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- ItemKinetics versus thermodynamics of the metal incorporation in molecular beam epitaxy of (InxGa1−x)2O3(New York : American Institute of Physics, 2016) Vogt, Patrick; Bierwagen, OliverWe present a detailed study of the reaction kinetics and thermodynamics of the plasma-assisted oxide molecular beam epitaxy of the ternary compound (InxGa1−x)2O3 for 0 ≤ x ≤ 1. We measured the growth rate of the alloy in situ by laser reflectrometry as a function of growth temperature T G for different metal-to-oxygen flux ratios r Me, and nominal In concentrations x nom in the metal flux. We determined ex situ the In and Ga concentrations in the grown film by energy dispersive X-ray spectroscopy. The measured In concentration x shows a strong dependence on the growth parameters T G, r Me, and x nom whereas growth on different co-loaded substrates shows that in the macroscopic regime of ∼μm3 x does neither depend on the detailed layer crystallinity nor on crystal orientation. The data unveil that, in presence of In, Ga incorporation is kinetically limited by Ga2O desorption the same way as during Ga2O 3 growth. In contrast, In incorporation during ternary growth is thermodynamically suppressed by the presence of Ga due to stronger Ga–O bonds. Our experiments revealed that Ga adatoms decompose/etch the In–O bonds whereas In adatoms do not decompose/etch the Ga–O bonds. This result is supported by our thermochemical calculations. In addition we found that a low T G and/or excessively low r Me kinetically enables In incorporation into (InxGa1−x)2O3. This study may help growing high-quality ternary compounds (InxGa1−x)2O3 allowing band gap engineering over the range of 2.7–4.7 eV.
- ItemSilane-Mediated Expansion of Domains in Si-Doped κ-Ga2O3 Epitaxy and its Impact on the In-Plane Electronic Conduction(Weinheim : Wiley-VCH, 2022) Mazzolini, Piero; Fogarassy, Zsolt; Parisini, Antonella; Mezzadri, Francesco; Diercks, David; Bosi, Matteo; Seravalli, Luca; Sacchi, Anna; Spaggiari, Giulia; Bersani, Danilo; Bierwagen, Oliver; Janzen, Benjamin Moritz; Marggraf, Marcella Naomi; Wagner, Markus R.; Cora, Ildiko; Pécz, Béla; Tahraoui, Abbes; Bosio, Alessio; Borelli, Carmine; Leone, Stefano; Fornari, RobertoUnintentionally doped (001)-oriented orthorhombic κ-Ga2O3 epitaxial films on c-plane sapphire substrates are characterized by the presence of ≈ 10 nm wide columnar rotational domains that can severely inhibit in-plane electronic conduction. Comparing the in- and out-of-plane resistance on well-defined sample geometries, it is experimentally proved that the in-plane resistivity is at least ten times higher than the out-of-plane one. The introduction of silane during metal-organic vapor phase epitaxial growth not only allows for n-type Si extrinsic doping, but also results in the increase of more than one order of magnitude in the domain size (up to ≈ 300 nm) and mobility (highest µ ≈ 10 cm2V−1s−1, with corresponding lowest ρ ≈ 0.2 Ωcm). To qualitatively compare the mean domain dimension in κ-Ga2O3 epitaxial films, non-destructive experimental procedures are provided based on X-ray diffraction and Raman spectroscopy. The results of this study pave the way to significantly improved in-plane conduction in κ-Ga2O3 and its possible breakthrough in new generation electronics. The set of cross-linked experimental techniques and corresponding interpretation here proposed can apply to a wide range of material systems that suffer/benefit from domain-related functional properties.
- ItemTwo-dimensional electron gas of the In2O3 surface: Enhanced thermopower, electrical transport properties, and reduction by adsorbates or compensating acceptor doping(Woodbury, NY : Inst., 2020) Papadogianni, Alexandra; Rombach, Julius; Berthold, Theresa; Polyakov, Vladimir; Krischok, Stefan; Himmerlich, Marcel; Bierwagen, OliverIn2O3 is an n-type transparent semiconducting oxide possessing a surface electron accumulation layer (SEAL) like several other relevant semiconductors, such as InAs, InN, SnO2, and ZnO. Even though the SEAL is within the core of the application of In2O3 in conductometric gas sensors, a consistent set of transport properties of this two-dimensional electron gas (2DEG) is missing in the present literature. To this end, we investigate high-quality single-crystalline as well as textured doped and undoped In2O3(111) films grown by plasma-assisted molecular beam epitaxy to extract transport properties of the SEAL by means of Hall effect measurements at room temperature while controlling the oxygen adsorbate coverage via illumination. The resulting sheet electron concentration and mobility of the SEAL are ≈1.5×1013cm−2 and ≈150cm2/Vs, respectively, both of which are strongly reduced by oxygen-related surface adsorbates from the ambient air. Our transport measurements further demonstrate a systematic reduction of the SEAL by doping In2O3 with the deep compensating bulk acceptors Ni or Mg. This finding is supported by x-ray photoelectron spectroscopy (XPS) measurements of the surface band bending and SEAL electron emission. Quantitative analyses of these XPS results using self-consistent, coupled Schrödinger-Poisson calculations indicate the simultaneous formation of compensating bulk donor defects (likely oxygen vacancies), which almost completely compensate the bulk acceptors. Finally, an enhancement of the thermopower by reduced dimensionality is demonstrated in In2O3: Seebeck coefficient measurements of the surface 2DEG with partially reduced sheet electron concentrations between 3×1012 and 7×1012cm−2 (corresponding average volume electron concentration between 1×1019 and 2.3×1019cm−3) indicate a value enhanced by ≈80% compared to that of bulk Sn-doped In2O3 with comparable volume electron concentration.
- ItemEpitaxial synthesis of unintentionally doped p-type SnO (001) via suboxide molecular beam epitaxy(Melville, NY : AIP, 2023) Egbo, Kingsley; Luna, Esperanza; Lähnemann, Jonas; Hoffmann, Georg; Trampert, Achim; Grümbel, Jona; Kluth, Elias; Feneberg, Martin; Goldhahn, Rüdiger; Bierwagen, OliverBy employing a mixed SnO2 + Sn source, we demonstrate suboxide molecular beam epitaxy (S-MBE) growth of phase-pure single-crystalline metastable SnO (001) thin films on Y-stabilized ZrO2 (001) substrates at a growth rate of ∼1.0 nm/min without the need for additional oxygen. These films grow epitaxially across a wide substrate temperature range from 150 to 450 °C. Hence, we present an alternative pathway to overcome the limitations of high Sn or SnO2 cell temperatures and narrow growth windows encountered in previous MBE growth of metastable SnO. In situ laser reflectometry and line-of-sight quadrupole mass spectrometry were used to investigate the rate of SnO desorption as a function of substrate temperature. While SnO ad-molecule desorption at TS = 450 °C was growth-rate limiting, the SnO films did not desorb at this temperature after growth in vacuum. The SnO (001) thin films are transparent and unintentionally p-type doped, with hole concentrations and mobilities in the range of 0.9-6.0 × 1018 cm-3 and 2.0-5.5 cm2 V-1 s-1, respectively. These p-type SnO films obtained at low substrate temperatures are promising for back-end-of-line (BEOL) compatible applications and for integration with n-type oxides in pn heterojunctions and field-effect transistors.
- ItemDelayed crystallization of ultrathin Gd2O3 layers on Si(111) observed by in situ X-ray diffraction(London : BioMed Central, 2012) Hanke, Michael; Kaganer, Vladimir M.; Bierwagen, Oliver; Niehle, Michael; Trampert, AchimWe studied the early stages of Gd2O3 epitaxy on Si(111) in real time by synchrotron-based, high-resolution X-ray diffraction and by reflection high-energy electron diffraction. A comparison between model calculations and the measured X-ray scattering, and the change of reflection high-energy electron diffraction patterns both indicate that the growth begins without forming a three-dimensional crystalline film. The cubic bixbyite structure of Gd2O3 appears only after a few monolayers of deposition.
- ItemFaceting 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, OliverWe 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.
- ItemAnisotropic optical properties of highly doped rutile SnO2: Valence band contributions to the Burstein-Moss shift(New York : American Institute of Physics, 2018) Feneberg, Martin; Lidig, Christian; White, Mark E.; Tsai, Min Y.; Speck, James S.; Bierwagen, Oliver; Galazka, Zbigniew; Goldhahn, RüdigerThe interband absorption of the transparent conducting semiconductor rutile stannic oxide (SnO2) is investigated as a function of increasing free electron concentration. The anisotropic dielectric functions of SnO2:Sb are determined by spectroscopic ellipsometry. The onsets of strong interband absorption found at different positions shift to higher photon energies with increasing free carrier concentration. For the electric field vector parallel to the optic axis, a low energy shoulder increases in prominence with increasing free electron concentration. We analyze the influence of different many-body effects and can model the behavior by taking into account bandgap renormalization and the Burstein-Moss effect. The latter consists of contributions from the conduction and the valence bands which can be distinguished because the nonparabolic conduction band dispersion of SnO2 is known already with high accuracy. The possible originsof the shoulder are discussed. The most likely mechanism is identified to be interband transitions at jkj > 0 from a dipole forbidden valence band.