Common issues in the hetero-epitaxial seeding on SiC substrates in the sublimation growth of AlN crystals

Aluminium nitride (AlN) is a futuristic material for efficient next-generation high-power electronic and optoelectronic applications. Sublimation growth of AlN single crystals with hetero-epitaxial approach using silicon carbide substrates is one of the two prominent approaches emerged, since the pioneering crystal growth work from 1970s. Many groups working on this hetero-epitaxial seeding have abandoned AlN growth altogether due to lot of persistently encountered problems. In this article, we focus on most of the common problems encountered in this process such as macro- and micro-hole defects, cracks, 3D-nucleation, high dislocation density, and incorporation of unintentional impurity elements due to chemical decomposition of the substrate at very high temperatures. Possible ways to successfully solve some of these issues have been discussed. Other few remaining challenges, namely low-angle grain boundaries and deep UV optical absorption, are also presented in the later part of this work. Particular attention has been devoted in this work on the coloration of the crystals with respect to chemical composition. Wet chemical etching gives etch pit density (EPD) values in the order of 105 cm-2 for yellow-coloured samples, while greenish coloration deteriorates the structural properties with EPD values of at least one order more.

Critical View on Buffer Layer Formation and Monolayer Graphene Properties in High-Temperature Sublimation

In this work we have critically reviewed the processes in high-temperature sublimation growth of graphene in Ar atmosphere using closed graphite crucible. Special focus is put on buffer layer formation and free charge carrier properties of monolayer graphene and quasi-freestanding monolayer graphene on 4H–SiC. We show that by introducing Ar at higher temperatures, TAr, one can shift the formation of the buffer layer to higher temperatures for both n-type and semi-insulating substrates. A scenario explaining the observed suppressed formation of buffer layer at higher TAr is proposed and discussed. Increased TAr is also shown to reduce the sp3 hybridization content and defect densities in the buffer layer on n-type conductive substrates. Growth on semi-insulating substrates results in ordered buffer layer with significantly improved structural properties, for which TAr plays only a minor role. The free charge density and mobility parameters of monolayer graphene and quasi-freestanding monolayer graphene with different TAr and different environmental treatment conditions are determined by contactless terahertz optical Hall effect. An efficient annealing of donors on and near the SiC surface is suggested to take place for intrinsic monolayer graphene grown at 2000 ∘C, and which is found to be independent of TAr. Higher TAr leads to higher free charge carrier mobility parameters in both intrinsically n-type and ambient p-type doped monolayer graphene. TAr is also found to have a profound effect on the free hole parameters of quasi-freestanding monolayer graphene. These findings are discussed in view of interface and buffer layer properties in order to construct a comprehensive picture of high-temperature sublimation growth and provide guidance for growth parameters optimization depending on the targeted graphene application.

Critical View on Buffer Layer Formation and Monolayer Graphene Properties in High-Temperature Sublimation

In this work we have critically reviewed the processes in high-temperature sublimation growth of graphene in Ar atmosphere using enclosed graphite crucible. Special focus is put on buffer layer formation and free charge carrier properties of monolayer graphene and quasi-freestanding monolayer garphene on 4H-SiC. We show that by introducing Ar at different temperatures, TAr one can shift to higher temperatures the formation of the buffer layer for both n-type and semi-insulating substrates. A scenario explaining the observed suppresed formation of buffer layer at higher TAr is proposed and discussed. Increased TAr is also shown to reduce the sp3 hybridization content and defect densities in the buffer layer on n-type conductive substrates. Growth on semi-insulating substrates results in ordered buffer layer with significantly improved structural properties, for which TAr plays only a minor role. The free charge density and mobility parameters of monolayer graphene and quasi-freestanding monolayer graphene with different TAr and different environmental treatment conditions are determined by contactless terahertz optical Hall effect. An efficient annealing of donors on and near the SiC surface takes place in intrinsic monolayer graphene grown at 2000∘C, and which is found to be independent of TAr. Higher TAr leads to higher free charge carrier mobility parameters in both intrinsically n-type and ambient p-type doped monolayer graphene. TAr is also found to have a profound effect on the free hole parameters of quasi-freestanding monolayer graphene. These findings are discussed in view of interface and buffer layer properties in order to construct a comprehensive picture of high-temperature sublimation growth and provide guidance for growth parameters optimization depending on the targeted graphene application.

Homogenization of Radial Temperature by a Tungsten Sink in Sublimation Growth of 45 mm AlN Single Crystal

To reduce the thermal stress during the sublimation growth of 45 mm AlN single crystal, a tungsten sink was put on the top of the crucible lid. Numerical experiments showed that the radial temperature gradient was reduced due to the homogenization effect on temperature as a result of the sink. Therefore, this simple tungsten sink method has the potential to grow large-size AlN ingots with fewer cracks. It also reveals that enhancing the heat exchange of the crucible lid is an effective way to improve the quality of crystal growth.

Investigation on the Threading Dislocations Formed by Lattice Misfits during Initial Stage of Sublimation Growth of 4H-SiC

We investigated the relation between the nucleation of dislocations and the lattice misfits by nitrogen concentration difference between seed and grown crystal during the initial stage of growth. 4H-SiC single crystals were grown with various nitrogen gas flow rates introduced into the crystal growing chamber under the same temperature and pressure to minimize the effect of thermal stress on the nucleation of dislocations. The nitrogen atomic concentrations of grown crystals depended on the introduced nitrogen gas ratios and they highly increased at the very early stage of growth. The generation of new threading dislocations at the interface also was affected by the nitrogen atomic concentrations differences between seed and grown crystals. Very few generated threading dislocations were observed in low nitrogen atomic concentration samples, however nucleation of threading dislocations at the interface were found in high nitrogen atomic concentrations samples. At initial stages of PVT growth process, the generation of threading dislocations induced by lattice misfits originated from nitrogen concentration difference between seed and grown crystals were investigated and found the appropriate nitrogen gas flow rates and profile at the heating and depressurized stage.