Influence of ambient oxygen pressure on the preferred orientation, microstructures, and dielectric properties of (Ba1-xSrx)TiO3 thin films with compositionally graded structures

Compositionally graded (Ba_1-xSr_x)TiO₃ (BST) thin films, with x decreasing from 0.25 to 0.0, were deposited on Pt(111)/Ti/SiO₂/Si(100) substrates by pulsed-laser ablation at 600 °C and under ambient oxygen pressures ranging from 50 to 400 mTorr. The influence of the ambient gas pressure on the preferred orientation, microstructures, and dielectric properties of compositionally graded BST films was investigated by X-ray diffraction, scanning electron microscopy, and dielectric frequency spectra, respectively. As the ambient oxygen pressure was increased, the preferred orientation evolved in the order: (100)+(110)(110)+(111) random orientation, and the surface roughness of the graded BST films also increased. The graded BST films deposited at high ambient oxygen pressures (300400 mTorr) exhibited a grainy structure with polycrystalline grains throughout the film thickness, whereas the graded films deposited at low ambient oxygen pressures (50200 mTorr) possessed a columnar structure. The evolution of the microstructure was ascribed to the different physical and chemical properties of the species that were incident onto the substrates at the various oxygen pressures. The dielectric properties of the graded BST films were dependent upon the ambient oxygen pressures. The graded BST films deposited at 200 mTorr exhibited the highest dielectric constant. PACS 77.55.+f; 77.22.Ch; 81.15.Fg     

Surface plasmon resonance of sputtered Ag films: substrate and mass thickness dependence

The influence of substrate on the tunability of the localized surface plasmon resonance wavelength, _SPR, of silver island films was investigated by magnetron sputtering the films on various substrates. It reveals that increasing refractive index of the substrate, n_sub, not only leads to redshift, but also an extension of the tunable range in _SPR. Such effects can be greatly enhanced by increasing the mass thickness of the metallic islands. The resonance wavelength of an island film can be readily adjusted from the visible to the near infrared region of the electromagnetic spectrum. The sensitivity factor, _SPR/_av, where _av is the interisland dielectric constant, was found to increase approximately linearly with the silver mass thickness up to 4 nm, from 60 nm to about 160 nm per dielectric constant unit. PACS 61.46.+w; 81.07.-b; 36.40.GK     

Effects of thickness on the infrared optical properties of Ba<Subscript>0.9</Subscript>Sr<Subscript>0.1</Subscript>TiO<Subscript>3</Subscript> ferroelectric thin films

Using infrared spectroscopic ellipsometry (IRSE), the optical properties of the Ba_0.9Sr_0.1TiO₃ (BST) ferroelectric thin films with different film thicknesses on Pt/Ti/SiO₂/Si substrates prepared by a modified sol-gel method have been investigated in the 2.5–12.6 m wavelength range. By fitting the measured ellipsometric parameter ( and ) data with a three-phase model (Air/BST/Pt) and the classical dispersion relation for the BST thin films, the optical constants and thicknesses of the thin films have been obtained. The average thickness of the single layer decreases with increasing film thickness. The refractive index of the BST films decreases with increasing thickness in the wavelength range 2.5–11 m, and increases with increasing thickness in the wavelength range 11–12.6 m. However, the extinction coefficient of the BST films monotonously decreases with increasing thickness. It is closely associated with the crystallinity of the thin films, the crystalline size effect and the influence of the interface layer. The absorption coefficient of the BST films with different thicknesses decreases with increasing thickness. PACS 77.55.+f; 78.20.Ci; 78.30.Am; 81.70.Fy; 81.40.Tv     

Investigations of sol–gel-derived highly (100)-oriented Ba0.5Sr0.5TiO3 : MgO composite thin films for phase-shifter applications

Sol–gel deposition of highly oriented Ba_0.5Sr_0.5TiO₃:MgO composite thin films has shown desirable dielectric constant reduction and higher figure of merit for phase-shifter applications. In this multilayer configuration, MgO distributed homogeneously through the Ba_0.5Sr_0.5TiO₃ (BST50) matrix, and it helped in tailoring the dielectric constant and reducing the loss tangent significantly. In the present study, the high-frequency dielectric behavior of the films has been evaluated by fabricating an eight-element coupled microstrip phase shifter and measuring the degree of phase shift and insertion loss as a function of applied voltage at room temperature. An increase in phase-shifter figure of merit (degree of phase shift per dB insertion loss) from 28°/dB for pure BST50 to 71°/dB for a BST50:MgO film (at 14 GHz and 333 kV/cm) has been observed. PACS 77.55.+f; 81.20.Fw; 73.40.-c; 85.50.-n     

Characteristics of Ba xSr 1–xTiO 3 thin films grown by pulsed laser ablation of rotating split targets of BaTiO 3 and SrTiO 3

We have grown heterostructures of Ba_xSr_1-xTiO₃(BST)/La_0.7Sr_0.3MnO₃(LSMO) on LaAlO₃(LAO) substrates by the pulsed laser deposition method. BST films with x=0.2,0.5,0.7 and 0.8 have been prepared using a novel rotating split-target arrangement. The lattice constant of the BST films is found to vary linearly with Ba/Sr ratio. An excellent cube-on-cube epitaxial relationship of (100)_BST||(100)_LSMO||(100)_LAO has also been obtained. Scanning electron microscopy studies have revealed smooth and crack-free BST films with a uniform grain size of about 100 nm. Dielectric measurements, made with patterned Au top electrodes and conducting LSMO bottom layers, have shown a maximum permittivity of approximately 280 at 5 kHz in BST films with x=0.7. P–E loop analyses of the Ba_0.7Sr_0.3TiO₃ and Ba_0.8Sr_0.2TiO₃ films have yielded remnant polarization values of 1.66 and 1.81C/cm², respectively. PACS 81.15Fg; 68.55Jk; 77.55+f     

Growth and characterization of (001)-oriented Pb(Zr0.52Ti0.48)O3/LaNiO3/LaAlO3 heterostructures prepared by pulsed laser deposition

Completely (001)-oriented ferroelectric Pb(Zr_0.52Ti_0.48)O₃/LaNiO₃ heterostructures on single-crystal LaAlO₃(001) substrates have been successfully grown by pulsed laser deposition. X-ray-diffraction analyses (–2 scan, scan and scan) indicate that good out-of-plane orientation and in-plane alignment have been obtained with the epitaxial relationship of PZT(001)//LNO(001)//LAO(001) and PZT001//LNO001//LAO001. Scanning electron and atomic force microscopic images reveal very smooth LNO surfaces with roughness of about 0.4–0.6 nm. Based on a microstructural study of the LNO and PZT films, a layer-by-layer growth mode for the LNO growth is proposed, while island growth is dominant for the PZT films. Secondary ion mass spectroscopy analyses show that no distinct interdiffusion can be found between the PZT and LNO layers. P–E hysteresis loop measurements of the PZT films with LNO as bottom electrodes and Au as top electrodes were carried out at an applied voltage of 5 V. The best remanent polarization P_r and coercive field E_c were found to be 28 C/cm² and 74.5 kV/cm, respectively. PACS 81.15.Fg; 68.55.Jk; 77.22.Ej; 77.84.Bw; 68.65.Ac     

Tailoring of the functional properties of sol–gel films on Pt/TiO2/SiO2/(100)Si substrates: (Pb,La)TiO3/(Pb,Ca)TiO3 multilayer heterostructures

Preferentially oriented sol–gel (Pb,Ca)TiO₃/(Pb,La)TiO₃/(Pb,Ca)TiO₃ and (Pb,La)TiO₃/(Pb,Ca)TiO₃/(Pb,La)TiO₃ multilayer heterostructure thin films deposited on silicon-based substrates have been studied and compared with identically prepared (Pb,La)TiO₃ (PTL) and (Pb,Ca)TiO₃ (PTC) films. The existence in their texture of two components that contribute to the net polarization in the direction normal to the plane of the film, 001 and 111, results in significant ferroelectric and pyroelectric properties. P_r=26 Ccm^-2 and =28.5×10^-9 Ccm^-2K^-1, and P_r=17 Ccm^-2 and =22.8×10^-9 Ccm^-2K^-1, have been achieved, respectively, in the PTL/PTC/PTL and PTC/PTL/PTC heterostructures. The surface roughness of these films provides a high specific surface that can be interesting for infrared detectivity. An increase of the dielectric permittivity in the whole temperature interval up to the transition temperature has been observed for both heterostructures with respect to the PTL and PTC films. This effect is due to a release of stress in the heterostructures that is revealed by the increase of the tetragonal distortion, c/a, of these films. PACS 68.55.Jk; 77.80.-e; 77.84.Dy     

Morphology dependence of the dielectric properties of epitaxial BaTiO3 films and epitaxial BaTiO3/SrTiO3 multilayers

Epitaxial BaTiO₃ films and epitaxial BaTiO₃/SrTiO₃ multilayers were grown by pulsed laser deposition on vicinal surfaces of (001)-oriented Nb-doped SrTiO₃ (SrTiO₃:Nb) single-crystal substrates. Atomic force microscopy was used to investigate the surface topography of the deposited films. The morphology of the films, of the BaTiO₃/SrTiO₃ interfaces, and of the column boundaries was investigated by cross-sectional high-resolution transmission electron microscopy. Measurements of the dielectric properties were performed by comparing BaTiO₃ films and BaTiO₃/SrTiO₃ multilayers of different numbers of individual layers, but equal overall thickness. The dielectric loss saturates for a thickness above 300 nm and linearly decreases with decreasing film thickness below a thickness of 75 nm. At the same thickness of 75 nm, the thickness dependence of the dielectric constant also exhibits a change in the linear slope both for BaTiO₃ films and BaTiO₃/SrTiO₃ multilayers. This behaviour is explained by the change observed in the grain morphology at a thickness of 75 nm. For the thickness dependence of the dielectric constant, two phenomenological models are considered, viz. a series-capacitor model and a dead-layer model. PACS 77.22.-d; 77.22.Ch; 77.55.+f; 77.22.Gm; 77.84.Dy; 81.15.-z ; 81.16.Mk; 81.65.-b; 68.55.-a; 68.37.-d     

Optical properties of thin metallic film/dielectric superlattices constrained by the size effect

The dispersion relation of the 1D Bloch wave vector accompanied with an incident transverse electromagnetic wave on thin metallic film/dielectric superlattices is crucial to its optical properties. The interference of excited longitudinal plasmons between neighbouring metallic films induces a collective oscillation of the whole superlattice causing coupled plasmon polariton waves. A calculation of the optical reflectance manipulated by the size effect on the dielectric constant induces more allowable bands at < as the specularity parameters p and q decrease, meanwhile the cut-off frequency for band rejection also shows a blue shift.     

High quality,high-<Emphasis Type="Italic">k</Emphasis> gate dielectric: amorphous LaAlO<Subscript>3</Subscript> thin films grown on Si(100) without Si interfacial layer

High-k dielectric amorphous LaAlO₃ thin films have been grown on n-type Si(100) substrates by laser molecular beam epitaxy. The interfacial characteristics of the LaAlO₃ films on Si were measured by high-resolution transmission electron micrography and X-ray photoemission spectroscopy. A sharp interface without a silica inter-layer between the LaAlO₃ film and Si substrate was observed. Atomic force microscopy measurements indicated that the root-mean-square surface roughness within a 2m×2m area of the LAO films was 0.12 nm. The flatband voltage and fixed charge density of the 8 nm thickness LaAlO₃ films were about 0.355 V and 1.8×10¹²/cm², respectively. The leakage currents of the LaAlO₃/Si(100) samples with different film thicknesses of 5, 8 and 12 nm were 0.45, 0.23 and 0.05 mA/cm², respectively, at a +1 V dc bias voltage. LaAlO₃ appears to be one of the most promising high dielectric constant materials for use in future ultra large scale integrated devices. PACS 77.55+f; 77.84.Bw; 73.40.Qv     

P-Polarized nonlinear surface polaritons in layered structures

We found an exact solution of Maxwell's equations, which describes the propagation ofp-polarized nonlinear surface polaritons and ofp-polarized nonlinear guided wave polaritons in two cases:i) in a film of a surface active material placed on a substrate described by a diagonal dielectric tensor whose elements depend on the amplitude of the electric field according to _{1 1}=_{2 2}= + (|E ₁|² + |E ₂|²), _{3 3}=, andii) in a film described by the same dielectric tensor (optically uniaxial nonlinear crystal) placed on a substrate with dielectric constant ₃ (optically linear medium). The power carried in the surface waves has also been exactly calculated.     

Synthesis of epitaxial γAl<Subscript>2</Subscript>O<Subscript>3</Subscript> thin films by thermal oxidation of AlN/sapphire(0001) thin films

The synthesis of epitaxial Al₂O₃ films by oxidizing AlN/sapphire(0001) films was investigated in a synchrotron X-ray scattering experiment. Porous Al₂O₃ nucleates on the surface of the AlN film when annealed above 700 °C in oxygen ambient. As the annealing temperature increases above 900 °C, the entire AlN film is oxidized into an epitaxial Al₂O₃ film that has a cubic spinel structure. With increasing oxidation temperature, more oxygen atoms are incorporated into the oxide structure, resulting in denser oxide films with a larger lattice constant. The crystal domain size increases from 50 Å to 210 Å, suggesting that the initial nucleation of the Al₂O₃ crystalline domains is followed by gradual grain growth. PACS 61.10.Eq; 81.65.Mq; 68.55.Jk; 68.35.Ct     

Measurements of optical parameters of antimony trisulphide films

In the course of a systematic investigation of thin absorbing films, the optical constants of antimony trisulphide (Sb₂S₃) films evaporated on glass were determined for a fairly wide range of thicknesses. The measurements were performed at the wavelength of _Na=5893 Å by the ellipsometric method on the one hand and by intensity measurements of reflected and transmitted light on the other. Independently, the film thickness was measured by the Tolansky interference method. In this way it was possible in both cases to determine both the refractive index of the film and the absorption index using a method currently employed with transparent dielectric films: that of the interpolation of tabulated values. The results of measurements revealed a change in both the refractive and the absorption index with film thickness. The ellipsometric and the intensity measurements gave results in very close agreement. The paper is dedicated to the memory of Dr. A. Vaíek, Professor of the J. E. Purkyn University in Brno, who died on November 16, 1966.     

Measurement of the normal thermal diffusivity of a dielectric film by a pulsed photoacoustic method

A method of determining the thermal diffusivity of a thin film of a transparent dielectric in the direction normal to the surface has been developed. It is based on excitation of reflecting dynamic gratings. The effectiveness of the method is checked experimentally with the example of a thermally oxidized submicron SiO₂ film on a silicon substrate. The temperature dependence of in the range 290–420 K is measured. The possibilities of setting up thermal measurements of films tens of nanometers thick and its problems are discussed.Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 71, No. 6, pp. 793–797, November–December, 2004.This revised version was published online in April 2005 with a corrected cover date.     

A comparative microstructural study of compositionally up- and down-graded (Ba,Sr)TiO3 thin films epitaxially grown on (La,Sr)CoO3-covered MgO(100) substrates by pulsed laser deposition

We report a comparative study of the microstructure of compositionally graded (Ba_1-xSr_x)TiO₃ (BST) films with two compositionally graded directions, up and down, with respect to the substrate, which were deposited epitaxially on (La,Sr)CoO₃ (LSCO)-covered MgO(100) single-crystal substrates by pulsed laser deposition. Cross-sectional transmission electron microscopy (TEM) images and electron diffraction show that the graded films grow epitaxially with their (100) plane parallel to the (100) surface of the MgO single-crystal substrate, and with an in-plane orientation relationship of 〈001〉_BST//〈001〉_LSCO//〈001〉_MgO. The crystalline quality and surface morphology of the graded films are closely related to the direction of the compositional gradient built into the graded films. Down-graded films (starting with a BaTiO₃ layer at the film/substrate interface) have a much better crystalline quality and a smoother surface than the up-graded films (starting with a (Ba_0.75Sr_0.25)TiO₃ layer at the film/substrate interface). Obviously, the BaTiO₃ bottom layer in the down-graded film acts not only as a part of the graded film but also as an excellent seeding layer to enhance the crystallization of the subsequent film layers, resulting in a high crystalline quality of the down-graded film and an enhanced dielectric behavior. Planar (high-resolution) TEM images also demonstrate that down-graded films have a larger, and more uniform, grain size than up-graded films, and that the latter contain voids. PACS 81.15.-z; 77.55.+f; 68.37.Lp; 61.14.-x     

Preparation of single-crystal-like MgO films on Si and orientation control of platinum films on MgO/Si

Growth of a Pt/MgO bilayer on Si(100) was investigated by pulsed-laser deposition. The growth modes of both MgO and platinum films are layer-by-layer growth, which were revealed by in situ reflection high energy electron diffraction observations. Two kinds of orientations of platinum films, viz. epitaxially (100) and (111)-oriented platinum films, were obtained on the same MgO(100)/Si(100) substrate only by varying the laser fluence. The effect of laser fluence on the orientation of platinum films is briefly discussed. The platinum films prepared in our experiments are epitaxially grown and exhibit atomic-scale surface flatness. It is believed that the improvement in the quality of platinum films can be attributed to the perfectly single-crystalline quality of the MgO buffer layer, which was further confirmed by the excellent dielectric properties. For a 150 nm thick MgO film, the leakage current density was found to be 10^-7 Acm^-2 with an electric field of 8×10⁵ Vcm^-1 and the relative dielectric constant (_r) was 10.6. PACS 68.55.Jk; 81.15.Fg; 85.50.Gk     

Mosaic Structure of (001)YBa2Cu3O7-δ/(10.2)Al2O3 Epitaxial Films and Millimeter Waveband Properties of Microstrip Resonators

The c-axis single-phase YBa₂Cu₃O_7- films ( = 0-0.15) on sapphire substrates prepared by the laser ablation technique and the band-pass stripline resonators for 34 GHz-range have been investigated. Increasing disorientation of mosaic block structure of YBa₂Cu₃O_7- films is related to increasing surface resistance R_s at 135 GHz-range and decreasing unloaded quality factor Q_o of linear stripline resonators. The linear dependence between the YBa₂Cu₃O_7- film mosaicity (M) and half-width B₁ of 00.13 reflecting component is determined. The reflection spreading is due to microstrains resulted mainly from the coherent adjustment of the YBa₂Cu₃O_7- film lattice to GdBa₂Cu₃O_7- sub-layer and sapphire substrate. Increasing number of the block characterized by a weak radial lattice adjustment () is demonstrated by spreading of 00.13 reflection. It is found out that depends on the Bragg angle of reflection due to inhomogenity of YBa₂Cu₃O_7- mosaic structure, which resulted from the gradual mosaicity decreasing with the depth.     

Field emission from a metal covered with a semiconducting layer: A model calculation

The electron field emission from a metal covered with a thin layer of a semiconductor with electron affinity and dielectric constant is considered. The model takes into account the metal-semiconductor (Schottky) barrier of height _b, the conduction current inside the semiconductor, and the band bending at the semiconductor-vacuum interface due to the external field penetration. For thick films under moderately high electric fields, the metal-semiconductor interface does not influence the emission behaviour whereas for thin films, the interface plays an important role, depending on the barrier heights. In particular, for /_b<^2/3 the I–V characteristics will, for strong fields, be dominated by the field emission process at the interface. In such cases important deviations from Fowler-Nordheim behaviour are found.     

Relationship between low frequency dielectric dispersion and ferroelectric phase transition in pulsed-laser-deposited Bi<Subscript>4-x</Subscript>La<Subscript>x</Subscript>Ti<Subscript>3</Subscript>O<Subscript>12</Subscript> thin film

The frequency and temperature dependence of the complex dielectric constant of Bi_4-xLa_xTi₃O₁₂ (BLT, x=0.9) ferroelectric thin film was studied in the frequency range of 10^-110⁶ Hz and the temperature range of 298673 K. A low frequency dielectric dispersion (LFDD) was found. A model was proposed to account for this observed phenomena. The complex dielectric constant data obtained in the measured frequency and temperature ranges have been found to fit very well to the dielectric dispersion relation: ^*=+i/₀+[B(i)^n-1]/₀. The knee in the log of the electrical conductivity versus the reciprocal temperature curve occurs at T_c. The activation energies associated with charge conduction are E_a,II=0.73 eV below T_c and E_a,I=0.95 eV above T_c. The occurrence of an anomaly in both the n and parameters near T_c indicates a coupling between charge carries and phonons. PACS 77.55.+f; 77.80.-e; 77.22.Jp     

Electrical properties (dc and ac) of vanadium-borate glass

The results of an investigation into the temperature and frequency dependence of the electrical conductivity [dc and ac (10²–10⁵ Hz)] of glass of the composition 35% B₂O₃-15% CaO-20% V₂O₄-30% V₂O₅ (weight %) are discussed. The resistivity of the glass at T=300°K is =1.2·10¹¹ ·cm. The activation energy of the dc conductivity is E=(0.652±0.004) eV and equal to E for ₂ at high temperatures. The temperature-frequency dependences of the polarization component _p, the dielectric loss coefficient, and the permittivity are explained on the basis of the Fröhlich model proposed for uncoupled relaxation oscillators for which the heights of the potential barriers are uniformly distributed in some range of energies.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika. No. 3, pp. 35–38, March, 1981.