We report the growth and optical characterization of single-crystal BiFe1−xMnxO3 thin films directly on SrTiO3/Si(001) substrates using molecular beam epitaxy. X-ray diffraction confirmed epitaxial growth, film crystallinity, and sharp interface quality. Scanning electron microscopy and energy dispersive X-ray spectroscopy verified uniform film morphology and successful Mn incorporation. Spectroscopic ellipsometry revealed a systematic bandgap reduction with increasing Mn concentration, from 2.7 eV in BiFeO3 to 2.58 eV in BiFe0.74Mn0.26O3, consistent with previous reports on Mn-doped BiFeO3. These findings highlight the potential of BiFe1₋xMnxO3 films for bandgap engineering, advancing their integration into silicon-compatible multifunctional optoelectronic and photovoltaic applications.
more »
« less
MnO(001) thin films on MgO(001) grown by reactive MBE using supersonic molecular beams
MnO(001) thin films were grown on commercial MgO(001) substrates at 520 °C by reactive molecular beam epitaxy (MBE) using Mn vapor and O2-seeded supersonic molecular beams (SMBs) both with and without radio frequency (RF) plasma excitation. For comparison, MnO(001) films were grown by reactive MBE using O2 from a leak valve. X-ray photoelectron spectroscopy confirmed the Mn2+ oxidation state and 10%–15% excess oxygen near the growth surface. Reflection high-energy electron diffraction and x-ray diffraction evidenced that the films were rock salt cubic MnO with very strong (001) orientation. High-angle annular dark field scanning transmission electron microscopy with energy-dispersive x-ray spectroscopy demonstrated abrupt MnO/MgO interfaces and indicated [(001)MnO||(001)MgO] epitaxial growth. Ex situ atomic force microscopy of films deposited without RF excitation revealed smooth growth surfaces. An SMB-grown MnO(001) film was converted to Mn3O4 with strong (110) orientation by post-growth exposure to an RF-discharge (RFD) SMB source providing O atoms; the surface of the resultant film contained elongated pits aligned with the MgO110 directions. In contrast, using the RFD-SMB source for growth resulted in MnO(001) films with elongated growth pits and square pyramidal hillocks aligned along the MgO110 and 100 directions, respectively.
more »
« less
- Award ID(s):
- 2116724
- PAR ID:
- 10531657
- Publisher / Repository:
- AIP Publishing
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 160
- Issue:
- 15
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
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
-
In this work, we demonstrate the growth and phase stabilization of ultrawide bandgap polycrystalline rutile germanium dioxide (GeO2) thin films. GeO2 thin films were deposited using RF magnetron sputtering on r-plane sapphire (Al2O3) substrates. As-deposited films were x-ray amorphous. Postdeposition annealing was performed at temperatures between 650 and 950 °C in an oxygen or nitrogen ambient. Annealing at temperatures from 750 to 950 °C resulted in mixed-phase polycrystalline films containing tetragonal (rutile) GeO2, hexagonal (α-quartz) GeO2, and/or cubic (diamond) germanium (Ge). When nitrogen was used as the anneal ambient, mixed GeO2 phases were observed. In contrast, annealing in oxygen promoted stabilization of the r-GeO2 phase. Grazing angle x-ray diffraction showed a preferred orientation of (220) r-GeO2 for all crystallized films. The combination of O2 annealing and O2 flux during growth resulted in r-GeO2 films with highly preferential alignment. Using electron microscopy, we observed an interfacial layer of hexagonal-oriented GeO2 with epitaxial alignment to the (11¯02) Al2O3 substrate, which may help stabilize the top polycrystalline r-GeO2 film.more » « less
-
Background carbon incorporation and film cracking issue in (001) β-Ga2O3 films grown by metalorganic chemical vapor deposition (MOCVD) are investigated. Quantitative secondary ion mass spectrometry analysis shows that increasing the O2 flow rate significantly reduces carbon concentration, suggesting the importance of optimizing the VI/III ratio and growth temperature to achieve low compensation and controllable doping in MOCVD of (001) Ga2O3 films. MOCVD growth of (001) β-Ga2O3 films with a film thickness of 25 μm at a growth rate of 10 μm/h is achieved. However, film cracking remains a persistent challenge. Reducing the growth rate by adjusting the trimethylgallium (TMGa) flow rate or increasing chamber pressure effectively suppresses cracking, but it results in slower growth rates. In addition, lower growth temperature and high chamber pressure can help suppressing surface reconstruction and reduce the formation of cracking. Buffer layers grown at 850 °C, 100 Torr, and 58 μmol/min of TMGa significantly improve surface morphology of drift layers. Moreover, the use of AlGaO buffer layers with 8% of Al and a thickness of ∼130 nm leads to a lower crack density. X-ray rocking curve analysis confirms high crystalline quality at a growth rate of 10 μm/h, with no degradation observed from the introduction of an AlGaO buffer layer. These optimized growth conditions effectively improve surface smoothness and minimize defects. Results from this work provide fundamental insights in MOCVD epitaxy of β-Ga2O3 on (001) Ga2O3 substrates, revealing the opportunities and challenges of MOCVD (001) β-Ga2O3 thin films with fast growth rates for high-power electronic device technology.more » « less
-
We report the growth of nanoscale hafnium dioxide (HfO2) and zirconium dioxide (ZrO2) thin films using remote plasma-enhanced atomic layer deposition (PE-ALD), and the fabrication of complementary metal-oxide semiconductor (CMOS) integrated circuits using the HfO2 and ZrO2 thin films as the gate oxide. Tetrakis (dimethylamino) hafnium (Hf[N(CH3)2]4) and tetrakis (dimethylamino) zirconium (IV) (Zr[N(CH3)2]4) were used as the precursors, while O2 gas was used as the reactive gas. The PE-ALD-grown HfO2 and ZrO2 thin films were analyzed using X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and high-resolution transmission electron microscopy (HRTEM). The XPS measurements show that the ZrO2 film has the atomic concentrations of 34% Zr, 2% C, and 64% O while the HfO2 film has the atomic concentrations of 29% Hf, 11% C, and 60% O. The HRTEM and XRD measurements show both HfO2 and ZrO2 films have polycrystalline structures. n-channel and p-channel metal-oxide semiconductor field-effect transistors (nFETs and pFETs), CMOS inverters, and CMOS ring oscillators were fabricated to test the quality of the HfO2 and ZrO2 thin films as the gate oxide. Current-voltage (IV) curves, transfer characteristics, and oscillation waveforms were measured from the fabricated transistors, inverters, and oscillators, respectively. The experimental results measured from the HfO2 and ZrO2 thin films were compared.more » « less
An official website of the United States government

