Highly reproducible large-area and double-sided pulsed laser deposition of HTSC YBCO:Ag thin films for microwave applications

Large-area pulsed laser deposition (PLD) producing high-quality YBa₂Cu₃O_7-x (YBCO) thin films on both sides of R-plane sapphire substrates with CeO₂ buffer layer is used routinely to optimize planar microwave stripline filters for satellite and mobile communication systems. A relatively simple PLD arrangement with fixed laser plume and rotating substrate, with an offset between the laser plume and the center of the substrate is employed to deposit laterally homogeneous 3-inch-diameter Ag-doped YBCO thin films. The YBCO:Ag films are about 250 nm thick and have laterally homogeneous critical current densities of more than 3.5 MA/cm² at 77 K and homogeneous maps of microwave surface resistance R_s of about 40 m Q at 145 GHz and 77 K. The R_s at 8.5 GHz and 77 K, determined in the center position of the YBCO:Ag films, remains constant at about 370 7 Q up to a microwave surface magnetic field of about 10 mT. After experience with more than 700 double-sided 3-inch-diameter films, a high degree of homogeneity and reproducibility of j_c and R_s is reached. The PLD-YBCO:Ag films are suitable for microwave applications envisaged for future communication systems.     

Deposition of Ti:sapphire thin films by reactive pulsed laser ablation using liquid metals and oxygen

Ti:sapphire films were grown using molten Al-Ti alloy ablation targets with either O₂ gas pulses or O₂ background reactive medium on sapphire (0001) substrates. The films were characterized by the use of XRD, RHEED, AFM, and XPS. While the films deposited at a substrate temperature of 650 °C showed three-dimensional epitaxial growth, the films deposited at 1000 °C exhibited a two-dimensional structure. Annealing of the low-temperature deposited films improved the crystal quality but failed to improve the surface morphology. Ti exists in the host sapphire lattice in the form of Ti³⁺ for films deposited at lower temperatures, whereas it assumes the tetravalent form in the high-temperature deposited films. The valence states of Ti identified by XPS studies are in agreement with low-temperature luminescence results.     

Growth of oriented Pb(ZrxTi1-x)O3 thin films on glass substrates by pulsed laser deposition

Oriented crystalline Pb(Zr_xTi_1-x)O₃ (x=0.53) (PZT) thin films were deposited on metallized glass substrates by pulsed laser deposition (1060-nm wavelength Nd:YAG laser light, 10-ns pulse duration, 10-Hz repetition rate, 0.35-J/pulse and 25-J/cm² laser fluence), from a commercial target at substrate temperatures in the range 380-400 °C. Thin films of 1-3 7m were grown on Au(111)/ Pt/NiCr/glass substrates with a rate of about 1 Å/pulse on an area of 1 cm². The deposited PZT films with perovskite structure were oriented along the (111) direction, as was revealed from X-ray diffraction spectra. Fourier transform infrared spectroscopy (FTIR) was performed on different PZT films so that their vibrational modes could be determined. Piezoelectric d₃₃ coefficients up to 30 pC/N were obtained on as-deposited films. Ferroelectric hysteresis loops at 100 Hz revealed a remanent polarization of 20 7C/cm² and a coercive field of 100 kV/cm.     

Electrical and optical properties of indium tin oxide thin films grown by pulsed laser deposition

Indium tin oxide (ITO) thin films (200-400 nm in thickness) have been grown by pulsed laser deposition (PLD) on glass substrates without a post-deposition anneal. The electrical and optical properties of these films have been investigated as a function of substrate temperature and oxygen partial pressure during deposition. Films were deposited at substrate temperatures ranging from room temperature to 300 °C in O₂ partial pressures ranging from 0.1 to 100 mTorr. For 300 nm thick ITO films grown at room temperature in oxygen pressure of 10 mTorr, the electrical conductivity was 2.6᎒^-3 Q^-1cm^-1 and the average optical transmittance was 83% in the visible range (400-700 nm). For 300 nm thick ITO films deposited at 300 °C in 10 mTorr of oxygen, the conductivity was 5.2᎒^-3 Q^-1cm^-1 and the average transmittance in the visible range was 87%. Atomic force microscopy (AFM) measurements showed that the RMS surface roughness for the ITO films grown at room temperature was ~7 Å, which is the lowest reported value for the ITO films grown by any film growth technique at room temperature.     

Low-temperature growth of epitaxial ZnO films on (001) sapphire by ultraviolet- assisted pulsed laser deposition

ZnO thin films have been grown on thin Si₃N₄ membranes and (001) sapphire substrates by an ultraviolet-assisted pulsed laser deposition (UVPLD) technique. The microstructure of the films grown on Si₃N₄ membranes, investigated by transmission electron microscopy, showed that crystalline and textured films can be grown by UVPLD at a substrate temperature of only 100 °C. For deposition temperatures higher than 400 °C, ZnO films grown on sapphire substrates were found to be epitaxial by Rutherford backscattering (RBS) and X-ray diffraction measurements. The minimum yield of channeling RBS spectra recorded from films deposited at 550 °C was around 2% and the FWHM of the rocking curve for the (002) diffraction peak was 0.17°; these values are similar to those recorded from ZnO layers grown by conventional PLD at 750 °C.     

Off-axis pulsed laser deposition system for epitaxial oxide growth on substrates up to 2 inches in diameter

A novel off-axis pulsed-laser deposition (PLD) system for ferroelectric oxide thin films has been developed. The substrates are mounted "upside-down" and are rotating. The maximum substrate size is 2 inches in diameter. The optical and structural properties of the grown BaTiO₃ films are compared to the films produced by an on-axis PLD system. The stoichiometry and thickness were checked with Rutherford backscattering spectrometry (RBS). The crystalline quality and orientation were investigated with X-ray diffraction (XRD) and Rutherford backscattering spectrometry in channeling configuration (RBS/C). Using atomic force microscopy, the rms surface roughness was measured. The BaTiO₃ films grown on MgO form a planar optical waveguide. The optical losses and the refractive indices of these waveguides were determined with a prism coupling setup. Films grown on 10᎒ mm² MgO (100) substrates in on-axis geometry show optical waveguide losses less than 3 dB/cm.     

A laser-ablation system for deposition of high-temperature superconducting thin films for device applications

We present a compact-size laser-ablation system to produce high-temperature superconducting (HTS) YBa₂Cu₃O_7-' (YBCO) thin films for component applications. The system has been designed for deposition of multilayer structures on 5-cm-diameter substrates and for reliable operation with reduced need for maintenance. The performance of the system has been studied by depositing YBCO films on small LaAlO₃ substrates. The films have critical temperatures of 88-90 K and critical current densities of 0.9-4.5 MA/cm² as measured with an inductive technique.     

Cubic boron nitride deposition on silicon substrates at room temperature by KrF excimer laser ablation of h-BN

A hexagonal-BN target was ablated by high-fluence (6 and 12 J/cm²) KrF excimer laser pulses in low-pressure (5 Pa) N₂ atmosphere, without any aid of ion bombardment and heating of the Si substrate. Investigations of the deposited films show that the cubic-BN phase was deposited. The film deposited at 6 J/cm² appears to contain a higher cubic phase content with respect to the one deposited at 12 J/cm².     

Structural and electrical properties of La0.5Sr0.5CoO3 films on SrTiO3 and porous a-Al2O3 substrates

Films of La_0.5Sr_0.5CoO₃ (LSCO) have been deposited on specially treated TiO₂-terminated (001) SrTiO₃ substrate surfaces and on macroporous polycrystalline !-Al₂O₃ substrates, having a mean pore diameter of 80 nm, by pulsed laser deposition. The films deposited on SrTiO₃ are good conducting, (001) textured, and exceptionally smooth (1-2 Å for 100 nm thick films). LSCO films deposited on porous !-Al₂O₃ are polycrystalline and exhibit good crystallographic and electrical properties despite the large substrate roughness and the differences in lattice parameters and crystal structure between the film and the substrate. Different growth modes have been observed on the porous !-Al₂O₃ substrates depending on the oxygen pressure during film deposition. Films grown at an oxygen pressure of 10^-1 mbar are macroporous, whereas films grown at 10^-2 mbar completely cover the substrate pores. In the latter case, strain effects lead to film cracking.     

Ablation of transparent solids during self-limited deposition of diamond-like films from liquid hydrocarbons

A novel effect is studied of self-limitation of the diamond-like film thickness during laser irradiation of the interface of transparent substrates with liquid aromatic hydrocarbons. The interface is exposed through the transparent substrate to radiation of a copper vapor laser (wavelength of 510.6 nm, pulse duration of 20 ns). The thickness of diamond-like film increases linearly to 80-100 nm with the number of laser pulses and then saturates, while the substrate is ablated with nearly constant rate. This ablation rate depends on the thermal expansion coefficient of the substrate (glass, fused silica, sapphire, or CaF₂). The absorption of extinction coefficient of deposited films measured by ellipsometry is of order of 10⁴ cm^-1 and is sufficient to cause the significant heating of the interface. The ablation of the transparent substrates is due to their unequal thermal expansion compared to the diamond-like film having different thermal expansion coefficient. The measured ablation rates scale from 0.2 Å/pulse for glass to 4.5 Å/pulse for CaF₂. A 7m spatial resolution of the ablation process has been demonstrated for fused silica.     

Deposition of highly oriented Bi12SiO20 thin films on Y-stabilized zirconia and SiO2 by pulsed-laser deposition

We describe the deposition and characterization of Bi₁₂SiO₂₀ (bismuth silicon oxide; BSO) thin films on Y-stabilized zirconia (YSZ) and SiO₂ glass substrates by pulsed-laser deposition (PLD) for the application of an electric field sensor. It was found that all films deposited on YSZ substrates heated at 400 °C and more were crystallized and the (310) plane was perpendicular to the substrate normal. The highly (310) oriented crystallized films were even deposited on SiO₂ glass substrates, and this will make it possible to grow the crystallized films on the end surface of a SiO₂ glass fiber.     

Self-injection length in La0.7Ca0.3MnO3-YBa2Cu3O7-δ ferromagnet-superconductor multilayer thin films

We have carried out extensive studies on the self-injection problem in barrierless heterojunctions between La_0.7Ca_0.3MnO₃ (LCMO) and YBa₂Cu₃O_7-δ (YBCO) thin films. The heterojunctions were formed in situ by sequentially growing LCMO and YBCO films on 〈100〉 LaAlO₃ (LAO) substrate using a pulsed laser deposition (PLD) system. YBCO micro-bridges with 64 μm width were patterned both on the LAO (control) and LCMO side of the substrate. Critical current, I _c, was measured at 77 K on both the control side as well as the LCMO side for different YBCO film thickness. It was observed that while the control side showed a J _c of ∼ 2 × 10⁶ A/cm², the LCMO side showed about half the value for the same thickness (1800 ?). The difference in J _c indicates that a certain thickness of YBCO has become ‘effectively’ normal due to self-injection. From the measurement of J _c at two different thicknesses (1800 ? and 1500 ?) of YBCO films both on the LAO as well as the LCMO side, the value of self-injection length (at 77 K) was estimated to be ∼ 900 ?. To the authors’ best knowledge, this is the first time that self-injection length has been quantified. A control experiment carried out with LaNiO₃ deposited by PLD on YBCO did not show any evidence of self-injection.     

Electrical Characterization of Deep Trap Properties in High-k Thin-Film HfO2 Dielectric

Deep-trap properties of high-dielectric-constant （k） HfO2 thin films are investigated by deep-level transient spectroscopy and capacitance-voltage methods. The hole traps of the HfO2 dielectric deposited on a p-type Si substrate by sputtering are investigated in a metal-oxide-semiconductor structure over a temperature range of 300-500K. The potential depth, cross section and concentration of hole traps are estimated to be about 2.5eV, 1.8 ×10^-16 cm^2 and 1.0 × 10^16 cm^-3, respectively.     

Preferential orientation of modified SrBi2Nb2O9 ferroelectric thin films prepared by pulsed laser deposition

We report on the deposition of SrBi₂Nb₂O₉ and Sr_1-xNa_xBi_2-xTe_xNb₂O₉ ferroelectric thin films on Pt/TiO₂/SiO₂/(100)Si substrates using the pulsed laser deposition technique. Deposition on substrates heated to 600-700 °C produces {11l} film texture and dense films with grain sizes up to about 500 nm. The recrystallization at 700 °C of amorphous films deposited at lower temperatures enhances the contribution of the {100} and {010} orientations. These films show smaller grain size, namely 50-100 nm. {11l}-oriented Sr_1-xNa_xBi_2-xTe_xNb₂O₉ films have remnant polarization P_rۆ 7C/cm², a coercive field E_c䏐 kV/cm and dielectric constant, )𪓴. The low value of P_r is probably related to the low fraction of grains with the ferroelectric axis in the direction of the applied field, E. The recrystallized films have more grains with the ferroelectric axis parallel to E; however, they have a low resistivity which so far has prevented electrical characterization.     

Adjusting chemical bonding of hard amorphous CSixNy thin films by N*-plasma-assisted pulsed laser deposition

Hard amorphous carbon silicon nitride thin films have been grown by pulsed laser deposition (PLD) of various carbon silicon nitride targets by using an additional nitrogen RF plasma source on [100] oriented silicon substrates at room temperature. The influence of the number of laser shots per target site on the growth rate and film surface morphology was studied. Up to about 30 at. % nitrogen and up to 20 at. % silicon were found in the films by Rutherford backscattering spectroscopy (RBS) and X-ray photoelectron spectroscopy (XPS). The XPS of the films showed a clear correlation of binding energy to the variation of PLD parameters. The films show a universal hardness value up to 23 GPa (reference value for silicon substrate 14 GPa) in dependence on target composition and PLD parameters. The results emphasise the possibility of variation of chemical bonding and corresponding properties, such as nanohardness, of amorphous CSi_xN_y thin films by the plasma-assisted PLD process.     

Role of bismuth precursor in crystallization of SrBi2Ta2O9 thin films

Crystallization of SrBi₂Ta₂O₉ (SBT) thin films was studied as a function of viscosity of bismuth precursor and baking temperature, in order to fabricate capacitors with improved ferroelectric properties. SBT thin films were deposited on to Pt substrates using a chemical solution deposition (CSD) technique. Post-deposition anneal at 750 °C for 1 h in oxygen atmosphere revealed a significant influence of baking temperature and the viscosity of bismuth precursor on the microstructure and the ferroelectric properties of SBT thin films. A high baking temperature (350 °C) and a low viscosity of bismuth precursor (8 cp) yielded larger amounts of Bi₂O₃ secondary phase, smaller SBT grains (104 nm), and lower remanent polarization (P_r=2.0 7c/cm²). Additionally, these films exhibited a very high rate of ageing (>45% reduction in P_r after 7 days). A modified CSD process is suggested, which could suppress the formation of Bi₂O₃ secondary phase. Films fabricated using modified CSD technique exhibited a much larger grain size of 165 nm, higher P_r of 7.2 7c/cm², and significantly improved ageing characteristics (<1% reduction in P_r after 7 days). A qualitative model to describe the ageing in SBT-based capacitors is also suggested.     

Fabrication of ZnO thin films by femtosecond pulsed laser deposition

The growth of ZnO thin films on sapphire substrate using the femtosecond PLD technique is reported. The effect of substrate temperature and oxygen pressure on the structural properties of the films was studied. Highly c-axis oriented ZnO films can be grown on sapphire substrates under vacuum conditions using the femtosecond PLD process. There is an optimum substrate temperature for the pulsed laser deposition of ZnO film that enhances the thermodynamic stability and allows the formation of well-crystallized thin films. The crystal quality of the films can be further improved by increasing the deposition time and introducing oxygen during the pulsed laser deposition process.     

Piezoelectric Pb0.7La0.2TiO3 prepared by pulsed laser deposition on (100)InP

La-modified PbTiO₃ (PLT) thin films have been deposited by pulsed laser deposition on (100)InP substrates. The nominal target composition was selected to optimize piezoelectric properties of the material. It is shown that PLT deposition on as-received InP produces amorphous PLT films because of the presence of a native oxide on the substrate. PLT films deposited on bare InP have poor adhesion as a result of the surface reoxidation of the substrate due to the high oxygen pressure required for the deposition of stoichiometric PLT. To prevent substrate oxidation, several buffer oxides (CeO₂, ZrO₂, SrO, Y-stabilized ZrO₂, MgO, and SrTiO₃) have been grown in vacuum on (100)InP. Highest-quality heteroepitaxy was found with Y-stabilized ZrO₂ (YSZ), being 𘜄¢{100} YSZ𘜄¢{100} InP oriented. The PLT deposited on this buffer layer is oriented with the [101] direction perpendicular to the substrate surface plane.     

A new method to preserve the c-axis growth of thick YBa2Cu3O7–δ films grown by pulsed laser deposition

YBa₂Cu₃O_7–δ (YBCO) films were prepared on (1 0 0) MgO substrates by pulsed laser deposition (PLD) method. In order to eliminate the a-axis growth, which is commonly observed in the YBCO film thicker than a critical value, we developed a new PLD target that was sintered at a temperature far below YBCO 123 phase formation. The surface analysis made by AFM technique confirmed that very fine particles of around 20 nm size could be ejected from the new target to the substrate. The fine oxide clusters could be easily moved and incorporated into the YBCO phase thus benefited the c-axis growth even in the thick films. For instance, only the c-axis growth in the new film with a thickness of about 650 nm was larger than a critical thickness of the a-axis growth. However, in the standard film of the same thickness, there is 24.5% of the a-axis growth accompanying the main c-axis growth. Therefore, the c-axis growth could be preserved in the very thick YBCO film by a non-superconducting target.     

Investigation on FR(LT)–FR(HT) phase transition and pyroelectric properties of pulsed laser deposited Pb(Zr0.93Ti0.07)O3 thin films

The preparation process, crystallinity and electrical properties of pulse laser deposited Pb(Zr_xTi_1−x)O₃ (PZT) thin films were investigated in this paper. PZT (x = 0.93) thin film samples deposited at different substrate temperatures were prepared. Si (1 1 0) was the substrate; Ag and YBCO were the top electrode and the bottom electrode respectively. The bottom electrode YBCO was deposited on the Si substrate by pulsed laser deposition (PLD), and then PZT was epitaxially deposited on YBCO also by PLD. After annealing, the top electrode Ag was prepared on PZT by thermal evaporation, and then the Ag/PZT/YBCO/Si structured thin films were obtained. The XRD and the analysis of their electrical characters showed that, when the substrate temperature was elevated from 600 °C to 800 °C, the crystallinity and electrical properties of PZT thin films became better and better, and the F_R(LT)–F_R(HT) phase transition of PZT (x = 0.93) thin films occurred at 62 °C. The PZT film deposited at 800 °C had the best pyroelectric properties, and when the F_R(LT)–F_R(HT) phase transition of this film occurred, the peak value of pyroelectric coefficient (p) was obtained, with a value of 1.96 × 10⁻⁶ C/(cm² K). The PZT film deposited at 800 °C had the highest remnant polarization (P_r) and the lowest coercive field (E_c), with the values of 34.3 μC/cm² and 41.7 kV/cm respectively.