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  1. Abstract

    The anisotropic dielectric functions (DF) of corundum structuredm-planeα-(AlxGa1−x)2O3thin films (up tox= 0.76) grown onm-plane sapphire substrate by metalorganic CVD have been investigated. IR and visible–UV spectroscopic ellipsometry yields the DFs, while X-ray diffraction revealed the lattice parameters (a,m,c), showing the samples are almost fully relaxed. Analysis of the IR DFs from 250 to 6000 cm−1by a complex Lorentz oscillator model yields the anisotropic IR active phononsEuandA2uand the shift towards higher wavenumbers with increasing Al content. Analyzing the UV DFs from 0.5 to 6.6 eV we find the change in the dielectric limitsεand the shift of the Γ-point transition energies with increasing Al content. This results in anisotropic bowing parameters forα-(AlxGa1−x)2O3ofb= 2.1 eV andb∣∣= 1.7 eV.

     
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  2. β-phase gallium oxide (Ga2O3) is an emerging ultrawide bandgap (UWBG) semiconductor with a bandgap energy of ∼ 4.8 eV and a predicted high critical electric field strength of ∼8 MV/cm, enabling promising applications in next generation high power electronics and deep ultraviolet optoelectronics. The advantages of Ga2O3 also stem from its availability of single crystal bulk native substrates synthesized from melt, and its well-controllable n-type doping from both bulk growth and thin film epitaxy. Among several thin film growth methods, metalorganic chemical vapor deposition (MOCVD) has been demonstrated as an enabling technology for developing high-quality epitaxy of Ga2O3 thin films, (AlxGa1−x)2O3 alloys, and heterostructures along various crystal orientations and with different phases. This tutorial summarizes the recent progresses in the epitaxial growth of β-Ga2O3 thin films via different growth methods, with a focus on the growth of Ga2O3 and its compositional alloys by MOCVD. The challenges for the epitaxial development of β-Ga2O3 are discussed, along with the opportunities of future works to enhance the state-of-the-art device performance based on this emerging UWBG semiconductor material system. 
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    Free, publicly-accessible full text available June 7, 2024
  3. In this Letter, the role of background carbon in metalorganic chemical vapor deposition (MOCVD) β-Ga2O3 growth using trimethylgallium (TMGa) as the Ga precursor was investigated. The quantitative C and H incorporations in MOCVD β-Ga2O3 thin films grown at different growth rates and temperatures were measured via quantitative secondary ion mass spectroscopy (SIMS). The SIMS results revealed both [C] and [H] increase as the TMGa molar flow rate/growth rate increases or growth temperature decreases. The intentional Si incorporation in MOCVD β-Ga2O3 thin films decreases as the growth rate increases or the growth temperature decreases. For films grown at relatively fast growth rates (GRs) (TMGa > 58 μmol/min, GR > 2.8 μm/h) or relatively low temperature (<950 °C), the [C] increases faster than that of the [H]. The experimental results from this study demonstrate the previously predicted theory—H can effectively passivate the compensation effect of C in n-type β-Ga2O3. The extracted net doping concentration from quantitative SIMS {[Si]-([C]-[H])} agrees well with the free carrier concentration measured from Hall measurement. The revealing of the role of C compensation in MOCVD β-Ga2O3 and the effect of H incorporation will provide guidance on designing material synthesis for targeted device applications. 
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    Free, publicly-accessible full text available June 5, 2024
  4. 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. 
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  5. Epitaxial growth of κ-phase Ga 2 O 3 thin films is investigated on c-plane sapphire, GaN- and AlN-on-sapphire, and (100) oriented yttria stabilized zirconia (YSZ) substrates via metalorganic chemical vapor deposition. The structural and surface morphological properties are investigated by comprehensive material characterization. Phase pure κ-Ga 2 O 3 films are successfully grown on GaN-, AlN-on-sapphire, and YSZ substrates through a systematical tuning of growth parameters including the precursor molar flow rates, chamber pressure, and growth temperature, whereas the growth on c-sapphire substrates leads to a mixture of β- and κ-polymorphs of Ga 2 O 3 under the investigated growth conditions. The influence of the crystalline structure, surface morphology, and roughness of κ-Ga 2 O 3 films grown on different substrates are investigated as a function of precursor flow rate. High-resolution scanning transmission electron microscopy imaging of κ-Ga 2 O 3 films reveals abrupt interfaces between the epitaxial film and the sapphire, GaN, and YSZ substrates. The growth of single crystal orthorhombic κ-Ga 2 O 3 films is confirmed by analyzing the scanning transmission electron microscopy nanodiffraction pattern. The chemical composition, surface stoichiometry, and bandgap energies of κ-Ga 2 O 3 thin films grown on different substrates are studied by high-resolution x-ray photoelectron spectroscopy (XPS) measurements. The type-II (staggered) band alignments at three interfaces between κ-Ga 2 O 3 and c-sapphire, AlN, and YSZ substrates are determined by XPS, with an exception of κ-Ga 2 O 3 /GaN interface, which shows type-I (straddling) band alignment. 
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  6. Metalorganic chemical vapor deposition (MOCVD) growths of β-Ga 2 O 3 on on-axis (100) Ga 2 O 3 substrates are comprehensively investigated. Key MOCVD growth parameters including growth temperature, pressure, group VI/III molar flow rate ratio, and carrier gas flow rate are mapped. The dependence of the growth conditions is correlated with surface morphology, growth rate, and electron transport properties of the MOCVD grown (100) β-Ga 2 O 3 thin films. Lower shroud gas (argon) flow is found to enhance the surface smoothness with higher room temperature (RT) electron Hall mobility. The growth rate of the films decreases but with an increase of electron mobility as the VI/III molar flow rate ratio increases. Although no significant variation on the surface morphologies is observed at different growth temperatures, the general trend of electron Hall mobilities are found to increase with increasing growth temperature. The growth rates reduce significantly with uniform surface morphologies as the chamber pressure increases. By tuning the silane flow rate, the controllable carrier concentration of (100) β-Ga 2 O 3 thin films between low-10 17  cm −3 and low-10 18  cm −3 was achieved. Under optimized growth condition, an (100) β-Ga 2 O 3 thin film with RMS roughness value of 1.64 nm and a RT mobility of 24 cm 2 /Vs at a carrier concentration of 7.0 × 10 17  cm −3 are demonstrated. The mobilities are primarily limited by the twin lamellae and stacking faults defects generated from the growth interface. Atomic resolution scanning transmission electron microscopy reveals the formation of twin boundary defects in the films, resulting in the degradation of crystalline quality. Results from this work provide fundamental understanding of the MOCVD epitaxy of (100) β-Ga 2 O 3 on on-axis Ga 2 O 3 substrates and the dependence of the material properties on growth conditions. The limitation of electron transport properties of the (100) β-Ga 2 O 3 thin films below 25 cm 2 /Vs is attributed to the formation of incoherent boundaries (twin lamellae) and stacking faults grown along the on-axis (100) crystal orientation. 
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  7. The in situ metalorganic chemical vapor deposition (MOCVD) growth of Al 2 O 3 dielectrics on β-Ga 2 O 3 and β-(Al x Ga 1−x ) 2 O 3 films is investigated as a function of crystal orientations and Al compositions of β-(Al x Ga 1−x ) 2 O 3 films. The interface and film qualities of Al 2 O 3 dielectrics are evaluated by high-resolution x-ray diffraction and scanning transmission electron microscopy imaging, which indicate the growth of high-quality amorphous Al 2 O 3 dielectrics with abrupt interfaces on (010), (100), and [Formula: see text] oriented β-(Al x Ga 1−x ) 2 O 3 films. The surface stoichiometries of Al 2 O 3 deposited on all orientations of β-(Al x Ga 1−x ) 2 O 3 are found to be well maintained with a bandgap energy of 6.91 eV as evaluated by high-resolution x-ray photoelectron spectroscopy, which is consistent with the atomic layer deposited (ALD) Al 2 O 3 dielectrics. The evolution of band offsets at both in situ MOCVD and ex situ ALD deposited Al 2 O 3 /β-(Al x Ga 1−x ) 2 O 3 is determined as a function of Al composition, indicating the influence of the deposition method, orientation, and Al composition of β-(Al x Ga 1−x ) 2 O 3 films on resulting band alignments. Type II band alignments are determined at the MOCVD grown Al 2 O 3 /β-(Al x Ga 1−x ) 2 O 3 interfaces for the (010) and (100) orientations, whereas type I band alignments with relatively low conduction band offsets are observed along the [Formula: see text] orientation. The results from this study on MOCVD growth and band offsets of amorphous Al 2 O 3 deposited on differently oriented β-Ga 2 O 3 and β-(Al x Ga 1−x ) 2 O 3 films will potentially contribute to the design and fabrication of future high-performance β-Ga 2 O 3 and β-(Al x Ga 1−x ) 2 O 3 based transistors using MOCVD in situ deposited Al 2 O 3 as a gate dielectric. 
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  8. 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. 
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  9. High crystalline quality thick β-Ga2O3drift layers are essential for multi-kV vertical power devices. Low-pressure chemical vapor deposition (LPCVD) is suitable for achieving high growth rates. This paper presents a systematic study of the Schottky barrier diodes fabricated on four different Si-doped homoepitaxial β-Ga2O3thin films grown on Sn-doped (010) and (001) β-Ga2O3substrates by LPCVD with a fast growth rate varying from 13 to 21  μm/h. A higher temperature growth results in the highest reported growth rate to date. Room temperature current density–voltage data for different Schottky diodes are presented, and diode characteristics, such as ideality factor, barrier height, specific on-resistance, and breakdown voltage are studied. Temperature dependence (25–250 °C) of the ideality factor, barrier height, and specific on-resistance is also analyzed from the J–V–T characteristics of the fabricated Schottky diodes.

     
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