Elizabeth A. Paisley

Generation of localized strain in a thin film piezoelectric to control individual magnetoelectric heterostructures

Experimental results demonstrate the ability of a surface electrode pattern to produce sufficient in-plane strain in a PbZr0.52Ti0.48O3 (PZT) thin film clamped by a Si substrate to control magnetism in a 1000 nm diameter Ni ring. The electrode pattern and the Ni ring/PZT thin film heterostructure were designed using a finite element based micromagnetics code. The magnetoelectric heterostructures were fabricated on the PZT film using e-beam lithography and characterized using magnetic force microscopy. Application of voltage to the electrodes moved one of the “onion” state domain walls. This method enables the development of complex architectures incorporating strain-mediated multiferroic devices.

Surfactant-enabled epitaxy through control of growth mode with chemical boundary conditions

Property coupling at interfaces between active materials is a rich source of functionality, if defect densities are low, interfaces are smooth and the microstructure is featureless. Conventional synthesis techniques generally fail to achieve this when materials have highly dissimilar structure, symmetry and bond type-precisely when the potential for property engineering is most pronounced. Here we present a general synthesis methodology, involving systematic control of the chemical boundary conditions in situ, by which the crystal habit, and thus growth mode, can be actively engineered. In so doing, we establish the capability for layer-by-layer deposition in systems that otherwise default to island formation and grainy morphology. This technique is demonstrated via atomically smooth {111} calcium oxide films on (0001) gallium nitride. The operative surfactant-based mechanism is verified by temperature-dependent predictions from ab initio thermodynamic calculations. Calcium oxide films with smooth morphology exhibit a three order of magnitude enhancement of insulation resistance.

Surfactant assisted growth of MgO films on GaN

Thin epitaxial films of 〈111〉 oriented MgO on [0001]-oriented GaN were grown by molecular beam epitaxy and pulsed laser deposition using the assistance of a vapor phase surfactant. In both cases, surfactant incorporation enabled layer-by-layer growth and a smooth terminal surface by stabilizing the {111} rocksalt facet. Metal-insulator-semiconductor capacitor structures were fabricated on n-type GaN. A comparison of leakage current density for conventional and surfactant-assisted growth reveals a nearly 100× reduction in leakage current density for the surfactant-assisted samples. These data verify numerous predictions regarding the role of H-termination in regulating the habit of rocksalt crystals.

Barrier layer mechanism engineering in calcium copper titanate thin film capacitors through microstructure control

A peak permittivity greater than 10 000 has been achieved for calcium copper titanate (CCT) thin films by engineering a thin film microstructure that maximizes space charge contributions to polarizability. This permittivity is an order of magnitude greater than previous polycrystalline thin film efforts. This unique microstructure control is accomplished using a chemical solution deposition process flow that produces highly dense parallel layers ∼100 nm in thickness. We observe a thickness dependent permittivity where the entire film thickness constitutes the conducting region of a barrier layer capacitor despite the presence of multiple grain boundaries within that thickness. The model predictions are in good agreement with experimental data and are consistent with existing literature reports. These trends in permittivity with dielectric thickness raise new questions regarding the nature of barrier layers in CCT—and specifically, these results suggest that grain boundaries may not always participate as h...

Polarity characterization by anomalous x-ray dispersion of ZnO films and GaN lateral polar structures

We demonstrate the use of anomalous x-ray scattering of constituent cations at their absorption edge, in a conventional Bragg-Brentano diffractometer, to measure absolutely and quantitatively the polar orientation and polarity fraction of unipolar and mixed polar wurtzitic crystals. In one set of experiments, the gradual transition between c+ and c− polarity of epitaxial ZnO films on sapphire as a function of MgO buffer layer thickness is monitored quantitatively, while in a second experiment, we map the polarity of a lateral polar homojunction in GaN. The dispersion measurements are compared with piezoforce microscopy images, and we demonstrate how x-ray dispersion and scanning probe methods can provide complementary information that can discriminate between polarity fractions at a material surface and polarity fractions averaged over the film bulk.

Smooth cubic commensurate oxides on gallium nitride

Smooth, commensurate alloys of ⟨111⟩-oriented Mg0.52Ca0.48O (MCO) thin films are demonstrated on Ga-polar, c+ [0001]-oriented GaN by surfactant-assisted molecular beam epitaxy and pulsed laser deposition. These are unique examples of coherent cubic oxide|nitride interfaces with structural and morphological perfection. Metal-insulator-semiconductor capacitor structures were fabricated on n-type GaN. A comparison of leakage current density for conventional and surfactant-assisted growth reveals a nearly 100× reduction in leakage current density for the surfactant-assisted samples. HAADF-STEM images of the MCO|GaN interface show commensurate alignment of atomic planes with minimal defects due to lattice mismatch. STEM and DFT calculations show that GaN c/2 steps create incoherent boundaries in MCO over layers which manifest as two in-plane rotations and determine consequently the density of structural defects in otherwise coherent MCO. This new understanding of interfacial steps between HCP and FCC crystals ...

Epitaxial PbxZr1−xTiO3 on GaN

Epitaxial integration of PbxZr1−xTiO3 (PZT) (111) with GaN (0002) presents the possibility of polarity coupling across a functional-oxide/nitride heteropolar interface. This work describes the synthesis and characterization of such thin film heterostructures by magnetron sputtering, with specific attention given to process optimization. Using x-ray diffraction and electrical characterization, the growth of epitaxial PZT (∼250 nm) on GaN and PZT on MgO/GaN stacks was verified. A two-stage growth process was developed for epitaxial PZT with a deposition temperature of 300 °C and an ex-situ anneal at 650 °C, which was effective in mitigating interfacial reactions and promoting phase-pure perovskite growth. Electrical analysis of interdigital capacitors revealed a nonlinear and hysteretic dielectric response consistent with ferroelectric PZT. Piezoresponse force microscopy (PFM) characterization shows clear evidence of ferroelectric switching, and PFM hysteresis loop analysis shows minimal evidence for direct...

Critical examination of growth rate for magnesium oxide (MgO) thin films deposited by molecular beam epitaxy with a molecular oxygen flux

The authors report a study of molecular beam deposition of MgO films on amorphous SiO 2 and (0001) GaN surfaces over a large range of temperatures (25–400 °C) and molecular oxygen growth pressures (10 −7 –10 −4 Torr). This study provides insight into the growth behavior of an oxide with volatile metal constituents. Unlike other materials containing volatile constituents (e.g., GaAs, PbTiO 3 ), all components of MgO become volatile at normal epitaxial growth temperatures (≥250 °C). Consequently, defining which species is the adsorption controller becomes ambiguous. Different growth regimes are delineated by the critical substrate temperature for Mg re-evaporation and the Mg:O flux ratio. These regimes have impact on phase purity, quartz crystal microbalance calibration, and film microstructure. The universal decay in deposition rate above growth 10 −5 Torr O 2 is also considered. By introducing a third flux of inert argon gas, rate reduction is attributed to increased molecular scattering and not oxidation of the metal source.

Spectroscopic investigations of band offsets of MgO|AlxGa1-xN epitaxial heterostructures with varying AlN content

Epitaxial (111) MgO films were prepared on (0001) AlxGa1−xN via molecular-beam epitaxy for x = 0 to x = 0.67. Valence band offsets of MgO to AlxGa1−xN were measured using X-ray photoelectron spectroscopy as 1.65 ± 0.07 eV, 1.36 ± 0.05 eV, and 1.05 ± 0.09 eV for x = 0, 0.28, and 0.67, respectively. This yielded conduction band offsets of 2.75 eV, 2.39 eV, and 1.63 eV for x = 0, 0.28, and 0.67, respectively. All band offsets measured between MgO and AlxGa1−xN provide a > 1 eV barrier height to the semiconductor.

Effect of microstructure on irradiated ferroelectric thin films

This work investigates the role of microstructure on radiation-induced changes to the functional response of ferroelectric thin films. Chemical solution-deposited lead zirconate titanate thin films with columnar and equiaxed grain morphologies are exposed to a range of gamma radiation doses up to 10 Mrad and the resulting trends in functional response degradation are quantified using a previously developed phenomenological model. The observed trends of global degradation as well as local rates of defect saturation suggest strong coupling between ferroelectric thin film microstructure and material radiation hardness. Radiation-induced degradation of domain wall motion is thought to be the major contributor to the reduction in ferroelectric response. Lower rates of defect saturation are noted in samples with columnar grains, due to increased grain boundary density offering more sites to act as defect sinks, thus reducing the interaction of defects with functional material volume within the grain interior. R...