skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: (010) β-(Alx, Ga1−x)2O3 growth using tritertiarybutylaluminum as Al gas precursor via hybrid molecular beam epitaxy
We report the epitaxial growth of (010) β-(AlxGa1−x)2O3 using tritertiarybutylaluminum (TTBAl) as an aluminum gas precursor in a hybrid molecular beam epitaxy (h-MBE) system. In conventional MBE systems, a thermal effusion cell is typically used to supply Al. However, in an oxide MBE system, using a conventional Al effusion cell can cause difficulties due to the oxidation of the Al source during growth. This often requires breaking the vacuum frequently to reload Al. Our approach utilizes TTBAl, a gaseous Al source, via a h-MBE to circumvent the oxidation issues associated with traditional solid Al sources. We investigated the growth conditions of β-(AlxGa1−x)2O3, varying TTBAl supply and growth temperature. For this purpose, we utilized both elemental Ga and Ga-suboxide as Ga precursors. Controllable and repeatable growth of β-(AlxGa1−x)2O3 with Al compositions ranging from 1% to 25% was achieved. The impurity incorporation and crystal quality of the resulting β-(AlxGa1−x)2O3 films were also studied. Using TTBAl as a gaseous precursor in h-MBE has proven to maintain stable Al supply, enabling the controlled growth of high-quality β-(AlxGa1−x)2O3 films.  more » « less
Award ID(s):
2043803 2426363
PAR ID:
10570503
Author(s) / Creator(s):
; ; ; ; ;
Publisher / Repository:
AIP
Date Published:
Journal Name:
Applied Physics Letters
Volume:
125
Issue:
16
ISSN:
0003-6951
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; ; et al (, APL Materials)
    We report the use of suboxide molecular-beam epitaxy (S-MBE) to grow α-(AlxGa1−x)2O3 films on (110) sapphire substrates over the 0 < x < 0.95 range of aluminum content. In S-MBE, 99.98% of the gallium-containing molecular beam arrives at the substrate in a preoxidized form as gallium suboxide (Ga2O). This bypasses the rate-limiting step of conventional MBE for the growth of gallium oxide (Ga2O3) from a gallium molecular beam and allows us to grow fully epitaxial α-(AlxGa1−x)2O3 films at growth rates exceeding 1 µm/h and relatively low substrate temperature (Tsub = 605 ± 15 °C). The ability to grow α-(AlxGa1−x)2O3 over the nominally full composition range is confirmed by Vegard’s law applied to the x-ray diffraction data and by optical bandgap measurements with ultraviolet–visible spectroscopy. We show that S-MBE allows straightforward composition control and bandgap selection for α-(AlxGa1−x)2O3 films as the aluminum incorporation x in the film is linear with the relative flux ratio of aluminum to Ga2O. The films are characterized by atomic-force microscopy, x-ray diffraction, and scanning transmission electron microscopy (STEM). These α-(AlxGa1−x)2O3 films grown by S-MBE at record growth rates exhibit a rocking curve full width at half maximum of ≊ 12 arc secs, rms roughness <1 nm, and are fully commensurate for x ≥ 0.5 for 20–50 nm thick films. STEM imaging of the x = 0.78 sample reveals high structural quality and uniform composition. Despite the high structural quality of the films, our attempts at doping with silicon result in highly insulating films. 
    more » « less
  2. ; ; ; ; ; ; ; ; (, Journal of Applied Physics)
    This study investigates the electrical and structural properties of metal–oxide–semiconductor capacitors (MOSCAPs) with in situ metal-organic chemical vapor deposition-grown Al2O3 dielectrics deposited at varying temperatures on (010) β-Ga2O3 and β-(AlxGa1−x)2O3 films with different Al compositions. The Al2O3/β-Ga2O3 MOSCAPs exhibited a strong dependence of electrical properties on Al2O3 deposition temperature. At 900 °C, reduced voltage hysteresis (∼0.3 V) with improved reverse breakdown voltage (74.5 V) was observed, corresponding to breakdown fields of 5.01 MV/cm in Al2O3 and 4.11 MV/cm in β-Ga2O3 under reverse bias. In contrast, 650 °C deposition temperature resulted in higher voltage hysteresis (∼3.44 V) and lower reverse breakdown voltage (38.8 V) with breakdown fields of 3.69 and 2.87 MV/cm in Al2O3 and β-Ga2O3, respectively, but exhibited impressive forward breakdown field, increasing from 5.62 MV/cm at 900 °C to 7.25 MV/cm at 650 °C. High-resolution scanning transmission electron microscopy (STEM) revealed improved crystallinity and sharper interfaces at 900 °C, contributing to enhanced reverse breakdown performance. For Al2O3/β-(AlxGa1−x)2O3 MOSCAPs, increasing Al composition (x) from 5.5% to 9.2% reduced net carrier concentration and improved reverse breakdown field contributions from 2.55 to 2.90 MV/cm in β-(AlxGa1−x)2O3 and 2.41 to 3.13 MV/cm in Al2O3. The electric field in Al2O3 dielectric under forward bias breakdown also improved from 5.0 to 5.4 MV/cm as Al composition increased from 5.5% to 9.2%. The STEM imaging confirmed the compositional homogeneity and excellent stoichiometry of both Al2O3 and β-(AlxGa1−x)2O3 layers. These findings demonstrate the robust electrical performance, high breakdown fields, and excellent structural quality of Al2O3/β-Ga2O3 and Al2O3/β-(AlxGa1−x)2O3 MOSCAPs, highlighting their potential for high-power electronic applications. 
    more » « less
  3. ; ; ; ; ; (, physica status solidi (RRL) – Rapid Research Letters)
    Growths of monoclinic (AlxGa1−x)2O3thin films up to 99% Al contents are demonstrated via metalorganic chemical vapor deposition (MOCVD) using trimethylgallium (TMGa) as the Ga precursor. The utilization of TMGa, rather than triethylgallium, enables a significant improvement of the growth rates (>2.5 μm h−1) of β‐(AlxGa1−x)2O3thin films on (010), (100), and (01) β‐Ga2O3substrates. By systematically tuning the precursor molar flow rates, growth of coherently strained phase pure β‐(AlxGa1−x)2O3films is demonstrated by comprehensive material characterizations via high‐resolution X‐ray diffraction (XRD) and atomic‐resolution scanning transmission electron microscopy (STEM) imaging. Monoclinic (AlxGa1−x)2O3films with Al contents up to 99, 29, and 16% are achieved on (100), (010), and (01) β‐Ga2O3substrates, respectively. Beyond 29% of Al incorporation, the (010) (AlxGa1−x)2O3films exhibit β‐ to γ‐phase segregation. β‐(AlxGa1−x)2O3films grown on (01) β‐Ga2O3show local segregation of Al along (100) plane. Record‐high Al incorporations up to 99% in monoclinic (AlxGa1−x)2O3grown on (100) Ga2O3are confirmed from XRD, STEM, electron nanodiffraction, and X‐ray photoelectron spectroscopy measurements. These results indicate great promises of MOCVD development of β‐(AlxGa1−x)2O3films and heterostructures with high Al content and growth rates using TMGa for next‐generation high‐power and high‐frequency electronic devices. 
    more » « less
  4. ; ; ; ; ; ; ; (, APL Materials)
    Phase pure β-(Al x Ga 1−x ) 2 O 3 thin films are grown on (001) oriented β-Ga 2 O 3 substrates via metalorganic chemical vapor deposition. By systematically tuning the precursor molar flow rates, the epitaxial growth of coherently strained β-(Al x Ga 1−x ) 2 O 3 films is demonstrated with up to 25% Al compositions as evaluated by high resolution x-ray diffraction. The asymmetrical reciprocal space mapping confirms the growth of coherent β-(Al x Ga 1−x ) 2 O 3 films (x < 25%) on (001) β-Ga 2 O 3 substrates. However, the alloy inhomogeneity with local segregation of Al along the ([Formula: see text]) plane is observed from atomic resolution STEM imaging, resulting in wavy and inhomogeneous interfaces in the β-(Al x Ga 1−x ) 2 O 3 /β-Ga 2 O 3 superlattice structure. Room temperature Raman spectra of β-(Al x Ga 1−x ) 2 O 3 films show similar characteristics peaks as the (001) β-Ga 2 O 3 substrate without obvious Raman shifts for films with different Al compositions. Atom probe tomography was used to investigate the atomic level structural chemistry with increasing Al content in the β-(Al x Ga 1−x ) 2 O 3 films. A monotonous increase in chemical heterogeneity is observed from the in-plane Al/Ga distributions, which was further confirmed via statistical frequency distribution analysis. Although the films exhibit alloy fluctuations, n-type doping demonstrates good electrical properties for films with various Al compositions. The determined valence and conduction band offsets at β-(Al x Ga 1−x ) 2 O 3 /β-Ga 2 O 3 heterojunctions using x-ray photoelectron spectroscopy reveal the formation of type-II (staggered) band alignment. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Journal of Applied Physics)
    In this work, the structural and electrical properties of metalorganic chemical vapor deposited Si-doped β-(Al x Ga 1−x ) 2 O 3 thin films grown on (010) β-Ga 2 O 3 substrates are investigated as a function of Al composition. The room temperature Hall mobility of 101 cm 2 /V s and low temperature peak mobility (T = 65 K) of 1157 cm 2 /V s at carrier concentrations of 6.56 × 10 17 and 2.30 × 10 17  cm −3 are measured from 6% Al composition samples, respectively. The quantitative secondary ion mass spectroscopy (SIMS) characterization reveals a strong dependence of Si and other unintentional impurities, such as C, H, and Cl concentrations in β-(Al x Ga 1−x ) 2 O 3 thin films, with different Al compositions. Higher Al compositions in β-(Al x Ga 1−x ) 2 O 3 result in lower net carrier concentrations due to the reduction of Si incorporation efficiency and the increase of C and H impurity levels that act as compensating acceptors in β-(Al x Ga 1−x ) 2 O 3 films. Lowering the growth chamber pressure reduces Si concentrations in β-(Al x Ga 1−x ) 2 O 3 films due to the increase of Al compositions as evidenced by comprehensive SIMS and Hall characterizations. Due to the increase of lattice mismatch between the epifilm and substrate, higher Al compositions lead to cracking in β-(Al x Ga 1−x ) 2 O 3 films grown on β-Ga 2 O 3 substrates. The (100) cleavage plane is identified as a major cracking plane limiting the growth of high-quality Si-doped (010) β-(Al x Ga 1−x ) 2 O 3 films beyond the critical thicknesses, which leads to highly anisotropic and inhomogeneous behaviors in terms of conductivity. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email