Optical properties of SrTiO<Subscript>3</Subscript> thin films by pulsed laser deposition

SrTiO₃ thin films were prepared on a fused-quartz substrate by pulsed laser deposition (PLD). Dense and homogeneous films with a thickness of 260 nm were prepared. Optical constants (refractive index n and extinction coefficient k) were determined from the transmittance spectra using the envelope method. The optical band gap energy of the films was found to be 3.58 eV, higher than the 3.22 eV for bulk SrTiO₃, attributable to the film stress exerted by the substrate. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The refractive index and the packing density for the PLD-prepared SrTiO₃ thin films are higher than those for the SrTiO₃ films prepared by physical vapor deposition, sol–gel and RF sputtering. Received: 18 March 2002 / Accepted: 7 October 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: mszhang@nju.edu.cn     

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     

Catalytic growth and characterization of Ga<Subscript>2</Subscript>O<Subscript>3</Subscript> nanowires

β-Ga₂O₃ nanowires have been synthesized using Ga metal and H₂O vapor at 800 °C in the presence of Ni catalyst on the substrate. Remarkable reduction of the diameter and increase of the length of the Ga₂O₃ nanowires are achieved by separation of Ga metal and H₂O vapor before they reach the substrate. Transmission electron microscopy analyses indicate that the β-Ga₂O₃ nanowires possess a single-crystalline structure. Photoluminescence measurements show two broad emission bands centered at 290 nm and 390 nm at room temperature. Received: 27 June 2002 / Accepted: 7 October 2002 / Published online: 17 December 2002 RID="*" ID="*"Corresponding author. Fax: +886-6/234-4496, E-mail: wujj@mail.ncku.edu.tw     

Large optical nonlinearity in CaCu<Subscript>3</Subscript>Ti<Subscript>4</Subscript>O<Subscript>12</Subscript> thin films

CaCu₃Ti₄O₁₂ (CCTO) thin films were successfully prepared on LaAlO₃ substrates by pulsed laser deposition technique. We measured the nonlinear optical susceptibility of the thin films using Z-scan method at a wavelength of 532 nm with pulse durations of 25 ps and 7 ns. The large values of the third-order nonlinear optical susceptibility, χ ⁽³⁾, of the CCTO film were obtained to be 2.79×10⁻⁸ esu and 3.30×10⁻⁶ esu in picosecond and nanosecond time regimes, respectively, which are among the best results of some representative nonlinear optical materials. The origin of optical nonlinearity of CCTO films was discussed. The results indicate that the CCTO films on LaAlO₃ substrates are promising candidate materials for applications in nonlinear optical devices.     

Third-order nonlinear optical response of Au-core CdS-shell composite nanoparticles embedded in BaTiO<Subscript>3</Subscript> thin films

Au-core CdS-shell composite nanoparticles were synthesized by a direct self-assembly process and integrated into BaTiO₃ thin films. Characterization by transmission electron microscopy showed that the average diameter of these composite nanoparticles was about 8 nm. Using the femtosecond time-resolved optical Kerr effect method, we investigated the third-order nonlinear optical response of the Au@CdS nanoparticles embedded in the BaTiO₃ thin films at a wavelength of 800 nm. An ultrafast nonlinear response and a large effective third-order nonlinear susceptibility of χ⁽³⁾=7.7×10^-11 esu were observed. We attributed the enhancement of the third-order optical nonlinearity to a localized electric field effect originating from the core-shell structure under off-surface-plasmon resonance conditions. Received: 13 May 2002 / Revised version: 23 October 2002 / Published online: 3 April 2003 RID="*" ID="*"Corresponding author. Fax: +86-21/6510-4949, E-mail: sxqian@fudan.ac.cn     

Features of the film-growth conditions by cross-beam pulsed-laser deposition

Spatial and energetic characteristics of the plasma plume by cross-beam pulsed-laser deposition (CBPLD) were investigated. Effective droplets filtering together with high efficiency of material usage are observed by this approach. Time-of-flight (TOF) technique with electrostatic ion collectors (Langmuir probes operating in the ion-collecting mode) were applied to obtain kinetic energy distribution functions of ionized particles and to compare the ionization degrees of the plasma by the CBPLD and by the conventional PLD. The average and maximum kinetic energies of the ions by the CBPLD are found to be 2–3 times lower as compared to the conventional PLD. At the same time, the fraction of ionized species and highly exited neutrals (Rydberg atoms) in the CBPLD plasma is 1.5–2 times larger in comparison to the conventional approach. Re-sputtering of the material of the growing film by fast ions is a considerable effect in both the PLD methods by the chosen experimental conditions. The angular width of the directional pattern of the plasma plume by CBPLD is comparable to that typical for the conventional PLD. Received: 21 December 1998 / Accepted: 28 March 1999 / Published online: 7 July 1999     

Pulsed laser deposition of BaGa<Subscript>2</Subscript>O<Subscript>4</Subscript>

This paper reports the first results obtained on monobarium gallate thin films grown on silicon and platinum coated substrates by pulsed laser deposition. The influence of oxygen background pressure and substrate (or post-annealing) temperature on the film properties was studied. The films were characterized by XRD, RHEED, AFM, photoelectron and electrical impedance spectroscopy. The structure analysis showed that the films crystallized into a hexagonal phase, most probably into (metastable) α-BaGa₂O₄. Depending on deposition conditions, films with different (from nearly epitaxial to polycrystalline) textures were obtained.     

Structural and optical properties of Bi<Subscript>3.25</Subscript>La<Subscript>0.75</Subscript>Ti<Subscript>3</Subscript>O<Subscript>12</Subscript> ferroelectric thin films prepared by chemical solution methods

Ferroelectric Bi_3.25La_0.75Ti₃O₁₂ (BLT) thin films have been grown on Pt/Ti/SiO₂/Si substrates by chemical solution methods. X-ray diffraction analysis shows that BLT thin films are polycrystalline with (171)-preferential orientation. Atomic force microscopy investigation shows that they have large grains about 120 nm in size. A Pt/BLT/Pt capacitor has been fabricated and showed excellent ferroelectricity, with a remnant polarization and coercive field of 24 μC/cm² and 116 kV/cm, respectively. The capacitor shows no polarization fatigue up to 10⁹ switching cycles. The optical constants (n,k) of the BLT thin films in the wavelength range 0.35–1.7 μm were obtained by spectroscopic ellipsometry measurements, and the band-gap energy was found to be about 3.25 eV. Received: 16 October 2001 / Accepted: 6 January 2002 / Published online: 3 June 2002 RID="*" ID="*"Corresponding author. Fax: +86-21/65830-734, E-mail: gswang@mail.sitp.ac.cn     

Femtosecond laser pulse filamentation versus optical breakdown in H<Subscript>2</Subscript>O

The competition between femtosecond laser pulse induced optical breakdown and femtosecond laser pulse filamentation in condensed matter is studied both experimentally and numerically using water as an example. The coexistence of filamentation and breakdown is observed under tight focusing conditions. The development of the filamentation process from the creation of a single filament to the formation of many filaments at higher pulse energy is characterized systematically. In addition, strong deflection and modulation of the supercontinuum is observed. They manifest themselves at the beginning of the filamentation process, near the highly disordered plasma created by optical breakdown at the geometrical focus. Received: 9 July 2002 / Revised version: 15 November 2002 / Published online: 19 March 2003 RID="*" ID="*"Corresponding author. Fax: +1-418/6562-623, E-mail: wliu@phy.ulaval.ca     

Deposition and stoichiometry control of Nd-doped gadolinium gallium garnet thin films by combinatorial pulsed laser deposition using two targets of Nd:Gd<Subscript>3</Subscript>Ga<Subscript>5</Subscript>O<Subscript>12</Subscript> and Ga<Subscript>2</Subscript>O<Subscript>3</Subscript>

We have demonstrated pulsed laser deposition of Nd-doped gadolinium gallium garnet on Y₃Al₅O₁₂ by the simultaneous ablation of two separate targets of Nd:Gd₃Ga₅O₁₂ (GGG) and Ga₂O₃. Such an approach is of interest as a method of achieving stoichiometry control over films whilst the growth parameters are kept constant and optimal for high quality crystal growth. We show here how the stoichiometry and resultant lattice parameter of a film can be controlled by changing the relative deposition rates from the two targets. Films have been grown with enough extra Ga to compensate for the deficiency that commonly occurs when depositing only from a GGG target. We have also grown crystalline GGG films with an enriched Ga concentration, and this unconventional approach to film stoichiometry control may have potential applications in the fabrication of films with advanced compositionally graded structures.     

Interface reactions in [Fe/B]<Subscript>n</Subscript> multilayers: a way to tune from crystalline/amorphous layer sequences to homogeneous amorphous Fe<Subscript>x</Subscript>B<Subscript>100-x</Subscript> films

[Fe/B]_{n ≥2} multilayers were prepared by thermal evaporation, ion-beam sputtering and laser ablation. By applying in situ electron spectroscopies (UPS, XPS) and monitoring the electrical resistance during layer growth, evidence could be provided for the occurrence of interface reactions within the range of studied deposition temperatures (77 K ≤T ≤300 K). These reactions result in amorphous Fe_xB_100-x phases, which are spatially restricted to a width of less than 3 nm at the original interface. The amorphicity of the reacted interlayers was unequivocally proven by additional high-resolution electron microscopy (HRTEM) and their characteristically changed magnetic properties. Due to the well-defined width of the interface reaction, homogeneous amorphous Fe_xB_100-x films can be obtained by reducing the individual Fe and B layer thicknesses to below the above reaction depth, while for larger thicknesses layer sequences of the crystalline/amorphous/crystalline type will result. Received: 30 January 2002 / Accepted: 31 January 2002 / Published online: 10 September 2002 RID="*" ID="*"Corresponding author. Fax: +49-731/502-2963, E-mail: hans-gerd.boyen@physik.uni-ulm.de     

Time-resolved spectroscopy measurements of a titanium plasma induced by nanosecond and femtosecond lasers

We have studied the plasma induced at the surface of a titanium target following irradiation with femtosecond and nanosecond laser pulses. Time-resolved imaging and spectroscopic measurements allowed us to evidence some features specific to the femtosecond-laser-induced plasma. In this ultrashort interaction regime, we could discriminate between three different velocity populations in the plasma expansion. Coulomb explosion firstly creates highly energetic Ti⁺ ions, which are followed by atomic neutral titanium and lastly by nanoscale titanium oxide clusters. Received: 28 September 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +33-1/6931-9996, E-mail: albert@ensta.fr     

Anisotropy of the dielectric permittivity of Sn<Subscript>2</Subscript>P<Subscript>2</Subscript>S<Subscript>6</Subscript> measured with light-induced grating techniques

We apply, for the first time to our knowledge, photorefractive grating spectroscopy to obtain not-yet-known data on the anisotropy of the dielectric permittivity of Sn₂P₂S₆. Two independent techniques are used, one based on measurements of the amplitude of the space-charge field grating as a function of grating spacing and the other based on measurements of the grating decay time, also as a function of grating spacing. Both techniques provide close values for the anisotropy, which appears to be well pronounced, a ratio ε_xx/ε_zz≈4 is revealed for two of the three independent components of the dielectric tensor. Our data also allow us to conclude that the charge mobility is nearly isotropic in the same plane, μ_xx/μ_zz≈1. Received: 2 December 2002 / Published online: 26 March 2003 RID="*" ID="*"Corresponding author. Fax: +380-44/265-2359, E-mail: odoulov@iop.kiev.ua     

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     

Pressure effects during pulsed-laser deposition of barium titanate thin films

2 , Ar) in a broad pressure range (10^-7–1 mbar) are correlated to the plasma expansion dynamics. It is found that the deposited films present an excess of Ba in the intermediate pressure range (10^-2<P<10^-1 mbar) and a peaked distribution of Ba to Ti atoms ratio, that is not related to either the substrate temperature or the nature of the gas environment. The results are discussed in terms of the dependence of the plume length (L_P) on the gas pressure and the existence of scattering processes for distances (d) from the target lower than L_P and the diffusion of the ejected species for L_P<d. Received: 7 November 1997/Accepted: 8 November 1997     

Superlinear photovoltaic currents in proton-exchanged LiNbO<Subscript>3</Subscript> waveguides

Photovoltaic currents along the c axis have been measured in α-phase LiNbO₃ proton-exchanged waveguides at several visible wavelengths for a guided-beam configuration. The light-intensity dependence is superlinear and all experimental curves are very well fitted by computer simulations using a two-centre model, with Fe²⁺/Fe³⁺ as primary and Nb_Li ⁴⁺/Nb_Li ⁵⁺ as secondary photovoltaic centres. The superlinear behaviour arises from a much higher effective photovoltaic length of Nb_Li ⁴⁺ (small polaron) compared with that of Fe²⁺. In β₁-phase guides, the photocurrents are much smaller than in α-phase guides and apparently do not show superlinear behaviour. Received: 22 October 2002 / Revised version: 6 January 2003 / Published online: 12 May 2003 RID="*" ID="*"Corresponding author. Fax: +34-91/3978-579, E-mail: m.carrascosa@uam.es     

Preparation of Mn<Subscript>3</Subscript>O<Subscript>4</Subscript> nanowires by calcining the precursor powders synthesized in a novel inverse microemulsion

Manganese oxide (hausmannite) nanowires were prepared by annealing precursor powders at a temperature of 800 °C for 3 h, which were produced in a novel inverse microemulsion (IμE) system. The microstructures of the as-prepared Mn₃O₄ nanowires were investigated by means of X-ray diffraction, transmission electron microscopy, and Raman spectra. It has been found that the Mn₃O₄ nanowires were relatively straight and their surfaces were smooth with a typical diameter of 75–150 nm. The formation mechanism of the Mn₃O₄ nanowires is discussed. Received: 30 May 2002 / Accepted: 7 October 2002 / Published online: 17 December 2002 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: wangqun@nju.edu.cn     

PLD and RF-PLD synthesis of Ba<Subscript>0.6</Subscript>Sr<Subscript>0.4</Subscript>TiO<Subscript>3</Subscript> ferroelectric thin films for electrically controlled devices

Ba_0.6Sr_0.4TiO₃ (BST) bulk ceramic synthesized by solid state reaction was used as target for thin films grown by pulsed laser deposition (PLD) and radiofrequency beam assisted PLD (RF-PLD). The X-ray diffraction patterns indicate that the films exhibit a polycrystalline cubic structure with a distorted unit cell. Scanning Electron Microscopy investigations showed a columnar microstructure with size of spherical grains up to 150 nm. The capacitance–voltage (C–V) characteristics of the BST films were performed by applying a DC voltage up to 5 V. A value of 280 for dielectric constant and 12.5% electrical tunability of the BST capacitor have been measured at room temperature.     

Pressure-controlled preparation of nanocrystalline complex oxides using pulsed-laser ablation at room temperature

Nanocrystalline thin films of complex oxides such as BaTiO₃ and LaFeO₃ were prepared by pulsed laser ablation without substrate heating. Targets under various Ar pressures were irradiated using an ArF excimer laser. The off-axis configuration of targets and substrates was used to synthesize the films. The crystallinity and chemical composition of the deposited films were strongly dependent on the processing Ar gas pressure. In case of BaTiO₃, the film deposited at 10 Pa was a single phase of BaTiO₃ with a crystallite size around 7.2 nm. With increasing Ar pressure to 200 Pa, XRD peaks of BaTiO₃ as well as BaCO₃ were observed. The by-products could be due to reaction with carbon dioxide in air after taking the sample out of the chamber. For LaFeO₃, the films deposited under 50 to 200 Pa had a single phase with a crystallite size below 10 nm. When the Ar pressure exceeded 100 Pa, the crystallite size tended to decrease for both BaTiO₃ and LaFeO₃, which could be due to formation of aggregated nanoparticles. Below 10 Pa, oxygen deficiency was observed. Over 50 Pa, the atomic concentration of all the constituent elements was almost constant, especially the [Ba]/[Ti] and [La]/[Fe] ratios, which were nearly unity. Received: 19 June 2002 / Accepted: 24 June 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +81-298/61-6355, E-mail: yoon-jw@aist.go.jp     

Growth of stoichiometric and textured LiNbO3 films on Si by pulsed laser deposition

Laser ablation of single-crystal LiNbO₃ in a gas environment is used to grow films on (100) Si substrates heated to 650 °C. The film composition and crystallinity are studied as a function of the nature (reactive, O₂, or inert, Ar) and pressure of the gas environment applied during deposition and cooling-down processes, the laser energy density and the target–substrate distance. Experimental results show that a gas pressure close to 1 mbar is required to produce stoichiometric films in either O₂ or Ar. The modification of the laser energy density and the target–substrate distance allows us to improve the crystallinity of the films that become textured along the (006) direction. The influence of the experimental parameters on the film properties is discussed in the frame of the formation of a blast wave, that leads to the focusing of the expanding Li species and thus, to the increase of the Li content in the films. Received: 8 February 2001 / Accepted: 9 February 2001 / Published online: 3 May 2001