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.
more »
« less
Deposition pressure-induced microstructure control and plasmonic property tuning in hybrid ZnO–Ag x Au 1−x thin films
Self-assembled oxide–metallic alloy nanopillars as hybrid plasmonic metamaterials ( e.g. , ZnO–Ag x Au 1−x ) in a thin film form have been grown using a pulsed laser deposition method. The hybrid films were demonstrated to be highly tunable via systematic tuning of the oxygen background pressure during deposition. The pressure effects on morphology and optical properties have been investigated and found to be critical to the overall properties of the hybrid films. Specifically, low background pressure results in the vertically aligned nanocomposite (VAN) form while the high-pressure results in more lateral growth of the nanoalloys. Strong surface plasmon resonance was observed in the UV-vis region and a hyperbolic dielectric function was achieved due to the anisotropic morphology. The oxide–nanoalloy hybrid material grown in this work presents a highly effective approach for tuning the binary nanoalloy morphology and properties through systematic parametric changes, important for their potential applications in integrated photonics and plasmonics such as sensors, energy harvesting devices, and beyond.
more »
« less
- Award ID(s):
- 1565822
- NSF-PAR ID:
- 10289930
- Date Published:
- Journal Name:
- Nanoscale Advances
- Volume:
- 3
- Issue:
- 10
- ISSN:
- 2516-0230
- Page Range / eLocation ID:
- 2870 to 2878
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Metamaterials present great potential in the applications of solar cells and nanophotonics, such as super lenses and other meta devices, owing to their superior optical properties. In particular, hyperbolic metamaterials (HMMs) with exceptional optical anisotropy offer improved manipulation of light–matter interactions as well as a divergence in the density of states and thus show enhanced performances in related fields. Recently, the emerging field of oxide–metal vertically aligned nanocomposites (VANs) suggests a new approach to realize HMMs with flexible microstructural modulations. In this work, a new oxide–metal metamaterial system, CeO 2 –Au, has been demonstrated with variable Au phase morphologies from nanoparticle-in-matrix (PIM), nanoantenna-in-matrix, to VAN. The effective morphology tuning through deposition background pressure, and the corresponding highly tunable optical performance of three distinctive morphologies, were systematically explored and analyzed. A hyperbolic dispersion at high wavelength has been confirmed in the nano-antenna CeO 2 –Au thin film, proving this system as a promising candidate for HMM applications. More interestingly, a new and abnormal in-plane epitaxy of Au nanopillars following the large mismatched CeO 2 matrix instead of the well-matched SrTiO 3 substrate, was discovered. Additionally, the tilting angle of Au nanopillars, α , has been found to be a quantitative measure of the balance between kinetics and thermodynamics during the depositions of VANs. All these findings provide valuable information in the understanding of the VAN formation mechanisms and related morphology tuning.more » « less
-
more » « less
The growth of monoclinic phase‐pure gallium oxide (β‐Ga2O3) layers by metal–organic chemical vapor deposition on c‐plane sapphire and aluminum nitride (AlN) templates using silicon‐oxygen bonding (SiO
x ) as a phase stabilizer is reported. The β‐Ga2O3layers are grown using triethylgallium, oxygen, and silane for gallium, oxygen, and silicon precursors, respectively, at 700 °C, with and without silane flow in the process. The samples grown on sapphire with SiOx phase stabilization show a notable change from samples without phase stabilization in the roughness and resistivity, from 16.2 to 4.2 nm and from 85.82 to 135.64 Ω cm, respectively. X‐ray diffraction reveals a pure‐monoclinic phase, and Raman spatial mapping exhibits higher tensile strain in the films in the presence of SiOx . The β‐Ga2O3layers grown on an AlN template, using the same processes as for sapphire, show an excellent epitaxial relationship between β‐Ga2O3and AlN and have a significant change in β‐Ga2O3surface morphology. -
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.more » « less
-
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
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/d0na00887g
