Extended abstract of a paper presented at Microscopy and Microanalysis 2012 in Phoenix, Arizona, USA, July 29 – August 2, 2012.

By using aberration corrected scanning transmission electron microscopy we have found no small scale lateral In composition fluctuations exist in the In0.15Ga0.85N active region of a light emitting diode. Images were acquired at 2% of the electron dose known to create electron beam damage, so the acquired images reflect the intrinsic structure of the InGaN active region. Position averaged convergent beam electron diffraction reveals the local sample thickness where images were acquired is 4.8 nm, eliminating the possibility that the absence of composition variation was observed due to projection through a thick sample. In addition, 2-3 atomic layer steps were observed in the top surface of In0.08Ga0.92N layers and the In0.15Ga0.85N active layers, providing a possible mechanism for lateral carrier confinement.

Epitaixal Ba0.5Sr0.5TiO3 (BST) thin films were grown on SrTiO3 (STO) and DyScO3 substrates by radio-frequency magnetron sputtering system using three-step method which involves a relatively low-temperature (573-773 K) growth of a BST interlayer sandwiched between two BST layers deposited at a high substrate temperature of 1068 K. X-ray diffraction measurement showed different strains on the films with interlayers grown at different temperatures. Post-growth thermal treatment reduced film strain to a great extent (the film strain of a tri-layer film with a 773 K grown interlayer is only -0.001). Comparing with the control films grown at high temperature, three-step technique improved the dielectric properties, especially increased dielectric constant by 60% for BST/STO and 31% for BST/DyScO3, respectively. High dielectric constant of 1631.4 and its tuning of 36.7% were achieved on the BST/STO with an interlayer grown on 773 K.

Extended abstract of a paper presented at Microscopy and Microanalysis 2011 in Nashville, Tennessee, USA, August 7–August 11, 2011.

Epitaxial ZnO layers heavily doped with Ga (GZO) were grown at 400 °C under metaland oxygen-rich conditions in terms of metal-to-reactive oxygen ratio by plasma-assisted molecular beam epitaxy (MBE). Several atomic force microscopy (AFM) techniques were used to characterize the surface morphology and electrical properties of these GZO films in ambient conditions. Local I-V spectra indicate that layers grown under both O-rich and metal-rich conditions are highly resistive until a relatively high voltage sweep (±12 V) is used. After removal of an insulating surface layer, conduction is possible at lower voltages, but eventually the film resistivity increases and it again becomes insulating. In addition to local I-V spectra, local charge injection and subsequent surface potential measurements were used to probe surface charging characteristics. For charge injection experiments, a reverse-bias voltage is applied to the sample while scanning in contact mode with a metallized tip. The resultant change in surface potential due to trapped charge is subsequently observed using scanning Kelvin probe microscopy (SKPM). The layers deposited in a metal-rich environment demonstrate the expected behavior, but the O-rich layers show anomalous negative and positive charging. Finally, surface photovoltage (SPV) measurements using above-bandgap UV illumination were performed. The GZO layers produce SPV values of 0.4 to 0.5 eV, where the films deposited in an O-rich environment have slightly higher SPV values and faster restoration.

We report on a strong effect of p-GaN surface morphology on the growth mode and surface roughness of ZnO:Ga films grown by plasma-assisted molecular-beam epitaxy on p-GaN/c-sapphire templates. A range of ZnO:Ga surface morphologies varying from rough surfaces with well defined three-dimensional islands, capable to enhance light extraction in light-emitting diodes, to rather smooth surfaces with a surface roughness of ~ 2 nm suitable for vertical-cavity lasers can be achieved by controlling the surface morphologies of p-GaN. Optical transmittance measurements revealed high transparency exceeding 90% in the visible spectral range for ZnO:Ga with both types of surface morphology.

Extended abstract of a paper presented at Microscopy and Microanalysis 2010 in Portland, Oregon, USA, August 1 – August 5, 2010.

The evolution of the surface morphology of unintentionally doped and Si-doped GaN samples subjected to photoelectrochemical (PEC) etching in the carrier-limited regime in aqueous KOH is reported. It was found that a nanoporous structure precedes whisker formation in samples in which high densities of whiskers ultimately form. Increasing the light intensity accelerated the rate of change of the surface morphology, but increasing the molarity of the KOH had no effect on the etching. Applying biases to the samples during etching also accelerated or decelerated the rates of change of the surface morphology. Thus, the surface morphology in the carrier-limited regime tends to only depend on parameters of the starting layers, as well as how much etching in total has occurred. The identification of variations in surface morphology at different times during PEC etching of GaN may have utility in that assorted nanopatterning of the GaN surface can be intentionally achieved in a controllable, large-scale, and inexpensive manner.

We studied several photoluminescence (PL) bands in undoped, Li-, Ga-, and N-doped high-quality ZnO bulk crystals and thin films grown by molecular beam epitaxy (MBE). By analyzing PL in a wide range of excitation power densities, sample temperature, and decay time after a laser pulse, we distinguished and analyzed more than 10 broad bands with unique luminescence properties. Among these bands, only the Cu-related green band with a characteristic fine structure and the Li-related orange band were well-studied and reliably identified in the past.

Pb(ZrxTi1−x)O3 (PZT) films were grown by molecular beam epitaxy using hydrogen peroxide as a source of reactive oxygen. Phase composition as well as structural and electrical properties of the films were studied by x-ray diffractometry, scanning and transmission electron microscopy, conductive atomic force microscopy, and electrical (I-V and polarization-field) measurements. The hydrogen peroxide pressure was found to control the phase composition of the films. Excess peroxide leads to PbO inclusions in PZT layers, whereas deficiency results in the TiO2 or the ZrO2 phase. The second-phase inclusions can be responsible for high leakage current in the films. Precise control over the peroxide pressure is imperative for single-phase PZT films with good ferroelectric properties.

In this work, thin layers of poly(methyl methacrylate) (PMMA) on Ni on silicon <111> substrates were etched almost completely away by oxygen RIE, leaving only the topmost portion of the roughness, generating nanodots of PMMA approximately 30-40nm or smaller in size. After sufficiently hard baking the samples to promote PMMA adhesion to the Ni and to increase the robustness of the PMMA, the nanodots were used as a mask to etch the thin Ni films, thus generating Ni nanodots on Si. The Ni nanodots were then used as a reactive ion (RIE) etch mask, thereby generating Si nanopillars. With further understanding of the mechanism of the generation of the roughness of the PMMA, or with the use of other polymeric materials suitable as wet etching masks, nanodots of varying size should be attainable. This method represents a very simple, low cost, scalable, and general technique to produce nanodots of various thin metals on various substrates.

We studied spin-orbit coupling in wurtzite AlxGa1−xN/AlN/GaN heterostructures with different Al concentrations using weak antilocalization measurements at 1.6 K. Using the persistent photoconductivity effect we change the carrier density in controllable manner. We find that the electron spin splitting energies does not scale linearly with the Fermi wavevector at high carrier densities. From this deviation, for the first time, we are able to extract the cubic spin-orbit parameter for this material system.

The dependence of traps and their concentration in GaN on the quality of templates, on which the layers are grown, has been studied by deep-level transient spectroscopy (DLTS). Thin GaN layers studied were grown on GaN templates employing conventional epitaxial lateral overgrowth (ELO) and nano-ELO with SiNx nanonetwork. The concentrations of traps found in these layers were compared with a reference sample grown on a standard GaN template not utilizing ELO. Two traps A (0.55 eV – 0.58 eV) and B (0.20 eV – 0.23 eV) were detected in the temperature range from 80 K to 400 K. A reduction of traps in layers grown on the ELO and nano-ELO templates was noted. We attribute this reduction to the reduction of threading dislocation density and as a result reduced capture of point defects and complexes as part of dislocation core structure and/or reduced formation of defects and complexes in the vicinity of line defects where the formation can be energetically favorable.

Transmission electron microscopy was used to study defects in lateral epitaxial layers of GaN which were overgrown on a template of a-plane (1120) GaN grown on (1102) r-plane Al2O3. A high density of basal stacking faults is formed in these layers because the c-planes of wurtzite structure are arranged along the growth direction. Density of these faults is decreasing at least by two orders of magnitude lower in the wings compared to the seed areas. Prismatic stacking faults and threading dislocations are also observed, but their densities drastically decrease in the wings. The wings grow with opposite polarities and the Ga-wing width is at least 6 times larger than N-wing and coalescence is rather difficult. Some tilt and twist was detected using Large Angle Convergent Beam Electron Diffraction.

We report a two-step growth method to obtain uniformly coalesced epitaxial lateral overgrown a-plane GaN by metalorganic chemical vapor deposition (MOCVD). By obtaining a large wing height to width aspect ratio in the first step followed by enhanced lateral growth in the second step via controlling the growth temperature, we reduced the tilt angle between the advancing Ga-polar and N-polar wings for improved properties. Transmission electron microscopy (TEM) showed that the threading dislocation density in the wing area was 1.0×108cm−2, more than two orders of magnitude lower than that in the window area (4.2×1010cm−2). However, a high density of basal stacking faults, 1.2×104cm−1, was still observed in the wing area. Near field scanning optical microscopy (NSOM) at room temperature revealed that the luminescence was mainly from the wing regions with very little contribution from the windows and meeting fronts. These observations suggest that due to significant reduction of threading dislocations radiative recombination is enhanced in the wings.

The influence of passivation with SiO2 and SiNx on optical properties and surface band bending in unintentionally doped GaN has been studied by steady-state photoluminescence (PL) and surface potential electric force microscopy (SP-EFM). For both types of passivation we observed a significant increase of PL intensity in air ambient at room temperature. The measured surface potential was the same for control and passivated samples within the experimental error. The value of the surface band-bending was determined as 1.0±0.2 eV in all cases. We suggest that the strong enhancement of PL is caused by reduction of contribution of the surface states to recombination of photogenerated carriers after passivation.

A study of screw dislocations in hydride-vapor-phase-epitaxy (HVPE) template and molecular-beam-epitaxy (MBE) overlayers was performed using transmission electron microscopy (TEM) in plan view and in cross section. It was observed that screw dislocations in the HVPE layers were decorated by small voids arranged along the screw axis. However, no voids were observed along screw dislocations in MBE overlayers. This was true both for MBE samples grown under Ga-lean and Ga-rich conditions. Dislocation core structures have been studied in these samples in the plan-view configuration. These experiments were supported by image simulation using the most recent models. A direct reconstruction of the phase and amplitude of the scattered electron wave from a focal series of high-resolution images was applied. It was shown that the core structures of screw dislocations in the studied materials were filled. The filed dislocation cores in an MBE samples were stoichiometric. However, in HVPE materials, single atomic columns show substantial differences in intensities and might indicate the possibility of higher Ga concentration in the core than in the matrix. A much lower intensity of the atomic column at the tip of the void was observed. This might suggest presence of lighter elements, such as oxygen, responsible for their formation.

We studied photoluminescence (PL) from deep-level defects in GaN grown under Garich conditions at relatively low temperatures (700–800°C) by molecular-beam epitaxy (MBE). The dominant features of PL spectrum are red and green bands peaking respectively at ∼1.8 and ∼2.35 eV. Both PL bands decay exponentially at low temperatures (15 – 100 K) after pulsed excitation. The characteristic lifetime for the red band decreases by almost two orders of magnitude from 110 to 2 μs with increasing temperature from 15 to 100 K, while its integrated intensity after each pulse remains nearly unchanged in the same temperature range due to an increase in the peak intensity in the time-resolved PL curve. The lifetime of the green band remained unchanged in this temperature range. We suggest that these PL bands are caused by transitions between excited and ground states of some deep defects rather than transitions involving a shallow donor, conduction or valence bands.

We have conducted a systematic magnetic characterization of a series of Zn1-xCoxO samples with different cobalt composition. The Zn1-xCoxO thin films were epitaxially grown by metal organic chemical vapor deposition (MOCVD) on quartz and ZnO substrates. The Co composition was adjusted by controlling the bubbler temperature and carrier gas flow. The magnetization measurements were performed using a Quantum Design MPMS system, which utilizes a superconducting quantum interference device (SQUID) magnetometer. Magnetic hysteresis curves were observed at 5K which persisted up to 300K, possibly characteristic of ferromagnetic behavior. Temperature dependent magnetization was recorded under both zero-field cooled (ZFC) and field cooled (FC) conditions. Changes of magnetization were observed under ZFC and FC conditions in some samples from 5K up to 300K. Composition-dependent changes in magnetization were also observed among samples with different cobalt doping, indicative of ferromagnetism related directly to cobalt incorporation. Magnetic field dependent magnetization at various temperatures with field up to 5 Tesla suggests the Zn1-xCoxO layers were not paramagnetic.

We report a new defect-related photoluminescence (PL) band peaking at 2.56 eV at 15 K in undoped GaN layers grown by molecular beam epitaxy (MBE) on GaN templates. The maximum of the aquamarine luminescence (AL) band shifts to higher energies by about 100 meV with increasing temperature from 15 to 300 K. In spite of the fact that the shape and the peak position of the AL band are close to the characteristics of the green luminescence band in a freestanding GaN template, we were able to delineate these two bands for their markedly different behavior with temperature and excitation intensity. The origin of defect responsible for this PL band remains unknown.