning the physics of the ablation process and important practical considerations for the production of high quality superconducting films were obtained.

High temperature superconducting thin films: The physics of pulsed laser ablation

Thin films of Ho1Ba2Cu3O7 − x and Y1Ba2Cu3O7 − x were deposited on SrTiO3 and Al2O3, substrates by pulsed laser deposition of high-Tc bulk superconductor pellets in vacuum. Following annealing in O2 at 800–900 °C the films were superconducting with typical Tc (50%) = 89 K and transition widths of 10 K. Rutherford backscattering spectrometry (RBS) and secondary ion mass spectrometry (SIMS) were utilized to study the stoichiometry of the as-deposited films for laser energy, densities between 0.11 and 4.5 J cm−2. The films were deficient in holmium and yttrium for energy densities below 0.6 and 0.4 J cm −2, respectively. The films were stoichiometric for fluences above 0.6 J cm−2. In addition, preliminary time dependence and spectroscopic observations of the laser-produced plasma are presented. The results indicate an ablation mechanism that at high energy densities preserves stoichiometry. TEM and x-ray characterization of annealed, superconducting Ho1Ba2Cu3O7 − x films on (100) SrTiO3 showed mixed regions of epitaxially oriented 1:2:3 material with either the c axis or a axis oriented along the surface normal. The a-axis-oriented material grew preferentially in the films with b, c, twinning.

R. E. Valiga

Papers

Pulsed laser deposition of thin superconducting films of Ho1Ba2Cu3O7 − x and Y1Ba2Cu3O7 − x