National Institute Of Materials Physics - Romania

In this paper, we report on the structural, optical, and electrical properties of a wide compositional range of AlxIn1-xN thin layers deposited on glass and polyethylene terephthalate substrates. AlxIn1-xN layers of controlled composition were obtained by a simple reactive magnetron co-sputtering protocol, using a single aluminium target with indium insets, by varying the Al/In target surface area ratio, and the composition of the deposition atmosphere. The relevant physical properties were investigated and discussed. It is shown that the texture of the thin films is dependent on the cation ratio, while the bowing parameters of lattice constants and band gap values are larger than those of epitaxial layers. (C) 2014 AIP Publishing LLC.

The use of amorphous and transparent oxides is a key for the development of new thin film transistors and displays. Recently, indium zinc oxide (IZO) was shown to exhibit high transparency in the visible range, low resistivity, and high mobility. Since the properties and the cost of these films depend on the In/(In + Zn) values, the measurement of this ratio is paramount for future developments and applications. We report on accurate analysis of the elemental composition of IZO thin films synthesized using a Combinatorial Pulsed Laser Deposition technique. The monitoring of the thin films elemental composition by Laser-Induced Breakdown Spectroscopy was chosen in view of further in situ and real-time technological developments and process control during IZO fabrication. Our analytical approach is based on plasma modeling, the recorded spectra being then compared to the spectral radiance computed for plasmas in local thermal equilibrium. The cation fractions measured were compared to values obtained by complementary measurements using energy dispersive X-ray spectroscopy and Rutherford backscattering spectrometry. Spectroscopic ellipsometry assisted the scientific discussion. A good agreement between methods was found, independently of the relative fraction of indium and zinc that varied from about 65 to 90 and 35 to 10 at%, respectively, and the measurement uncertainties associated to each analytical method.

The pyroelectric signal generated by an epitaxial Pb(Zr0.2Ti0.8)O-3 film can be enhanced by continuous illumination with ultraviolet (UV) light. The measured signal increases more than 2 times at low modulation frequencies of the incident infrared (IR) radiation (similar to 10 Hz) and at wavelengths where the short-circuit photocurrent presents the maximum value (similar to 280-300 nm). The tentative explanation is that the changes in polarization induced by the temperature variation under modulated IR illumination are generating a variable internal electric field, able to collect the photogenerated carriers produced under continuous UV illumination leading to an additional signal in phase with the pyroelectric one. This finding could be exploited for designing pyroelectric detectors with enhanced characteristics by combining both UV and IR responses. (C) 2014 AIP Publishing LLC.

The photocatalytic performance of magnetron-sputtered titanium dioxide (TiO2) coatings of different thickness in anatase crystalline structure deposited on aluminium 1050 alloy substrates was investigated using a combination of photo-electrochemistry, methylene blue decomposition, and microscopic and spectroscopic methods, such as high resolution scanning and transmission electron microscopy, atomic force microscopy and ellipsometry. The reaction resistance was measured by AC impedance, while photocurrent measurements were carried out using the zero resistance ammetry (ZRA) method. The results showed that the TiO2 grains grow in dipyramidal columns having a linear increase in surface area with increased coating thickness. The refractive index values indicate also an evolutionary growth. The refractive index values obtained for the thin coatings on aluminium substrate were well below the values reported for monocrystalline anatase. The photocatalytic performance increased with increased coating thickness, though more rapidly over a range of 100-500 nm thickness. The dielectric constant also increased linearly with coating thickness. (C) 2014 Elsevier B.V. All rights reserved.

High density (above 93%) superconducting bulks of MgB2 with addition of hexagonal BN (h-BN) and cubic BN (c-BN) with compositions ((MgB2) + (BN)(x), x = 0.01, 0.03, 0.05) were obtained by ex situ spark plasma sintering. All the investigated samples have the critical temperature T-c = 38.8 K. The variation of the critical current density J(c) with the external magnetic field H for h-BN added sample is almost overlapping the J(c)(H) dependence for the pristine MgB2 sample. On the other hand, J(c) for the samples added with c-BN is larger at high magnetic fields, while the decrease of J(c) at low H is very small. At T = 20 K, a J(c) of 10(2) A cm(-2) is determined for the sample with x(c-BN) = 0.005 at H = 58 kOe, and for the sample with x(c-BN) = 0.01 at 54 kOe. Magnetic relaxation measurements indicate a significant flux pinning enhancement in MgB2 samples added with c-BN. It is proposed that the disorder at the interface caused by the convenient lattice matching relationship between the lateral plane of the MgB2 crystal prism and the face of the c-BN crystal cube is responsible for the observed vortex pinning increase.

Magnetic and electrical properties of the nanostructured ZnO films are affected by the nonrandom distribution of impurities in the film due to segregation at grain boundaries (GBs) or extended defects. However, mapping the nature and distribution of the impurities in the film is not trivial. Here we demonstrate a simple, statistically relevant, and nondestructive procedure of quantitative determination of the paramagnetic impurities segregated at the GBs in nanostructured semiconducting and insulating films. From correlated electron paramagnetic resonance and transmission electron microscopy investigations, we determined the localization of trace amounts of Mn2+ ions, present as native impurities in a ZnO film deposited by magnetron sputtering at room temperature. In the as-deposited ZnO film, the Mn2+ ions were all localized in nanosized pockets of highly disordered ZnO dispersed between nanocrystalline columns. After the samples had been annealed in air at >400 degrees C, the size of the intercrystalline region decreased and the diffusion in GBs was activated, resulting in the localization of a portion of the Mn2+ ions in the peripheral atomic layers of the ZnO columns neighboring the GBs. The proportion of Mn2+ ions still localized at the GBs after annealing at 600 degrees C was 37%. The proposed method for the assessment of the presence and nature of impurities and the quantitative evaluation of their distribution in semiconducting and insulating nanostructures is expected to find direct applications in nanotechnology, in the synthesis and quality assurance of thin films for spintronics and opto- and nanoelectronics.

Relaxor-to-ferroelectric transformations induced by varying electric fields and temperatures are studied experimentally in acube-on-cubetype epitaxial PbSc1/2Nb1/2O3 film grown on La1/2Sr1/2CoO3/MgO(001). Dielectric response, quasi-static and dynamic polarization, and dynamic current-voltage characteristics evidence the absence of spontaneous relaxor-to-ferroelectric transition. The electricfield-induced transformation from a glass-like relaxor state to a new dynamic polar state is detected at low temperatures below 100 K only. The frustration of ferroelectricity is discussed in relation to orientational anisotropy of the dipolar system in the epitaxial (001) film.

The GeTiO2 amorphous films were deposited by magnetron sputtering and subsequently annealed at 400, 550, 600 and 700 degrees C for nanostructuring. The structure of annealed films was investigated by X-ray diffraction and transmission electron microscopy. The transmittance spectra of all annealed GeTiO2 films were measured and simulated by using Bruggeman effective medium approximation considering components of TiO2 anatase, crystalline Ge, GeO2 and voids determined from the structure investigations. The electrical behavior of 400, 600 and 700 degrees C annealed films was studied by measuring current-voltage characteristics. We found that by increasing the annealing temperature the films thickness decreases from 330 nm (as-deposited films) to 290 nm (700 degrees C annealed films). The 400 degrees C annealed films are amorphous, while all the others annealed at higher temperatures are crystallized (X-ray diffraction and transmission electron microscopy). In the 550 and 600 degrees C annealed films we found the (TiGe)O-2 rutile structure which is formed by starting from the GeO2 tetragonal structure with high Ti content. Additionally, these films contain TiO2 anatase structure and cubic Ge nanocrystals. At 700 degrees C annealing temperature, a surface layer of GeO2 tetragonal nanocrystals is formed by Ge diffusion and a part of Ge is lost. The experimental transmittance spectra indicate a broadening of the transparency range by increasing the annealing temperature, and the simulated ones also indicate this behavior with the decrease of Ge content, the experimental and simulated spectra being in good agreement. Also, the increase of annealing temperature produces an increase of electrical conductivity. (C) 2014 Elsevier B.V. All rights reserved.

Voltage and frequency dependent capacitance measurements were performed on epitaxial BaTiO3 and Pb(Zr0.2Ti0.8)O-3 thin films deposited on single crystal SrTiO3 substrates with (001) and (111) orientations. The measured capacitors have common bottom SrRuO3 contact and different metals as top electrodes: SrRuO3, Pt, Cu, Al, and Au. The capacitance-voltage characteristics were used to extract information regarding the density of the free carriers and the linear contribution to the static dielectric constant. The frequency dependent impedance was used to develop a suitable equivalent circuit for the epitaxial ferroelectric capacitors. It was found that the frequency dependence of the imaginary part of the impedance can be well simulated, in all cases, using a circuit composed of Schottky-type capacitance related to electrode interfaces, contact resistance, and the R-C parallel connection related to the ferroelectric volume of the film. Values for the components of the equivalent circuit were obtained by fitting the experimental data with the simulated curves. These were then used to extract quantities such as dielectric constant in the ferroelectric volume, the width of the depletion layers, and the apparent built-in potential. It was found that, although the investigated capacitors are of different ferroelectric materials, grown on substrates with different orientations, and having different metals as top electrodes, the values for the capacitance associated with the Schottky contacts and the apparent built-in potential are not very different. The results suggest a strong influence of ferroelectric polarization on the electrode interface properties in the case of epitaxial ferroelectric films. (C) 2014 AIP Publishing LLC.

In this paper, we analyze the structural distortions observed by transmission electron microscopy in thin epitaxial SrRuO3 layers used as bottom electrodes in multiferroic coatings onto SrTiO3 substrates for future multiferroic devices. Regardless of the nature and architecture of the multilayer oxides deposited on the top of the SrRuO3 thin films, selected area electron diffraction patterns systematically revealed the presence of faint diffraction spots appearing in forbidden positions for the SrRuO3 orthorhombic structure. High-resolution transmission electron microscopy (HRTEM) combined with Geometric Phase Analysis (GPA) evidenced the origin of these forbidden diffraction spots in the presence of structurally disordered nanometric domains in the SrRuO3 bottom layers, resulting from a strain-driven phase transformation. The local high compressive strain (-4% divided by -5%) measured by GPA in the HRTEM images induces a local orthorhombic to monoclinic phase transition by a cooperative rotation of the RuO6 octahedra. A further confirmation of the origin of the forbidden diffraction spots comes from the simulated diffraction patterns obtained from a monoclinic disordered SrRuO3 structure. (C) 2014 AIP Publishing LLC.