Structural, electrical, and surface characteristics of La0.5Sr0.5CoO3 thin films prepared by pulsed-laser deposition

A parametric study of the growth of La_0.5Sr_0.5CoO₃ (LSCO) thin films on (100) MgO substrates by pulsed-laser deposition (PLD) is reported. Films are grown under a wide range of substrate temperature (450–800 °C), oxygen pressure (0.1–0.9 mbar), and incident laser fluence (0.8–2.6 J/cm²). The optimum ranges of temperature, oxygen pressure, and laser fluence to produce c-axis oriented films with smooth surface morphology and high metallic conductivity are identified. Films deposited at low temperature (500 °C) and post-annealed in situ at higher temperatures (600–800 °C) are also investigated with respect to their structure, surface morphology, and electrical conductivity. Received: 20 November 1998 / Accepted: 6 July 1999 / Published online: 21 October 1999     

Pulsed laser deposition of ZnO as conductive buffer layer of (001)-LiNbO3 thin films

1 (LO) mode peak at 579 cm^-1, indicating oxygen deficiency in the films. Significant dependence of the electrical property for the films on substrate temperature was shown. The I–V relation of the films exhibited non-ohmic behavior. Whereas the films deposited above 500 °C showed a metal-like property, at a lower substrate temperature semiconducting thin films were achieved. The (001)-oriented LiNbO₃/ZnO heterostructure was successfully prepared on quartz fused and (001) sapphire plates. Received: 6 April 1998/Accepted: 26 May 1998     

Defect reduction and surface passivation of SiO2/Si by heat treatment with high-pressure H2O vapor

Heat treatment with high-pressure H₂O vapor was applied to improve interface properties of SiO₂/Si and passivate the silicon surface. Heat treatment at 180–420 °C with high-pressure H₂O vapor changed SiO_x films, 150 nm thick formed at room temperature by thermal evaporation in vacuum, into SiO₂ films with a Si-O-Si bonding network similar to that of thermally grown SiO₂ films. Heat treatment at 130 °C with 2.8×10⁵ Pa H₂O for 3 h reduced the recombination velocity for the electron minority carriers from 405 cm/s (as-fabricated 150-nm-thick SiO_x/Si) to 5 cm/s. Field-effect passivation was demonstrated by an additional deposition of defective SiO_x films on the SiO₂ films formed by heat treatment at 340 °C with high-pressure H₂O vapor. The SiO_x deposition reduced the recombination velocity from 100 cm/s to 48 cm/s. Received: 1 March 1999 / Accepted: 28 March 1999 / Published online: 24 June 1999     

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.     

Structural and electrical properties of polycrystalline PbZr0.5Ti0.5O3 films deposited on La0.5Sr0.5CoO3 coated silicon by sol-gel process

La_0.5Sr_0.5CoO₃ (LSCO) films have been grown on Si (100) by a metalorganic chemical liquid deposition (MOCLD) technique using lanthanum acetate, strontium acetate and cobalt acetate as the starting materials. Subsequent PbZr_0.5Ti_0.5O₃ (PZT) films were deposited onto LSCO films by a modified sol-gel method. Field-emission scanning electron microscopy and X-ray diffraction analysis show that PZT and LSCO films are polycrystalline and entirely perovskite phase. At an applied electric field of 250 kV/cm, the Pt/PZT/LSCO capacitor shows no polarization fatigue after 3×10⁹ switching cycles and an internal electric field; the remnant polarization P_r and the coercive field E_c are about 22 μC/cm² and 73 kV/cm, respectively. The dielectric constant of PZT films is 650 at a frequency of 1 kHz. Received: 20 February 2001 / Accepted: 6 June 2001 / Published online: 30 August 2001     

Growth of polycrystalline La0.5Sr0.5CoO3 films by femtosecond pulsed laser deposition

In this paper we present the growth of La_0.5Sr_0.5CoO₃ (LSCO) films on MgO, quartz, and silicon substrates by pulsed laser deposition (PLD) using a Ti:sapphire laser (50 fs, 800 nm wavelength). The morphology and the structure of the films were studied by X-ray diffraction, atomic force microscopy, and scanning electron microscopy. The films were polycrystalline and exhibit a good adherence to the Si substrate. Different deposition parameters such as substrate temperature, oxygen pressure, and laser fluence were varied to achieve good surface quality and low resistivity crystalline films. We also defined the optimum conditions in which the deposited film surface is particulate free. The best films (droplets free) were grown at 625 °C, in an ambient oxygen pressure of 6 mbar, with an incident laser fluence of 0.19 J/cm². This is a mandatory step in the complex work of fabricating La_0.5Sr_0.5CoO₃/BaTiO₃/La_0.5Sr_0.5CoO₃ heterostructures for the development of thin film capacitors for non-volatile ferroelectric access memory devices. PACS 81.15 Fg; 42.62-b; 68.65.Ac     

Production and characterization of Nd,Cr:GSGG thin films on Si(001) grown by pulsed laser ablation

Nd,Cr:Gd₃Sc₂Ga₃O₁₂ (GSGG) thin films have been produced for the first time. They were grown on Si(001) substrates at 650 °C by pulsed laser ablation at 248 nm of a crystalline Nd,Cr:GSGG target rod. The laser plume was analyzed using time-of-flight quadrupole mass spectroscopy, and consisted of elemental and metal oxide fragments with kinetic energies typically in the range 10 to 40 eV, though extending up to 100 eV. Although films deposited in vacuum using laser fluences of 0.8±0.1 J cm⁻² reproduced the Nd,Cr:GSGG bulk stoichiometry, those deposited using fluences above ≈3 J cm⁻² resulted in noncongruent material transfer and were deficient in Ga and Cr. Attempts to grow films using synchronized oxygen or oxygen/argon pulses yielded mixed oxide phases. Under optimal growth conditions, the films were heteroepitaxial, with GSGG(001)[100]∥Si(001)[100], and exhibited Volmer–Weber-type growth. Room-temperature emission spectra of the films suggest efficient non-radiative energy transfer between Cr³⁺ and Nd³⁺ ions, similar to that of the bulk crystal. Received: 1 October 1999 / Accepted: 15 October 1999 / Published online: 23 February 2000     

Spin-polarized inter-grain tunneling as the probable mechanism for low-field magnetoresistance in partially crystallized La0.5Sr0.5MnO3 thin films

Amorphous/crystalline mixed La_0.5Sr_0.5MnO₃ (LSMO) thin films on quartz wafers are prepared at different depositing temperatures using laser ablation and their low-field magnetoresistive property is investigated. It is argued that the insulating amorphous layers separating the magnetic microcrystalline grains may act as the barriers for electron tunneling. The rapid decay of magnetoresistance with increasing temperature is explained by the spin-polarized inter-grain tunneling. Given the spin-polarized inter-grain tunneling as the probable mechanism, it is believed that the spin flip during inter-grain tunneling reaches a minimum at the optimized depositing temperature of 600 °C and consequently the maximal low-field magnetoresistance is obtained. Received: 7 September 2000 / Accepted: 19 December 2000 / Published online: 23 March 2001     

Pulsed laser deposition of NdNiO3 thin films

We report the structural and transport properties of NdNiO₃ thin films prepared via pulsed laser deposition over various substrates. The films were well textured and c-axis oriented with good crystalline properties. The electrical resistivity of the films undergoes a metal-insulator transition, depending on the deposition process. Well-defined first order metal-insulator phase transition (T_MI) was observed in the best quality films without high pressure processing. Various growth conditions such as substrate temperature, oxygen pressure and thickness were varied to see their influence on T_MI. Deposition temperature was found to have a great impact on the electrical and structural properties of these films. Further the films deposited on LaAlO₃ substrate were found to be highly oriented with uniform grain size as observed from X-ray diffraction and atomic force microscopy, whereas those on Si substrate were polycrystalline, dense and randomly oriented.     

Growth and structure of Bi0.5(Na0.7K0.2Li0.1)0.5TiO3 thin films prepared by pulsed laser deposition technique

Bi_0.5(Na_0.7K_0.2Li_0.1)_0.5TiO₃ (BNKLT) thin films were prepared on Pt/Ti/SiO₂/Si substrates by pulsed laser deposition (PLD) technique. The films prepared were examined by using X-ray diffraction (XRD), scanning electron microscopy (SEM) and atomic force microscopy (AFM). The effects of the processing parameters, such as oxygen pressure, substrate temperature and laser power, on the crystal structure, surface morphology, roughness and deposition rates of the thin films were investigated. It was found that the substrate temperature of 600 °C and oxygen pressure of 30 Pa are the optimized technical parameters for the growth of textured film, and all the thin films prepared have granular structure, homogeneous grain size and smooth surfaces.     

TbMnO3 epitaxial thin films by pulsed-laser deposition

Epitaxial TbMnO₃ films have been fabricated on SrTiO₃(001) and LaAlO₃(001) substrates by pulsed laser deposition (PLD), the structure and surface morphology of the films were characterized by X-ray diffraction with Cu K_α radiation and atomic force microscopy. The electrical transport and magnetic properties of the TbMnO₃ films and bulk were examined, the resistivity and the forbidden band width E_g change with epitaxial orientation, semiconductor transport properties are found in the films and bulk, the average of the E_g of the films on SrTiO₃ and on LaAlO₃ is equal to the E_g of the bulk. The two TMO films have different magnetization mode, the magnetization of the film on SrTiO₃ have an analogy to that of TbMnO₃ single crystal.     

Transport Behaviour of La0.8Sr0.2AlO3 Thin Film on Oxygen Deficient SrTiO3 Substrate

La_0.8Sr_0.2AlO₃ (LSAO) thin films are grown on SrTiO₃ (STO) and MgO substrates by laser molecular beam epitaxy. The LSAO thin film on oxygen deficient STO substrate exhibits metallic behaviour over the temperature range of 80--340K. The optical transmittance spectrum indicates that theLSAO thin films on MgO substrate are insulating at room temperature. The transport properties of LSAO thin films on STO substrates deposited in different oxygen pressure are compared. Our results indicate that oxygen vacancies in STO substrates should be mainly responsible for the transport behaviour of LSAO thin films.     

Piezoelectric non-linearity in PbSc0.5Ta0.5O3 thin films

Epitaxial (001)-oriented PbSc_0.5Ta_0.5O₃ (PST) thin films were deposited by pulsed laser deposition. Local piezoelectric investigations performed by piezoelectric force microscopy show a dual slope for the piezoelectric coefficient. A piezoelectric coefficient of 3 pm/V was observed at voltages up to 0.8 V. However, at voltages above 0.8 V, there is a steep increase in piezoelectric coefficient mounting to 23.2 pm/V. This nonlinear piezoelectric response was observed to be irreversible in nature. In order to better understand this nonlinear behavior, voltage dependent dielectric constant measurements were performed. These confirmed that the piezoelectric non-linearity is indeed a manifestation of a dielectric non-linearity. In contrast to classical ferroelectric systems, the observed dielectric non-linearity in this relaxor material cannot be explained by the Rayleigh model. Thus the dielectric non-linearity in the PST films is tentatively explained as a manifestation of a percolation of the polar nano regions.     

Effect of growth defects on microwave properties in epitaxial Ba0.5Sr0.5TiO3 thin films grown on (001) MgO by pulsed laser deposition

Ba_0.5Sr_0.5TiO₃ (BSTO) films have been grown heteroepitaxially on (001) MgO substrates by pulsed laser deposition (PLD) to fabricate microwave phase shifters for the wide frequency range 45 MHz–50 GHz. Both as-grown and ex situ annealed films have a cube on cube epitaxial relationship with ?100?BSTO//?100?MgO. Threading dislocations are the dominant defects, mostly with Burgers vectors b = ?101?. Growth at 10^?1 mbar oxygen pressure, compared to 10^?4 mbar, resulted in significantly better properties. Ex situ annealing of the film grown at 0.1 mbar resulted in a reduction of 40% in threading dislocation density and a 40% increase in dielectric tunability.     

Anisotropic in-plane strain in W-doped (Ba,Sr)TiO<Subscript>3</Subscript> thin films deposited by pulsed-laser deposition on (001)MgO

The structural and the microwave dielectric properties of Ba_xSr_(1-x)TiO₃ films (BST) with x=0.5, 0.6 and 0.7, containing 1 mol % W have been investigated. The films were grown by pulsed-laser deposition on MgO (001) substrates at a temperature of 720 °C in an oxygen pressure from 3 to 500 mTorr. The film structures were determined by X-ray diffraction. The lattice parameters were fitted to a tetragonal distortion of a cubic lattice. The out-of-plane lattice parameter (c) was calculated from the position of the (004) reflection. Using c, the in-plane lattice parameter, a, was calculated from the position of the (024) and (224) reflections. A deviation in the calculated values for a, beyond the systematic error, was found in the in-plane lattice parameter, suggesting an in-plane orthorhombic distortion (a, a’). Films with x=0.7 showed a minimum in-plane distortion due to a better lattice match with the substrate. The ratio of the in-plane and out-of-plane lattice parameters was calculated as a measure of the lattice distortion (a/c and a’/c). The dielectric properties of the films deposited were measured at room temperature at 2 GHz using gap capacitors fabricated on top of the dielectric film. For all Ba/Sr ratios investigated in the W-doped material, the dielectric Q (1/cosδ) was observed to be insensitive to the oxygen deposition pressure. A peak in the change in the dielectric constant, as a function of an applied electric field (0–80 kV/cm), was observed for films deposited in 50 mTorr of oxygen. The largest K-factor, K=(ε(0)-ε(V )/ε(0)×Q(0)), for films deposited from a BST x=0.6 (1 mol % W-doped) target was observed in the film that had a minimum in-plane strain, where a∼a’ and c was greater than a and a’. Received: 4 July 2002 / Accepted: 5 July 2002 / Published online: 17 December 2002 RID="*" ID="*"Permanent address: Nuclear Research Center–Negev, P.O. Box 9001 Beer-Sheva, Israel RID="**" ID="**"Corresponding author. Fax: +1-202/767-5301, E-mail: horwitz@ccsalpha3.nrl.navy.mil     

Improvement of metal–ferroelectric–silicon structures without buffer layers between Si and ferroelectric films

Si-based metal–ferroelectric–semiconductor (MFS) structures without buffer layers between Si and ferroelectric films have been developed by depositing SrBi₂Ta₂O₉ (SBT) directly on n-type (100)-oriented Si. Some effective processes are adopted to improve the electrical properties of these MFS structures. Contrary to the conventional MFS structures with top electrodes directly on ferroelectrics, our MFS structures have been developed with thin dense SiO₂ films deposited between ferroelectric films and top electrodes. Due to the SiO₂ films, the leakage current densities of MFS structures are reduced to 2×10^-8 A/cm² under the bias of 5 V. The C-V electrical properties of the MFS structures are greatly improved after annealing at 400 °C in N₂ ambient for 1 h. The C-V memory windows are increased to 3 V, which probably results from the decrease of the interface trap density at the Si/SBT interface. Received: 7 September 1999 / Accepted: 24 November 1999 / Published online: 2 August 2000     

Room-temperature epitaxial growth of CeO2(001) films on YSZ buffered Si(001) substrates

2 (001) epitaxial thin films deposited on Si(001) with yttria-stabilized zirconia buffers have been obtained for the first time at room temperature by pulsed-laser deposition. The influence of oxygen pressure on the crystal quality of CeO₂ was studied for the films deposited at 100 °C. The rocking curve full width at half maximum of the CeO₂(002) peak for films deposited at room temperature and 100 °C was between 1° and 2°, for oxygen pressures below 3×10^-2 mbar. The best crystal quality was obtained at around 3×10^-3 mbar. Epitaxial growth at room temperature was confirmed by cross-sectional transmission electron microscopy. Scanning electron microscopy and atomic force microscopy revealed very smooth surfaces for oxygen pressure below 3×10^-2 mbar, with rms roughness values around 0.3 nm over 5 μm×5 μm. Received: 25 September 1997/Accepted: 22 April 1998     

Properties of K0.5Bi0.5TiO3 thin films deposited on different substrates

K_0.5Bi_0.5TiO₃ thin films were deposited on fused quartz, n-type Si(100) and Pt/TiO₂/SiO₂/Si substrates by repeated coating/dying cycles. X-ray diffraction analysis shows that the films annealed at 700 °C for 10 min present perovskite phase. Atomic force microscopy reveals that the surface morphology is smooth, the grain sizes of the films on Si(100) are quite larger than on fused quartz. The capacitance-voltage hysteresis loops at various sweeping speed are collected as are polarization types. The films in the ON and OFF states are relatively stable. The films also exhibit a hysteresis loop at an applied voltage of 4 V, with a remanent polarization of 9.3 μC/cm² and a coercive voltage of 2 V. The insulating property of negative bias voltage is better than that of positive bias voltage. The transmittance of the films is between 74 and 82% in the wavelength range of 200-2000 nm.     

Trap characterization for Bi4Ti3O12 thin films by thermally stimulated currents

Thermally stimulated current (TSC) measurements performed in the 100 K–400 K temperature range on Bi₄Ti₃O₁₂ (BiT) thin films annealed at 550 °C and 700 °C had revealed two trapping levels having activation energies of 0.55 eV and 0.6 eV. The total trap concentration was estimated at 10¹⁵ cm⁻³ for the samples annealed at 550 °C and 3×10¹⁵ cm⁻³ for a 700 °C annealing and the trap capture cross-section was estimated about 10⁻¹⁸ cm². From the temperature dependence of the dark current in the temperature range 20 °C–120 °C the conduction mechanism activation energy was found to be about 0.956–0.978 eV. The electrical conductivity depends not only on the sample annealing temperature but also whether the measurement is performed in vacuum or air. The results on the dark conductivity are discussed considering the influence of oxygen atoms and oxygen vacancies. Received: 28 January 1998 / Accepted: 8 January 1999 / Published online: 5 May 1999     

Role of growth temperature and oxygen partial pressure on the structural and electrical properties of pulsed laser deposited La1−xSrxnO3−δ thin films

The paper presents the fabrication and characterization of La_0.65Sr_0.35MnO_3−δ (LSMO) polycrystalline thin films deposited directly on Si (1 0 0) substrates using pulsed laser deposition technique. Various deposition parameters like substrate temperature and oxygen partial pressure have been varied systematically to obtain stoichiometric, crack-free films with smooth surface morphology having nearly monodisperse grain size distribution. The substrate temperature variation from 600 to 800 °C had profound effects on the microstructure and topography of the deposited film, with optimum result being obtained at 700 °C. The variation of partial pressure of oxygen controls the deposition kinetics as well as the stoichiometry of the film in terms of oxygen vacancy, which influences the magnetic and electrical transport properties of the manganate films. The microstructure and crystallinity of the deposited films have been studied using X-ray diffraction, scanning electron microscopy and atomic force microscopy. A correlation between the oxygen stoichiometry and micro-structural and transport properties of the deposited films has been obtained.