D. Zhuang

Growth of Large AlN Single Crystals Along the [0001] Direction

We have demonstrated growth of large AlN single crystals using (0001)-oriented AlN seeds. Boules with a diameter of 15 mm and length up to 12 mm were obtained from 5 mm seeds. Step flow growth was observed on both Al and N-polar surfaces. N-polar face was suitable for growth within a large window of growth parameters while the Al-polar seeds yielded high-quality crystals only at low supersaturation.

Grain Expansion and Subsequent Seeded Growth of AlN Single Crystals

Ongoing efforts of growing large AlN single crystals at NCSU using an induction-heated, high-temperature reactor are based on (1) engineered expansion of single crystalline grains with increasing boule length, as well as (2) the development of a growth process that enables seeded growth on AlN surfaces previously exposed to air. The growth process is based on physical vapor transport (PVT), where AlN powder is sublimed in a high purity nitrogen atmosphere. The growth temperature was typically in the range of 2250 to 2300 °C. In this study, tungsten crucibles were used in combination with graphite insulation and were found to be durable for AlN growth. Boule growth was interrupted several times in order to refill the AlN powder source and the growth surface was subjected to surface preparation to facilitate epitaxial re-growth. Grain expansion was studied as a function of process parameters. Crystalline quality of large single crystalline grains was correlated with their surface morphology.

Structural Characterization of Bulk AlN Single Crystals Grown from Self-Seeding and Seeding by SiC Substrates

Using a combination of synchrotron white beam x-ray topography (SWBXT) and high resolution x-ray diffraction (HRXRD), the structural quality of AlN crystals grown by various sublimation-based techniques have been non-destructively analyzed. Spontaneously nucleated AlN crystals are characterized by very low defect densities but their size is small. Self-seeding results in nucleation of multiple grains of different orientations, a few of which are of good quality while most are highly strained. Using readily available commercial 4H and 6H-SiC substrates, several growth runs have been carried out using different growth conditions to obtain thick AlN layers, either attached to the seed or free-standing. While attached layers are typically cracked and highly strained, crack-free free-standing layers can be obtained by delamination or SiC decomposition. X-ray characterization reveals these crystals have good purity but moderately high defect densities.

Wet Etching of Bulk AlN Crystals

AlN bulk crystals of different crystallographic orientations were etched in aqueous KOH solution (general etchant) and molten KOH/NaOH eutectic alloy (defect selective etchant). In the general etchant, the aluminum polar surface (0001) was found to be stable while the nitrogen polar (000 1 ) surface and non-polar m -plane (10 1 0) surfaces showed significant etching. Etch patterns on nitrogen polar surfaces consisted of complete coverage of hexagonal pyramids while the m -plane surfaces were etched in a layer-by-layer mode. TEM studies revealed that the observed etch hillocks on nitrogen polar surfaces were not associated with extended structural defects. When etched in a defect-selective etchant, the aluminum polar surface showed well-defined hexagonal etch pits, with an etch pit density (EPD) of 2×10 4 cm −2 . The nitrogen polar surfaces and m -plane surfaces showed etch features similar to the one obtained during general etching, however, the etch feature density was significantly lower. The etch mechanisms, etch kinetics, as well as the correlation between the observed etch features and structural defects in bulk crystals will be discussed.

The effect of aluminum nitride-silicon carbide alloy buffer layers on the sublimation growth of aluminum nitride on SiC (0001) substrates

The benefits of depositing AlN-SiC alloy transition layers on SiC substrates before the seeded growth of bulk AlN crystals were determined. The presence of the AlN-SiC alloy layer helped to suppress the SiC decomposition by providing vapor sources of silicon and carbon. It enabled a higher growth temperature, and hence a higher growth rate. In addition, cracks in the final AlN crystals can be decreased because of the intermediate lattice constants and thermal expansion coefficient of AlN-SiC alloy. AlN-SiC alloys were first grown on off-axis SiC substrates by the sublimation-recondensation method. Then pure AlN crystals were grown upon those. For comparison, AlN crystals were directly grown on SiC substrates under similar conditions. X-ray diffraction (XRD) confirmed the formation of a pure single crystalline AlN layer upon the AlN-SiC alloy on SiC substrate. The presence of an AlN-SiC transition layer effectively inhibited the appearance of cracks in the resultant AlN crystals. X-ray topography (XRT) demonstrated that the thick AlN layer effectively released the strain present.