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- ItemCobalt as a promising dopant for producing semi-insulating β -Ga2O3crystals: Charge state transition levels from experiment and theory(Melville, NY : AIP Publ., 2022) Seyidov, Palvan; Varley, Joel B.; Galazka, Zbigniew; Chou, Ta-Shun; Popp, Andreas; Fiedler, Andreas; Irmscher, KlausOptical absorption and photoconductivity measurements of Co-doped β-Ga2O3 crystals reveal the photon energies of optically excited charge transfer between the Co related deep levels and the conduction or valence band. The corresponding photoionization cross sections are fitted by a phenomenological model considering electron-phonon coupling. The obtained fitting parameters: thermal ionization (zero-phonon transition) energy, Franck-Condon shift, and effective phonon energy are compared with corresponding values predicted by first principle calculations based on density functional theory. A (+/0) donor level ∼0.85 eV above the valence band maximum and a (0/-) acceptor level ∼2.1 eV below the conduction band minimum are consistently derived. Temperature-dependent electrical resistivity measurement at elevated temperatures (up to 1000 K) yields a thermal activation energy of 2.1 ± 0.1 eV, consistent with the position of the Co acceptor level. Furthermore, the results show that Co doping is promising for producing semi-insulating β-Ga2O3 crystals.
- ItemSubstrate-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.
- ItemEfficient suboxide sources in oxide molecular beam epitaxy using mixed metal + oxide charges: The examples of SnO and Ga2O(Melville, NY : AIP Publ., 2020) Hoffmann, Georg; Budde, Melanie; Mazzolini, Piero; Bierwagend, OliverSources of suboxides, providing several advantages over metal sources for the molecular beam epitaxy (MBE) of oxides, are conventionally realized by decomposing the corresponding oxide charge at extreme temperatures. By quadrupole mass spectrometry of the direct flux from an effusion cell, we compare this conventional approach to the reaction of a mixed oxide + metal charge as a source for suboxides with the examples of SnO2 + Sn → 2 SnO and Ga2O3 + 4 Ga → 3 Ga2O. The high decomposition temperatures of the pure oxide charge were found to produce a high parasitic oxygen background. In contrast, the mixed charges reacted at significantly lower temperatures, providing high suboxide fluxes without additional parasitic oxygen. For the SnO source, we found a significant fraction of Sn2O2 in the flux from the mixed charge that was basically absent in the flux from the pure oxide charge. We demonstrate the plasma-assisted MBE growth of SnO2 using the mixed Sn + SnO2 charge to require less activated oxygen and a significantly lower source temperature than the corresponding growth from a pure Sn charge. Thus, the sublimation of mixed metal + oxide charges provides an efficient suboxide source for the growth of oxides by MBE. Thermodynamic calculations predict this advantage for further oxides as well, e.g., SiO2, GeO2, Al2O3, In2O3, La2O3, and Pr2O3 © 2020 Author(s).
- ItemSuitability of binary oxides for molecular-beam epitaxy source materials: A comprehensive thermodynamic analysis(Melville, NY : AIP Publ., 2020) Adkison, Kate M.; Shang, Shun-Li; Bocklund, Brandon J.; Klimm, Detlef; Schlom, Darrell G.; Liu, Zi-KuiWe have conducted a comprehensive thermodynamic analysis of the volatility of 128 binary oxides to evaluate their suitability as source materials for oxide molecular-beam epitaxy (MBE). 16 solid or liquid oxides are identified that evaporate nearly congruently from stable oxide sources to gas species: As2O3, B2O3, BaO, MoO3, OsO4, P2O5, PbO, PuO2, Rb2O, Re2O7, Sb2O3, SeO2, SnO, ThO2, Tl2O, and WO3. An additional 24 oxides could provide molecular beams with dominant gas species of CeO, Cs2O, DyO, ErO, Ga2O, GdO, GeO, HfO, HoO, In2O, LaO, LuO, NdO, PmO, PrO, PuO, ScO, SiO, SmO, TbO, Te2O2, U2O6, VO2, and YO2. The present findings are in close accord with available experimental results in the literature. For example, As2O3, B2O3, BaO, MoO3, PbO, Sb2O3, and WO3 are the only oxides in the ideal category that have been used in MBE. The remaining oxides deemed ideal for MBE awaiting experimental verification. We also consider two-phase mixtures as a route to achieve the desired congruent evaporation characteristic of an ideal MBE source. These include (Ga2O3 + Ga) to produce a molecular beam of Ga2O(g), (GeO2 + Ge) to produce GeO(g), (SiO2 + Si) to produce SiO(g), (SnO2 + Sn) to produce SnO(g), etc.; these suboxide sources enable suboxide MBE. Our analysis provides the vapor pressures of the gas species over the condensed phases of 128 binary oxides, which may be either solid or liquid depending on the melting temperature. © 2020 Author(s).
- ItemRefractory metal-based ohmic contacts on β-Ga2O3 using TiW(Melville, NY : AIP Publ., 2022) Tetzner, Kornelius; Schewski, Robert; Popp, Andreas; Anooz, Saud Bin; Chou, Ta-Shun; Ostermay, Ina; Kirmse, Holm; Würfl, JoachimThe present work investigates the use of the refractory metal alloy TiW as a possible candidate for the realization of ohmic contacts to the ultrawide bandgap semiconductor β-Ga2O3. Ohmic contact properties were analyzed by transfer length measurements of TiW contacts annealed at temperatures between 400 and 900 °C. Optimum contact properties with a contact resistance down to 1.5 × 10-5 ω cm2 were achieved after annealing at 700 °C in nitrogen on highly doped β-Ga2O3. However, a significant contact resistance increase was observed at annealing temperatures above 700 °C. Cross-sectional analyses of the contacts using scanning transmission electron microscopy revealed the formation of a TiOx interfacial layer of 3-5 nm between TiW and β-Ga2O3. This interlayer features an amorphous structure and most probably possesses a high amount of vacancies and/or Ga impurities supporting charge carrier injection. Upon annealing at temperatures of 900 °C, the interlayer increases in thickness up to 15 nm, featuring crystalline-like properties, suggesting the formation of rutile TiO2. Although severe morphological changes at higher annealing temperatures were also verified by atomic force microscopy, the root cause for the contact resistance increase is attributed to the structural changes in thickness and crystallinity of the interfacial layer.
- ItemEffect of post-metallization anneal on (100) Ga2O3/Ti–Au ohmic contact performance and interfacial degradation(Melville, NY : AIP Publ., 2022) Lee, Ming-Hsun; Chou, Ta-Shun; Bin Anooz, Saud; Galazka, Zbigniew; Popp, Andreas; Peterson, Rebecca L.Here, we investigate the effect of post-metallization anneal temperature on Ti/Au ohmic contact performance for (100)-oriented Ga2O3. A low contact resistance of ∼2.49 × 10−5 Ω·cm2 is achieved at an optimal anneal temperature of ∼420 °C for (100) Ga2O3. This is lower than the widely-used temperature of 470 °C for (010)-oriented Ga2O3. However, drastic degradation of the (100)-oriented contact resistance to ∼1.36 × 10−3 Ω·cm2 is observed when the anneal temperature was increased to 520 °C. Microscopy at the degraded ohmic contact revealed that the reacted Ti–TiOx interfacial layer has greatly expanded to 25–30 nm thickness and GaAu2 inclusions have formed between (310)-Ga2O3 planes and the Ti–TiOx layer. This degraded interface, which corresponds to the deterioration of ohmic contact properties, likely results from excess in-diffusion of Au and out-diffusion of Ga, concurrent with the expansion of the Ti–TiOx layer. These results demonstrate the critical influence of Ga2O3 anisotropy on the optimal post-metallization anneal temperature. Moreover, the observed Ti/Au contact degradation occurs for relatively moderate anneal conditions (520 °C for 1 min in N2), pointing to the urgent necessity of developing alternative metallization schemes for gallium oxide, including the use of Au-free electrodes
- ItemRecent progress in the development of β-Ga2O3 scintillator crystals grown by the Czochralski method(Washington, DC : OSA, 2021) Drozdowski, Winicjusz; Makowski, Michał; Witkowski, Marcin E.; Wojtowicz, Andrzej J.; Irmscher, Klaus; Schewski, Robert; Galazka, ZbigniewA high-quality bulk single crystal of β-Ga2O3 has been grown by the Czochralski method and its basic scintillation characteristics (light yield, energy resolution, proportionality, and scintillation decay times) have been investigated. All the samples cut from the crystal show promising scintillation yields between 8400 and 8920 ph/MeV, which is a noticeable step forward compared to previous studies. The remaining parameters, i.e. the energy resolution slightly above 10% (at 662 keV) and the scintillation mean decay time just under 1 μs, are at the same level as we have formerly recognized for β-Ga2O3. The proportionality of yield seems not to deviate from standards determined by other commercial scintillators.
- ItemFew-cycle 65-µJ pulses at 11.4 µm for ultrafast nonlinear longwave-infrared spectroscopy(Washington, DC : Optical Society of America, OSA, 2022) Fuertjes, Pia; Bock, Martin; Grafenstein, Lorenz von; Ueberschaer, Dennis; Griebner, Uwe; Elsaesser, ThomasLow-energy excitations can provide insight into the basic ultrafast nonequilibrium dynamics of condensed matter. High-energy femtosecond pulses in the long-wavelength infrared are required to induce such processes, and can be generated in an optical parametric chirped pulse amplification (OPCPA) system comprising three GaSe stages. A femtosecond Cr:ZnS laser serves as the front-end, providing the seed for the 2.0-µm pump and the 2.4-µm signal pulses without nonlinear conversion processes. The OPCPA system is pumped at 2.05 µm by a picosecond Ho:YLF regenerative amplifier at a 1-kHz repetition rate. The recompressed idler pulses at 11.4 µm have a duration of 185 fs and an unprecedented energy of 65 µJ, corresponding to a pump-to-idler conversion efficiency of 1.2%. Nonlinear transmission experiments in the range of the L2 infrared band of liquid water demonstrate the potential of the pulses for nonlinear vibrational spectroscopy of liquids and solids.