F. G. McIntosh

Effect of hydrogen on the indium incorporation in InGaN epitaxial films

The InN percent in metalorganic chemical vapor deposition (MOCVD) and atomic layer epitaxy (ALE) grown InGaN was found to be significantly influenced by the amount of hydrogen flowing into the reactor. The temperature ranges for this study are 710–780 °C for MOCVD, and 650–700 °C for ALE. For a given set of growth conditions, an increase of up to 25% InN in InGaN, as determined by x-ray diffraction, can be achieved by reducing the hydrogen flow from 100 to 0 sccm. Additionally, the hydrogen produced from the decomposition of ammonia does not seem to change the InN percent in the films, indicating that the ammonia decomposition rate is less than 0.1%. The phenomenon of having hydrogen control the indium incorporation was not reported in the growth of any other III–V compound previously studied.

GROWTH AND CHARACTERIZATION OF ALINGAN QUATERNARY ALLOYS

We report on the deposition of AlyInxGa1−x−yN in the (0<y<0.15) and (0<x<0.14) composition range by metalorganic chemical vapor deposition. AlInGaN quaternary alloys offer a lattice‐matched platform for InGaN‐based light emitting heterostructure devices. Epitaxial growth of AlInGaN on (0001) sapphire substrates has been achieved at 750 °C. Alloy composition, lattice constants, and band gaps were obtained by energy dispersive spectroscopy, x‐ray diffraction, and room temperature PL. Band edge emissions dominate the PL spectra of these quaternary films. Preliminary data suggest that the lattice constant of AlInGaN can be deduced from chemical composition using Vegard’s law, indicating solid solution in the grown quaternary films.

HIGH OPTICAL QUALITY ALINGAN BY METALORGANIC CHEMICAL VAPOR DEPOSITION

We report on the metalorganic chemical vapor deposition of the quaternary alloy AlInGaN. We found it desirable to grow quaternary films at temperatures greater than 855 °C in order to suppress deep level emissions in the room-temperature photoluminescence. Details of the conditions necessary to grow In0.1Ga0.9N at 875 °C are presented. Strained and relaxed AlInGaN films were grown with good optical and structural properties for AlN compositions up to 26% and InN content up to 11%. The effects of strain were observed by a difference in the band gap between thin and thick films with the same compositions. The potential impact of the use of quaternary films is discussed regarding strain engineering for the improvement of present device designs.

Growth and characterization of In-based nitride compounds

Abstract Development of In-based nitride compounds is lagging behind the corresponding Al- and Ga-based compounds. Potential problems facing the growth of Inx Ga1 − x N films and their double heterostructures will be outlined. A tentative model which describes the reaction pathways taking place during the growth of these In-based nitride compounds is presented and is used to explain both our ALE and MOCVD results. In addition, growth parameters leading to the achievement of high values of x, reduction of In metal incorporation and improvement of both the structural and optical properties of InGaN, AlGaInN and InN will be discussed. Properties of AlGaN/InGaN/AlGaN and AlGaInN/InGaN/AlGaInN double heterostructures will be presented, with emission wavelengths in the 400–550 nm range.

High quality InGaN films by atomic layer epitaxy

InxGa1−xN single‐crystal films were grown at 600–700 °C by atomic layer epitaxy (ALE). InGaN films with compositions of up to 27% indium were achieved. The full width at half‐maximum (FWHM) of the (0002) InxGa1−xN peak by double crystal x‐ray diffraction (DCXRD) was as small as 6 min, the lowest value reported for this ternary alloy. Strong photoluminescence band edge emission between 360 and 446 nm was observed at room temperature. These low temperature ALE grown films were achieved without the need to use excessive flows of the In organometallic source and thus demonstrate the potential for growth of this ternary alloy over the entire composition range.

OPTICAL MEMORY EFFECT IN GAN EPITAXIAL FILMS

We report on memory effects in the optical properties of GaN and AlN epitaxial-films grown by atmospheric pressure metal organic chemical vapor deposition. After exposing selected areas of particular samples with He–Cd laser light (3.8 eV), we observed a persistent and marked decrease in the near band edge photoluminescence (PL) intensity emitted from these areas. This effect has been observed in epitaxial films that typically have a pyramidlike hillock surface. This ability to modulate PL emission intensity at individual points in these materials can be exploited as a method for optical data storage. A means of erasing information stored using this effect has also been investigated using lower energy (∼2 eV).

Impurity dependence on hydrogen and ammonia flow rates in InGaN bulk films

H, C, and O impurity concentrations in metalorganic chemical vapor deposition grown InGaN were found to be dependent on the hydrogen and NH3 flow rates. By increasing the hydrogen flow rate from 0 to 100 sccm, a decrease of greater than two orders of magnitude in the C and O impurity levels and one order of magnitude in the H impurity level was observed. Increasing the NH3 flow rate from 1 to 5 slm results in a decrease in the C concentration and an increase in the H and O concentrations indicating that high purity NH3 (99.999%) can be a significant source of O contamination. Additional studies show that when the InN percent in the InGaN films increases, the impurity concentrations increase regardless of changes in the growth conditions. The InGaN films were grown from 710 to 780 °C and the impurity concentrations were characterized by secondary ion mass spectrometry.

Epitaxial deposition of GaInN and InN using the rotating susceptor ALE system

The growth of GaInN ternary alloys has been investigated using atomic layer epitaxy. Single crystal films have been deposited at 100 Torr in the 600°C to 700°C temperature range using the rotating susceptor approach. The InN percentage in the deposited films were found to depend on more than just the gas phase In/Ga ratio. In addition to the relative indium to gallium composition of the precursor gases, the indium incorporation was also found to depend on the absolute partial pressures of the reactant gases. The indium incorporation increases with decreasing growth temperatures, and may reach a temperature dependent saturation limit for a given set of growth conditions. Optimization of the ALE growth process has resulted in single crystal films exhibiting band edge room temperature photoluminescence for InN percentages of up to 27% in the GaInN ternary films. In addition, single crystal indium nitride has been grown using the ALE technique at 480°C.

A Model for Indium Incorporation in the Growth of InGaN Films

The development of high quality indium based III-nitride compounds is lagging behind the corresponding aluminum and gallium based compounds. Potential problems confronting the growth of epitaxial and double heterostructure InGaN will be discussed. A mass balance model is presented describing the competing reaction pathways occurring during the growth of indium containing compounds. Atomic layer epitaxy and metalorganic chemical vapor deposition grown InGaN films will be used to explain this model. Also, the growth parameters leading to the attainment of high InN percentages, reduced indium metal formation, and improved structural and optical properties of indium containing nitrides will be discussed.

New Buffer Layers for GaN on Sapphire by Atomic Layer and Molecular Stream Epitaxy

The current approach of depositing a low temperature then annealed AlN or GaN buffer for the growth of GaN on sapphire results in a high dislocation density. These dislocations thread through the GaN layer to the surface. Reducing their density either by growing thicker films or using a strained layer superlattice is ineffective. Two new approaches for AlN/GaN buffer layer growth for GaN on sapphire have been employed: Atomic Layer Epitaxy (ALE) and molecular Stream Epitaxy (MSE). ALE is distinguished by organo-metallic/ammonia separation while MSE is distinguished by cyclic annealing of the growing film. Both ALE and MSE enhance two dimensional growth of single crystal GaN on sapphire. The structural quality of epitaxial GaN grown on these buffer layers was studied by transmission electron microscopy (TEM) and x-ray diffraction (XRD). The initial result for the ALE buffer shows an improved quality GaN film with lower defect densities. The MSE grown buffer layer closely resembles that of conventionally grown MOCVD buffer layers observed by others, with dislocations threading through the GaN epilayer. The effects of these buffer layers on the structural and optical properties of GaN grown on sapphire will be presented.