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- 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.
- ItemProtection Mechanism against Photocorrosion of GaN Photoanodes Provided by NiO Thin Layers(Weinheim : Wiley-VCH, 2020) Kamimura, Jumpei; Budde, Melanie; Bogdanoff, Peter; Tschammer, Carsten; Abdi, Fatwa F.; van de Krol, Roel; Bierwagen, Oliver; Riechert, Henning; Geelhaar, LutzThe photoelectrochemical properties of n-type Ga-polar GaN photoelectrodes covered with NiO layers of different thicknesses in the range 0–20 nm are investigated for aqueous solution. To obtain layers of well-defined thickness and high crystal quality, NiO is grown by plasma-assisted molecular-beam epitaxy. Stability tests reveal that the NiO layers suppress photocorrosion. With increasing NiO thickness, the onset of the photocurrent is shifted to more positive voltages and the photocurrent is reduced, especially for low bias potentials, indicating that hole transfer to the electrolyte interface is hindered by thicker NiO layers. Furthermore, cathodic transient spikes are observed under intermittent illumination, which hints at surface recombination processes. These results are inconsistent with the common explanation of the protection mechanism that the band alignment of GaN/NiO enables efficient hole-injection, thus preventing hole accumulation at the GaN surface that would lead to anodic photocorrosion. Interestingly, the morphology of the etch pits as well as further experiments involving the photodeposition of Ag indicate that photocorrosion of GaN photoanodes is related to reductive processes at threading dislocations. Therefore, it is concluded that the NiO layers block the transfer of photogenerated electrons from GaN to the electrolyte interface, which prevents the cathodic photocorrosion. © 2020 The Authors. Solar RRL published by Wiley-VCH GmbH