We synthesized BiFe1-xMnxO3 (BFMO) for various compositions by sol gel process and thin films were deposited by spin coating on platinum Pt/Ti/SiO2/Si substrates. X-ray diffraction shows all the diffraction planes corresponding to rhombohedrally distorted perovskite BiFeO3 structure. The absence of any impurity phase in the films suggests the incorporation Mn ion preferentially to Fe site in the structure for low concentration. Magnetic measurements reveal the formation of ferromagnetic phase at room temperature with increased Mn substitution. On the other hand, ferroelectric polarization decreases with increasing Mn ion concentration. Raman studies suggest the dopant induced structural distortion.

Microstructures of BiFeO3 (BFO) thin films epitaxially grown on SrRuO3 (SRO) buffered SrTiO3 (STO) (001) substrates by laser molecular beam epitaxy were investigated by means of transmission electron microscopy (TEM). The results showed that the films grown under the oxygen pressures of 1Pa and 0.3Pa, respectively, contain parasitic phase embedded in the BFO phase. The parasitic phase was revealed to be poor in Bi and rich in Fe by high-angle annular dark-field (HAADF) imaging and energy dispersive X-ray spectroscopy (EDS) compositional analysis. In combination with selected area electron diffraction patterns, the parasitic phase was determined to be α-Fe2O3. By lowering oxygen pressure, the density and the size of α-Fe2O3 phase increases whereas the regularity decreases. High resolution TEM images showed that approximately periodic misfit dislocations exist at the interface between the α-Fe2O3 phase and the BFO matrix, indicating that the α-Fe2O3 particles are semi-coherently embedded in the BFO films. Less misfit dislocations were detected at the interfaces between the BFO films and the SRO/STO substrates, implying that the misfit strains in the films may be fully relaxed by the formation of α-Fe2O3 phase.

Barium strontium titanate solidly mounted resonators (SMR) were fabricated with three different acoustic Bragg reflectors (ABR) on a sapphire substrate. The three devices had ABR structures consisting of W/SiO2/W/SiO2, Mo/SiO2/Mo/SiO2, and Pt/SiO2/Pt/SiO2 respectively. The s-parameters of all three devices were measured. The results showed that the quality factor increased as a function of the material in the ABR structure. The quality factor for the devices with tungsten, molybdenum and platinum in the ABR structures are 101, 88, and 31, respectively. This investigation showed how the material in the ABR structure can contribute to the acoustic loss in the device.

Asymmetric superlattices (SLs) with ferromagnetic La0.7Sr0.3MnO3 (LSMO) and ferroelectric Ba0.7Sr0.3TiO3 (BST) as constitutive layers were fabricated on conducting LaNiO3 (LNO) coated (001) oriented MgO substrates using pulsed laser deposition (PLD). The crystallinity, ferroelectric and magnetic properties of the SLs were studied over a wide range of temperatures and frequencies. The structure exhibited ferromagnetic behavior at 300K, and ferroelectric behavior over a range of temperatures between 100K and 300K. The dielectric response as a function of frequency obeys normal behavior below 300 K, whereas it follows Maxwell–Wagner model at elevated temperatures. The effect of ferromagnetic LSMO layers on ferroelectric properties of the SL indicated strong influence of the interfaces. The asymmetric behavior of ferroelectric loop and the capacitance-voltage relationship suggest development of a built field in the SLs due to high strain across the interfaces.

In this study, we have developed ferroelectric data storage test systems based on scanning nonlinear dielectric microscopy (SNDM) to conduct various experiments concerning read/write capability. Nanodomain formation on ferroelectric recording media was studied using the data storage test system. A nanodomain dot array was successfully written on a single-crystal LiTaO3 recording medium. The diameter of the written dot was as small as 7 nm. Epitaxial-thin-film LiTaO3 recording media were also developed. Nanodomain dots with the diameter of 25 nm were written on the thin-film recording medium. In addition, a non-contact probe-height control technique was adopted to solve the problem of tip abrasion using higher-order nonlinear dielectric response detection method. Finally, a hard-disk-drive (HDD)-type ferroelectric data storage test system was developed for conducting read/write tests under conditions close to those of actual operation. Capabilities of reading at the bit rate of 2 Mbps and writing at the bit rate of 20 Mbps were confirmed using the HDD-type data storage test system.

We studied the nucleation and crystallization of sol-gel derived (Ba0.7Sr0.3)TiO3 [BST(70/30)] thin films at low temperatures between 500 to 600°C on Pt(111)/TiO2/SiO2/Si substrates by a process using a combination of 2-ethyl-hexanoate based solutions and modified film preparation. We found that BST films could be crystallized at 500°C and that the films obtained had a columnar-like grainy microstructure with favorable electrical characteristic such as high relative permittivity (ɛr) of 310 at 10 kHz and high tunability of 51% at a bias electric field of 250 kV/cm. Moreover, we investigated annealing temperature dependence of BST(70/30) thin films. The results indicated er and tunability increased with annealing temperature up to 450 and 58%, respectively.

The structural response of a ferroelectric BaTiO3/dielectric CaTiO3 superlattice to the bipolar applied electric field was studied using time-resolved x-ray microdiffraction. Structural results were compared to the polarization-electric field hysteresis curve obtained from electrical measurements. The superlattice x-ray reflections were found to have a broad distribution of intensity in reciprocal space under applied electric fields exceeding the nominal coercive electric field. The broad distribution of the lattice constant at high electric fields is compared with a model in which the constituent layers of the superlattice have different coercive fields for the polarization switching.

We deposited BiFeO3 (BFO) thin films on SrRuO3 (SRO)/Pt bottom electrodes by radio-frequency (RF) sputtering. Some samples were formed at the substrate temperature of 550 °C, and others were foremed at 450 °C and post-annealed at 650°C for crystallization. The coercive field in the post-annealed BFO film was smaller than that in the 550°C-deposited BFO film. The coercive field in Mn-doped BiFeO3 (BFMO) films which were deposited at 550 ˚C on SRO/Pt(111) was lower than that in undoped BFO films. Degradation of the remanent polarization was less significant in the post-annealed BFO film.

TbMnO3 is a multiferroic magnetoelectric material known to simultaneously exhibit antiferromagnetism below 40K and ferroelectricity below 28K in the same crystalline phase [1]. Following interesting results of Cu substitution in LaMn1-yCuyO3 [2, 3], we report a study of TbMn1-x CuxO3 (0 < x < 0.15). We describe here our results of crystal structure refinement, together with measurements of magnetic and dielectric properties in the temperature range 2 - 320 K, and magnetic field 0 - 9 T. We find no major changes in structure or symmetry upon substitution of Cu up to x = 0.15 in TbMn1-x CuxO3. Unlike LaMn1-yCuyO3, which exhibits ferromagnetism with very low values of y, we observe antiferromagnetism at x = 0.15. Our study of dielectric properties as a function of temperature suggests increased lossy behavior upon substitution of Cu at the Mn site. In our temperature dependent studies of tan δ at 1 kHz, we observe a well-defined step-like feature near 120K in both pure and substituted samples, possibly ascribable to a change in carrier mobility, or a dielectric-relaxation process mediated by ordered oxygen vacancies [4, 5], which we will continue to study.

The magnetic flux density inside a Metglas sheet is much higher than that of the applied external magnetic field due to its high magnetic permeability, which is known as the magnetic flux concentration effect. Magnetic flux concentration of Metglas as a function of its sheet aspect ratio (width/length) was investigated for Metglas/Polyvinylidene fluoride (PVDF) laminar composites. Both the simulations and experimental results suggest that the magnetic flux concentration effect is markedly enhanced when the aspect ratio of a Metglas sheet is reduced. Consequently the magnetostriction of Metglas and the magnetoelectric (ME) voltage coefficients of the laminar composites are enhanced. The ME voltage coefficient for a laminar composite with a 1 mm wide and 30 mm long Metglas sheet (25 μm thick) is 21.46 V/cm•Oe, which is much higher than those reported earlier in similar laminar composites without making use of the flux concentration effect. The results demonstrate an effective means to significantly enhance the sensitivity of the magnetostrictive/piezoelectric composites as weak magnetic field sensors.

The field-induced phase transition driven by electric field was observed in poly(vinylidene fluoride – hexafluoropropylene) (P(VDF-HFP)) 90/10 wt% copolymers. Experimental results indicated that the electric field may remarkably affect the remanent polarization in terms of changing the D-E loop forms from double loops to single loop, starting from 68 MV/m, and completing at 216 MV/m. It was found that the remanent polarization as well as the piezoelectric constant d31 had a linear relationship with the poling electric field in above electric field range. Thus the magnetoelectric (ME) coupling coefficient ME in P(VDF-HFP)/Metglas laminates increased with the poling electric field. Moreover, the cyclic poled ME device demonstrated different peak d.c. magnetic bias field HDC on the ME - HDC curves from conventional room temperature poled ones. The peak ME coefficient obtained was 4 V/cm Oe.

The high temperature phases of BiFeO3 have courted much controversy with many conflicting structural models reported, in particular for the paraelectric β-phase. High temperature powder neutron diffraction (PND) experiments indicate that the ferroelectric (R3c) α-phase transforms to the paraelectric β-phase at approximately 820 °C via a first order phase transition. We demonstrate that this phase is unambiguously orthorhombic, adopting the GdFeO3 structure-type with a space group Pbnm. On further heating BiFeO3 undergoes another first order phase transition (β-γ) at approximately 930 °C which is marked by a discontinuous decrease in cell volume consistent with an insulator-metal transition. Close inspection of the PND data show no evidence of any symmetry change, with the postulated γ-phase remaining orthorhombic Pbnm. In addition we present PND and impedance spectroscopy data for BiFeO3 which suggest that the so-called ‘Połomska’ transition observed by some authors at approximately 185 °C is not intrinsic.

Two fundamentally different types of domains were resolved in multiferroic MnWO4 by optical second harmonic generation (SHG). Hybrid-multiferroic (absolute) domains reflect the magnetic chirality coupled 1:1 to the spontaneous polarization because of the magnetic origin of the ferroelectric order. Magnetic translation (relative) domains reflect discontinuities in the progression of the magnetic spin spiral. SHG topography is the only experimental method so far allowing one to image both types of domains. The imaging procedure and the SHG contributions involved are therefore discussed in detail.

We report evidence of enhancement in ferroelectricity in thin films of vanadium (V) doped ZnO grown at higher oxygen pressure. This process reduces oxygen deficiency and the material becomes very insulating, which in turn lowers the leakage current through the ferroelectric capacitor. 2 at. % V doped ZnO films, with thickness of approximately 1 μm were grown epitaxially on c-cut sapphire (Al2O3) (0001) at a growth temperature of 600°C. X-ray analysis showed the layers to be epitaxial where the (0002) diffraction peak had a rocking curve FWHM below 1°. The films with higher oxygen pressure were more insulating than the one grown with lower oxygen pressure. The saturation polarization doubled when the growth pressure increased from 300 mT to 500 mT. Time gated ICCD imaging of the ablated plasma during various O2 pressures and how it translated to the film quality are presented.

One-axis oriented bismuth layer-structured dielectric (BLSD) films were designed using perovskite buffer layers for assembling the crystal orientation and the dielectric properties of the BLSD crystals on silicon wafer. The BLSD crystals with the general formula of (Bi2O2)2+-(Am-1BmO3m+1)2- possess excellent dielectric permittivity with lower size effect and temperature coefficient of capacitance (TCC), as well as high electrical resistivity along to the c-axis direction. These phenomena would contribute for constructing high performance dielectric devices driven under harsh environment, e.g., at high-temperature condition above 100°C. In this study, thin films of CaBi4Ti4O15 and SrBi4Ti4O15, kinds of BLSD compounds with the number of BO6 octahedra in pseudo-perovskite blocks, m, = 4, were prepared by chemical solution deposition (CSD) technique on (100)LaNiO3/(111)Pt/TiO2/(100)Si and (100)SrRuO3// (100)LaNiO3/(111)Pt/TiO2/(100)Si substrates. These films consisted of crystalline phase of BLSD crystal with preferential crystal orientation of (001) plane normal to the substrate surface. Anisotropic crystal growth of BLSD occurred by the lattice matching between pseudo-perovskite blocks in BLSD crystal and (100)LaNiO3 or (100)SrRuO3 plane with perovskite structure. The dielectric constants (εr) of (001)-plane oriented CaBi4Ti4O15 and SrBi4Ti4O15 films were approximately 250-350 at room temperature. The r values of the CaBi4Ti4O15 and SrBi4Ti4O15 films increased slightly with ambient temperature. The TCCs at a temperature range from 25 to 200°C were approximately +103 - +514 ppm/K respectively, which were significantly different from those of (Ba,Sr)TiO3 thin films and would satisfy the performance requirement for driving at high-temperature condition.

The nano-scale strain fields analysis around 90° domains and misfit dislocations in PbTiO3/SrTiO3 001 epitaxial thin film has been conducted using the geometric phase analysis (GPA) combined with high angle annular dark field - scanning transmission electron microscopy (HAADF-STEM). The films typically possess a-c mixed domain configuration with misfit dislocations. The PbTiO3 layer was formed from the two layer: the upper 200 nm layer shows the typical a- and c- mixed domain configuration where the a-domains are several tens nm in width; the bottom 100 nm layer shows the different domain configuration that the width is several nm. In the latter case, a-domains are terminated within the film and are short in length. On the other hand, the bottom of a-domains does not contact the film/substrate interface. It keeps away from the interface, and there is completely c-domain layer under a-domains. The HAADF-STEM-GPA shows that the strain fields around an a-domain and a misfit dislocation interact each other: the tensile strain field and lattice plane bending fit together. This result indicates that the a-domain originates from the misfit dislocation.

We have investigated the Pb depletion in laser ablated PZT (PbZr0.52Ti0.48O3) films through a systematic study of PZT target-laser interactions for both single laser and dual-laser ablation methods. The study includes films deposited from a stoichiometric and an excess PbO PZT targets. The films were deposited on single crystal SrTiO3[100] substrates at 550˚C with a background oxygen pressure of 500 mT. Single laser deposited films at a laser fluence of 5J/cm2 produced the highest Pb content while dual-laser ablated films where an excimer and a CO2 pulsed lasers were synchronized for ablation produced high Pb content for an excimer laser fluence of less than 2J/cm2. This enabled the growth of particulate-free PZT films with high Pb content. ICCD imaging of the plasma plumes showed variations in the expansion profiles at different laser fluencies that correlated well with the Pb content observed in the deposited films.

Ferroelectric film-on-foil capacitors hold special promise to replace discrete passive components in the development of electronic devices that require greater performance and smaller size. We have grown ferroelectric Pb0.92La0.08Zr0.52Ti0.48O3 (PLZT) films on nickel substrates by chemical solution deposition. The dielectric properties were determined for samples of ≈1.15-μm-thick PLZT film grown on LaNiO3-buffered nickel substrates. Measurements on these samples yielded a dielectric constant of ≈1300, dielectric loss (tan δ) of ≈0.05, and leakage current density of ≈7 × 10-9 A/cm2. An energy density of ≈74 J/cm3 was measured at room temperature with 250-μm-diameter capacitors. Highly accelerated lifetime tests were conducted at 100°C to determine the reliability of the ≈1.15-μm-thick film-on-foil capacitors under field stress conditions (with applied electric field from 8.7 × 105 V/cm to 1.3 × 106 V/cm). The breakdown behavior of the PLZT film-on-foil capacitors was evaluated by Weibull analysis. A voltage acceleration factor of ≈-6.3 was obtained. From the test results, a mean time to failure of >3000 hr was projected for capacitors operated at 100°C with ≈2.6 × 105 V/cm dc electric field.

We have investigated relationships between leakage current and microstructure or domain structure of BiFeO3 (BFO) thin films, and leakage current mappings of BFO thin films have been performed by current sensitive AFM. 350-nm-thick and 250-nm-thick BFO thin films were prepared on Pt/TiO2/SiO2/Si substrate by pulsed laser deposition (PLD) and chemical solution deposition (CSD), respectively. Average grain size of PLD-BFO thin film is about 480 nm, which is the same as the film thickness. From the leakage current mapping at a bias voltage of -16 Vdc, leakage current of the BFO thin film flows through not only grain boundary but also the grain itself. On the other hand, CSD-BFO thin film shows rosette structure and small size grains. From the leakage current mapping at a bias voltage of -10 Vdc, leakage current flows along boundaries of the rosette structures. These results indicate that leakage current of BFO strongly depends on its microstructure.

Highly oriented and epitaxial bilayers of PbZr0.52Ti0.48O3/La0.67Sr0.33MnO3 (PZT/LSMO) thin films have been grown by pulsed laser deposition on two different substrates (100) - MgO and -LaAlO3 (LAO) respectively. The structural analysis using X-ray diffraction (XRD) evidenced that layered structure was formed without any secondary phase. Atomic force microscopy (AFM) images shown change in the grain size and surface roughness with change of the substrate. Room temperature magnetization-field (M-H) exhibited well-shaped magnetization hysteresis loops, good saturation and low coercivity. The electrical properties of hetrostructure exhibited high remnant polarization (30-54 μC/cm2) and dielectric constant (400-1700) depending upon the different substrate and temperature deposition of FM layer. Frequency dependent change in dielectric constant and loss were observed above metallic ferromagnet to insulator paramagnet transition temperature. It is important to note that the frequency dependent dielectric anomalies are attributed to the change in metallic nature of LSMO bottom electrode and also the bilayer.