M. Yeadon

Optical Properties of GaN Grown on ZnO by Reactive Molecular Beam Epitaxy

High quality wurtzite GaN epilayers have been grown on ZnO(0001) substrates by reactive molecular beam epitaxy. Photoluminescence and reflectivity measurements point to high quality presumably due to the near match of both the crystal lattice parameter and the stacking order between GaN and ZnO. In addition, the good films lack the characteristic yellow photoluminescence band. Any misorientation of the GaN epilayer planes with respect to the ZnO substrate is not detectable with polarized reflectivity. The x-ray double crystal diffraction measurements indicate this misorientation is much smaller than those for GaN epilayers on SiC and Al2O3 .

Microstructure and optical properties of epitaxial GaN on ZnO (0001) grown by reactive molecular beam epitaxy

High quality GaN epilayers have been grown on oxygen and zinc surfaces of ZnO (0001) substrates by reactive molecular beam epitaxy and the effect of the intermediate buffer layer on the structural and optical properties of the GaN films has been investigated. The optical and structural characterization of the GaN epilayers and ZnO substrates were performed using photoluminescence, reflectivity, x-ray double diffraction, atomic force microscopy, and transmission electron microscopy. The optical results indicated that GaN was grown with compressive strain due to the difference in thermal expansion coefficient between GaN and ZnO. The surface roughness has been reduced by using an intermediate low temperature GaN buffer layer. The low temperature photoluminescence spectra of GaN/ZnO epilayers did not reveal any sign of the well-known midgap yellow signal. Linear polarized reflectivity and photoluminescence indicated that GaN epilayer planes were not misoriented with respect to the ZnO substrate planes: this ...

“Contact epitaxy” observed in supported nanoparticles

We have observed the formation of heteroepitaxial interfacial layers between silver nanoparticles and a single crystal copper surface by a phenomenon we term “contact epitaxy.” Upon depositing Ag nanoparticles (5–20 nm diameter) onto clean (001) Cu in an ultrahigh vacuum in situ transmission electron microscope, a thin (111)-oriented layer of Ag was detected at the interface between the substrate and particles. Molecular dynamics simulations reveal that the epitaxial layers form within picoseconds of impact, with rapid alignment arising from mechanical relaxation of the highly stressed interface formed upon initial contact. The simulations also show that multiple grains form in the nanoparticle as a consequence of this relaxation process. The unique structure of the nanoparticles, induced by contact epitaxy, is expected to significantly influence physical properties such as interfacial bonding, diffusion, chemical activity, and electrical transport, as well as forming a nucleus for grain growth and epitax...

Oxygen surface diffusion in three-dimensional Cu2O growth on Cu(001) thin films

By studying the growth of Cu2O islands during the initial oxidation stage of Cu(001) with in situ transmission electron microscopy, it is found that the dominant mechanism for the growth of three-dimensional islands is surface diffusion of oxygen. However, there exists a non-negligible contribution to the metal oxide growth by another mechanism, probably direct impingement of the oxygen atoms on the oxide island. These results demonstrate the importance of surface conditions in oxidation.

In-situ observations of classical grain growth mechanisms during sintering of copper nanoparticles on (001) copper

The sintering of randomly oriented copper nanoparticles in the size range 4–20 nm with a single crystal (001) copper substrate has been studied in real time using a novel in situ ultrahigh vacuum (UHV) transmission electron microscope. The particles were generated in situ using an UHV DC sputtering attachment and deposited directly onto an electron transparent copper foil inside the microscope. We demonstrate that these particles reorient upon heating to assume the same orientation as the substrate by a classical mechanism involving neck growth and grain boundary motion.

Sintering of silver and copper nanoparticles on (001) copper observed by in-situ ultrahigh vacuum transmission electron microscopy

The sintering of copper and silver nanoparticles with single crystal copper substrates has been studied using a novel in-situ ultrahigh vacuum transmission electron microscope (UHV TEM). The system is equipped with a UHV DC sputtering attachment enabling metal nanoparticles to be generated in-situ and transferred directly into the microscope in the gas phase. In both cases, we find the particles to be of initially random orientation on the substrate. Upon annealing, however, the particles reorient and assume the same orientation as the substrate. The process apparently occurs by a mechanism involving sintering and grain growth. In the case of silver on copper, grain growth cannot occur since the metals are immiscible. Our observations show that, upon annealing, the particles wet the substrate surface and form epitaxially oriented islands by surface diffusion and grain boundary migration. The post-anneal islands exhibit the orientation relationship (111)Ag∥001)Cu, [110]Ag∥[110]Cu.

In situ transmission electron microscopy of AlN growth by nitridation of (0001) α-Al2O3

Using a novel ultrahigh vacuum transmission electron microscope (TEM) with in situ reactive molecular beam epitaxy system, we report the successful synthesis of epitaxial AlN on the (0001) sapphire surface upon exposure to ammonia. The substrate, an electron transparent sapphire foil, was annealed in oxygen at high temperature to eliminate damage induced during preparation and to create large atomically flat regions. The sample was then held at 950 °C in flowing ammonia inside the microscope for 2 h during which periodic observations of microstructural development were made. We report direct observation of the formation of epitaxial AlN with the orientation relationship (0001)AlN//(0001)sub, [1010]AlN//[1120]sub and present both TEM and atomic force microscope images of the sample before and after nitridation. The results are consistent with a diffusion-limited reaction model involving transport of oxygen and nitrogen ions through the growing AlN epilayer between the free surface and the unreacted α-Al2O3.

A new surface science in situ transmission and reflection electron microscope

We describe an ultrahigh vacuum instrument for transmission electron microscopy and reflection electron microscopy for the study of surfaces and thin film growth. The focus of previous experiments was on the high spatial resolution (<3 A) generally associated with microscopy, at the cost of controlled growth and characterization. We have taken a different approach. It has been shown that most experiments using diffraction and diffraction contrast imaging can be performed well at poorer resolution (∼20 A), including the imaging of monatomic steps and monolayer coverages. The instrument is designed for best control of growth and vacuum, with sacrifices in optical resolution, which is theoretically ∼2 nm. The instrument is called SHEBA (surface high-energy electron beam apparatus). We can examine a ∼1 cm2 sample in both transmission electron microscopy and reflection electron microscopy, in situ with well-controlled molecular beam epitaxy (MBE) growth capabilities, well characterized vacuum, and surface char...

In-Situ Observation Of Aln Formation During Nitridation Of Sapphire By Ultrahigh Vacuum Transmission Electron Microscopy

Using a novel ultrahigh vacuum transmission electron microscope (UHV TEM) with insitu molecular beam epitaxy capability we have studied the nitridation of (0001) sapphire upon exposure to ammonia. Atomically flat sapphire surfaces for the experiments were obtained by high temperature annealing. Subsequent exposure to ammonia flow at 950°C led to the successful synthesis of epitaxial AIN; the films were characterized in-situ using TEM. Complimentary ex-situ atomic force microscopy (AFM) was also performed in order to characterize the surface morphology before and after nitridation. The experiments indicate that AIN grows by a 3D island growth mechanism. Electron diffraction patterns suggest an abrupt AIN/sapphire interface with no evidence of the formation of Al–O–N compounds. The rate limiting step in the nitridation reaction appears to be the diffusion of nitrogen and oxygen species between the free surface of the growing AIN film and the reaction interface. It is inferred from kinetic measurements that diffusion of these species occurs along the boundaries between coalescing AIN islands.

Novel interactions of supported clusters: contact epitaxy

Abstract The study of clusters of ‘model’ metal systems such as Cu and Ag provide a valuable route to explore critical issues in materials epitaxy. Our investigations have led to observations of novel interactions between supported metal clusters in both homo- and heteroepitaxial configurations. In the experiments, clusters of both Cu and Ag were produced by inert gas condensation and deposited on the clean (001)Cu surface under ultrahigh vacuum. Following deposition, the Cu clusters were observed to be of initially random orientation on the substrate surface, undergoing reorientation upon annealing by a mechanism involving sintering and grain growth. In the case of Ag clusters, the formation of a heteroepitaxial layer between the particle and substrate was observed upon initial contact. The phenomenon, which we call ‘contact epitaxy’, may be understood from molecular dynamics simulations of a ‘soft impact’ between the nanoparticle and substrate which indicate that the ordered layers form within picoseconds of impact. The experiments were performed in an ultrahigh vacuum transmission electron microscope equipped with an in-situ nanoparticle sputtering system.