G. B. Stephenson

In situ, real-time measurement of wing tilt during lateral epitaxial overgrowth of GaN

By performing in situ, real-time x-ray diffraction measurements in the metalorganic chemical-vapor deposition environment, we have directly observed the emergence and evolution of wing tilt that occurs during the lateral overgrowth of GaN from stripes patterned in a SiO2 mask. This was done by repeatedly performing line scans through the 1013 peak in the direction perpendicular to the [1010]GaN stripe direction. The wing tilt developed as soon as the wings started forming, and increased slightly thereafter to reach a value of ∼1.19° after 3600 s of growth. Upon cooldown to room temperature, the tilt increased to ∼1.36°, indicating that thermally induced stresses during cooldown have only a small effect on wing tilt. However, changes in mask density, composition, and stress state during early lateral overgrowth must be considered as possible origins of wing tilt.

Observation of growth modes during metal-organic chemical vapor deposition of GaN

We present real-time surface x-ray scattering measurements during homoepitaxial growth of GaN by metal-organic chemical vapor deposition. We observed intensity oscillations corresponding to the completion of each monolayer during layer-by-layer growth. The growth rate was found to be temperature independent and Ga-transport limited. Transitions between step-flow, layer-by-layer, and three-dimensional growth modes were determined as a function of temperature and growth rate.

Determination of the cubic to hexagonal fraction in GaN nucleation layers using grazing incidence x-ray scattering

Recent electron diffraction and microscopy studies of GaN nucleation layers have shown that faults in the stacking of the close-packed planes result in the coexistence of cubic and hexagonal phases within the layers. Using grazing incidence x-ray scattering, we have quantified the proportion of the cubic and hexagonal phases throughout the nucleation layer. We compare the structure of a 20 nm nucleation layer grown on sapphire by atmospheric pressure metal-organic chemical vapor deposition at 525u2009°C to that of an identical layer heated to 1060u2009°C. The fractions of cubic and hexagonal phases in the layers are determined by a comparison of the scattering data with a Hendricks–Teller model. High temperature exposure results in a decrease of the cubic fraction from 0.56 to 0.17. The good agreement with the Hendricks–Teller model indicates that the positions of the stacking faults are uncorrelated.

Layer-by-layer growth of GaN induced by silicon

We present in situ x-ray scattering studies of surface morphology evolution during metal–organic chemical vapor deposition of GaN. Dosing the GaN(0001) surface with Si is shown to change the growth mode from step-flow to layer-by-layer over a wide temperature range. Annealing of highly doped layers causes Si to segregate to the surface, which also induces layer-by-layer growth.

X-ray scattering evidence for the structural nature of fatigue in epitaxial Pb(Zr, Ti)O3 films

We have probed the microscopic distribution of 180° domains as a function of switching history in 40 nm epitaxial films of Pb(Zr0.30Ti0.70)O3 by analyzing interference effects in the x-ray scattering profiles. These as-grown films exhibit voltage offsets (imprint) in the polarization hysteresis loops, coupled with a strongly preferred polarization direction in the virgin state. Our x-ray results are consistent with models attributing the loss of switchable polarization to the inhibition of the formation of oppositely polarized domains in a unipolar matrix. Using such model epitaxial films, we demonstrate that different microscopic ensembles of domains resulting from, for example, fatigue, may be resolved by this technique.

Transition between the 1×1 and surface structures of GaN in the vapor-phase environment

Abstract Out-of-plane structures of the GaN (0 0 0 1) surface in the metal-organic chemical vapor deposition (MOCVD) environment have been determined using in situ grazing-incidence X-ray scattering. We measured 11 2 l crystal truncation rod intensities at a variety of temperatures and ammonia partial pressures on both sides of the 1×1 to ( 3 ×2 3 ) R 30° surface phase transition. The out-of-plane structure of the ( 3 ×2 3 ) R 30° phase appears to be nearly independent of temperature below the transition, while the structure of the 1×1 phase changes increasingly rapidly as the phase transition is approached from above. A model for the structure of the 1×1 phase with a partially occupied top Ga layer agrees well with the data. The observed temperature dependence is consistent with a simple model of the equilibrium between the vapor phase and the surface coverage of Ga and N. In addition, we present results on the kinetics of reconstruction domain coarsening following a “quench” into the ( 3 ×2 3 ) R 30° phase field.

In situ studies of the effect of silicon on GaN growth modes.

Abstract We present real-time X-ray scattering studies of the influence of silicon on the homoepitaxial growth mode of GaN grown by metal-organic vapor-phase epitaxy. Both annealing of Si-doped GaN and surface dosing of GaN with disilane are shown to change the mode of subsequent growth from step-flow to layer-by-layer. By comparing the growth behavior induced by doped layers which have been annealed to that induced by surface dosing, we extract an approximate diffusion coefficient for Si in GaN of 3.5 ×10 −18 cm 2 / s at 810°C.

IN SITU SYNCHROTRON X-RAY STUDIES OF FERROELECTRIC THIN FILMS

In situ synchrotron X-ray scattering was used to observe both the growth of PbTiO3 films by metal-organic chemical vapour deposition and the behaviour of the ferroelectric phase transition as a function of film thickness. The dependences of growth mode and deposition rate on gas flows and substrate temperature were determined by homoepitaxial growth studies on thick films (>50 nm). These studies facilitated the growth of thin coherently strained PbTiO3 films on SrTiO3 (001) substrates, with thicknesses ranging from 2 to 42 nm. Experiments on the ferroelectric phase transition as a function of film thickness were carried out in these films under controlled mechanical and electrical boundary conditions.

A time-resolved X-ray scattering experiment for the study of phase transitions and crystallization processes in metallic alloys

An experimental setup to perform high-resolution time-resolved X-ray scattering has been commissioned on the side station of beamline 8-ID at the Advanced Photon Source. A Peltier-cooled diode detector array covering an angle range of 20 degrees is mounted on a 4-circle goniometer and is used to temporally resolve X-ray scattering patterns with a resolution up to 10 ms. Metallic ribbon samples can be quickly heated and cooled from temperatures up to 500u200a°C inside a furnace with controllable atmosphere and equipped with a beryllium window. A description of the setup is presented along with actual results showing time-resolved phase transitions and crystallization processes in AlYNi metallic alloys. These results demonstrate the power of this technique to investigate complex crystallization processes as well as the versatility of this time-resolved X-ray scattering spectrometer.