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    Towards smooth (010) ß-Ga2O3films homoepitaxially grown by plasma assisted molecular beam epitaxy: The impact of substrate offcut and metal-to-oxygen flux ratio
    (Bristol : IOP Publ., 2020) Mazzolini, P.; Bierwagen, O.
    Smooth interfaces and surfaces are beneficial for most (opto)electronic devices that are based on thin films and their heterostructures. For example, smoother interfaces in (010) ß-Ga2O3/(AlxGa1-x)2O3 heterostructures, whose roughness is ruled by that of the ß-Ga2O3 layer, can enable higher mobility 2-dimensional electron gases by reducing interface roughness scattering. To this end we experimentally prove that a substrate offcut along the [001] direction allows to obtain smooth ß-Ga2O3 layers in (010)-homoepitaxy under metal-rich deposition conditions. Applying In-mediated metal-exchange catalysis (MEXCAT) in molecular beam epitaxy at high substrate temperatures (Tg = 900 °C) we compare the morphology of layers grown on (010)-oriented substrates having different unintentional offcuts. The layer roughness is generally ruled by (i) the presence of (110)-and bar 110-facets visible as elongated features along the [001] direction (rms < 0.5 nm), and (ii) the presence of trenches (5-10 nm deep) orthogonal to [001]. We show that an unintentional substrate offcut of only ˜ 0.1° almost oriented along the [001] direction suppresses these trenches resulting in a smooth morphology with a roughness exclusively determined by the facets, i.e. rms ˜ 0.2 nm. Since we found the facet-and-trench morphology in layer grown by MBE with and without MEXCAT, we propose that the general growth mechanism for (010)-homoepitaxy is ruled by island growth whose coalescence results in the formation of the trenches. The presence of a substrate offcut in the [001] direction can allow for step-flow growth or island nucleation at the step edges, which prevents the formation of trenches. Moreover, we give experimental evidence for a decreasing surface diffusion length or increasing nucleation density on the substrate surface with decreasing metal-to-oxygen flux ratio. Based on our experimental results we can rule-out step bunching as cause of the trench formation as well as a surfactant-effect of indium during MEXCAT. © 2020 The Author(s). Published by IOP Publishing Ltd.
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    Substrate-orientation dependence of β -Ga2O3 (100), (010), (001), and (2 ̄ 01) homoepitaxy by indium-mediated metal-exchange catalyzed molecular beam epitaxy (MEXCAT-MBE)
    (Melville, NY : AIP Publ., 2020) Mazzolini, P.; Falkenstein, A.; Wouters, C.; Schewski, R.; Markurt, T.; Galazka, Z.; Martin, M.; Albrecht, M.; Bierwagen, O.
    We experimentally demonstrate how In-mediated metal-exchange catalysis (MEXCAT) allows us to widen the deposition window for β-Ga2O3 homoepitaxy to conditions otherwise prohibitive for its growth via molecular beam epitaxy (e.g., substrate temperatures ≥800 °C) on the major substrate orientations, i.e., (010), (001), (2⎯⎯01), and (100) 6°-offcut. The obtained crystalline qualities, surface roughnesses, growth rates, and In-incorporation profiles are shown and compared with different experimental techniques. The growth rates, Γ, for fixed growth conditions are monotonously increasing with the surface free energy of the different orientations with the following order: Γ(010) > Γ(001) > Γ(2⎯⎯01) > Γ(100). Ga2O3 surfaces with higher surface free energy provide stronger bonds to the surface ad-atoms or ad-molecules, resulting in decreasing desorption, i.e., a higher incorporation/growth rate. The structural quality in the case of (2⎯⎯01), however, is compromised by twin domains due to the crystallography of this orientation. Notably, our study highlights β-Ga2O3 layers with high structural quality grown by MEXCAT-MBE not only in the most investigated (010) orientation but also in the (100) and (001) ones. In particular, MEXCAT on the (001) orientation results in both growth rate and structural quality comparable to the ones achievable with (010), and the limited incorporation of In associated with the MEXCAT deposition process does not change the insulating characteristics of unintentionally doped layers. The (001) surface is therefore suggested as a valuable alternative orientation for devices.
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    Faceting and metal-exchange catalysis in (010) β-Ga2O3 thin films homoepitaxially grown by plasma-assisted molecular beam epitaxy
    (New York : American Institute of Physics, 2018) Mazzolini, P.; Vogt, P.; Schewski, R.; Wouters, C.; Albrecht, M.; Bierwagen, Oliver
    We here present an experimental study on (010)-oriented -Ga2O3 thin films homoepitaxially grown by plasma assisted molecular beam epitaxy. We study the effect of substrate treatments (i.e., O-plasma and Ga-etching) and several deposition parameters (i.e., growth temperature and metal-to-oxygen flux ratio) on the resulting Ga2O3 surface morphology and growth rate. In situ and ex-situ characterizations identified the formation of (110) and (¯110)-facets on the nominally oriented (010) surface induced by the Ga-etching of the substrate and by several growth conditions, suggesting (110) to be a stable (yet unexplored) substrate orientation. Moreover, we demonstrate how metal-exchange catalysis enabled by an additional In-flux significantly increases the growth rate (>threefold increment) of monoclinic Ga2O3 at high growth temperatures, while maintaining a low surface roughness (rms < 0.5 nm) and preventing the incorporation of In into the deposited layer. This study gives important indications for obtaining device-quality thin films and opens up the possibility to enhance the growth rate in -Ga2O3 homoepitaxy on different surfaces [e.g., (100) and (001)] via molecular beam epitaxy.