skip to main content

This content will become publicly available on December 1, 2023

Title: MOCVD growth and band offsets of κ-phase Ga 2 O 3 on c-plane sapphire, GaN- and AlN-on-sapphire, and (100) YSZ substrates
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 more » 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. « less
Authors:
; ; ; ; ;
Award ID(s):
1810041 2019753
Publication Date:
NSF-PAR ID:
10383176
Journal Name:
Journal of Vacuum Science & Technology A
Volume:
40
Issue:
6
Page Range or eLocation-ID:
062704
ISSN:
0734-2101
Sponsoring Org:
National Science Foundation
More Like this
  1. Thick (23 µm) films of κ-Ga 2 O 3 were grown by Halide Vapor Phase Epitaxy (HVPE) on GaN/sapphire templates at 630 °C. X-ray analysis confirmed the formation of single-phase κ-Ga 2 O 3 with half-widths of the high-resolution x-ray diffraction (004), (006), and (008) symmetric reflections of 4.5 arc min and asymmetric (027) reflection of 14 arc min. Orthorhombic κ-Ga 2 O 3 polymorph formation was confirmed from analysis of the Kikuchi diffraction pattern in electron backscattering diffraction. Secondary electron imaging indicated a reasonably flat surface morphology with a few (area density ∼10 3  cm −2 ) approximately circular (diameter ∼50–100 µm) uncoalesced regions, containing κ-Ga 2 O 3 columns with in-plane dimensions and a height of about 10 µm. Micro-cathodoluminescence (MCL) spectra showed a wide 2–3.5 eV band that could be deconvoluted into narrower bands peaked at 2.59, 2.66, 2.86, and 3.12 eV. Ni Schottky diodes prepared on the films showed good rectification but a high series resistance. The films had a thin near-surface region dominated by E c − 0.7 eV deep centers and a deeper region (∼2 µm from the surface) dominated by shallow donors with concentrations of ≤10 16  cm −3 . Photocurrent and photocapacitance spectra showed the presence ofmore »deep compensating acceptors with optical ionization energies of ∼1.35 and 2.3 eV, the latter being close to the energy of one of the MCL bands. Deep level transient spectroscopy revealed deep traps with energies near 0.3, 0.6, 0.7, 0.8, and 1 eV from the conduction band edge. The results show the potential of HVPE to grow very thick κ-Ga 2 O 3 on GaN/sapphire templates.« less
  2. Halide vapor phase epitaxial (HVPE) Ga 2 O 3 films were grown on c-plane sapphire and diamond substrates at temperatures up to 550 °C without the use of a barrier dielectric layer to protect the diamond surface. Corundum phase α-Ga 2 O 3 was grown on the sapphire substrates, whereas the growth on diamond resulted in regions of nanocrystalline β-Ga 2 O 3 (nc-β-Ga 2 O 3 ) when oxygen was present in the HVPE reactor only during film growth. X-ray diffraction confirmed the growth of α-Ga 2 O 3 on sapphire but failed to detect any β-Ga 2 O 3 reflections from the films grown on diamond. These films were further characterized via Raman spectroscopy, which revealed the β-Ga 2 O 3 phase of these films. Transmission electron microscopy demonstrated the nanocrystalline character of these films. From cathodoluminescence spectra, three emission bands, UVL′, UVL, and BL, were observed for both the α-Ga 2 O 3 /sapphire and nc-Ga 2 O 3 /diamond, and these bands were centered at approximately 3.7, 3.2, and 2.7 eV.
  3. 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 themore »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.« less
  4. The hot-wall metalorganic chemical vapor deposition (MOCVD) concept, previously shown to enable superior material quality and high performance devices based on wide bandgap semiconductors, such as Ga(Al)N and SiC, has been applied to the epitaxial growth of β-Ga 2 O 3 . Epitaxial β-Ga 2 O 3 layers at high growth rates (above 1 μm/h), at low reagent flows, and at reduced growth temperatures (740 °C) are demonstrated. A high crystalline quality epitaxial material on a c-plane sapphire substrate is attained as corroborated by a combination of x-ray diffraction, high-resolution scanning transmission electron microscopy, and spectroscopic ellipsometry measurements. The hot-wall MOCVD process is transferred to homoepitaxy, and single-crystalline homoepitaxial β-Ga 2 O 3 layers are demonstrated with a [Formula: see text]01 rocking curve width of 118 arc sec, which is comparable to those of the edge-defined film-fed grown ([Formula: see text]01) β-Ga 2 O 3 substrates, indicative of similar dislocation densities for epilayers and substrates. Hence, hot-wall MOCVD is proposed as a prospective growth method to be further explored for the fabrication of β-Ga 2 O 3 .
  5. Controlling the growth of complex relaxor ferroelectric thin films and understanding the relationship between biaxial strain–structural domain characteristics are desirable for designing materials with a high electromechanical response. For this purpose, epitaxial thin films free of extended defects and secondary phases are urgently needed. Here, we used optimized growth parameters and target compositions to obtain epitaxial (40–45 nm) 0.67Pb(Mg 1/3 Nb 2/3 )O 3 –0.33PbTiO 3 /(20 nm) SrRuO 3 (PMN–33PT/SRO) heterostructures using pulsed-laser deposition (PLD) on singly terminated SrTiO 3 (STO) and ReScO 3 (RSO) substrates with Re = Dy, Tb, Gd, Sm, and Nd. In situ reflection high-energy electron diffraction (RHEED) and high-resolution X-ray diffraction (HR-XRD) analysis confirmed high-quality and single-phase thin films with smooth 2D surfaces. High-resolution scanning transmission electron microscopy (HR-STEM) revealed sharp interfaces and homogeneous strain further confirming the epitaxial cube-on-cube growth mode of the PMN–33PT/SRO heterostructures. The combined XRD reciprocal space maps (RSMs) and piezoresponse force microscopy (PFM) analysis revealed that the domain structure of the PMN–33PT heterostructures is sensitive to the applied compressive strain. From the RSM patterns, an evolution from a butterfly-shaped diffraction pattern for mildly strained PMN–33PT layers, which is evidence of stabilization of relaxor domains, to disc-shaped diffraction patterns formore »high compressive strains with a highly distorted tetragonal structure, is observed. The PFM amplitude and phase of the PMN–33PT thin films confirmed the relaxor-like for a strain state below ∼1.13%, while for higher compressive strain (∼1.9%) the irregularly shaped and poled ferroelectric domains were observed. Interestingly, the PFM phase hysteresis loops of the PMN–33PT heterostructures grown on the SSO substrates (strain state of ∼0.8%) exhibited an enhanced coercive field which is about two times larger than that of the thin films grown on GSO and NSO substrates. The obtained results show that epitaxial strain engineering could serve as an effective approach for tailoring and enhancing the functional properties in relaxor ferroelectrics.« less