By addressing precursor prevalence and energetics using the DFT-based synthetic growth concept (SGC), the formation mechanism of self-induced InAlN core–shell nanorods (NRs) synthesized by reactive magnetron sputter epitaxy (MSE) is explored. The characteristics of In- and Al-containing precursor species are evaluated considering the thermal conditions at a typical NR growth temperature of around 700 °C. The cohesive and dissociation energies of In-containing precursors are consistently lower than those of their Al-containing counterparts, indicating that In-containing precursors are more weakly bonded and more prone to dissociation. Therefore, In-containing species are expected to exhibit lower abundance in the NR growth environment. At increased growth temperatures, the depletion of In-based precursors is even more pronounced. A distinctive imbalance in the incorporation of Al- and In-containing precursor species (namely, AlN/AlN+, AlN2/AlN2+, Al2N2/Al2N2+, and Al2/Al2+ vs InN/InN+, InN2/InN2+, In2N2/In2N2+, and In2/In2+) is found at the growing edge of the NR side surfaces, which correlates well with the experimentally obtained core–shell structure as well as with the distinctive In-rich core and vice versa for the Al-rich shell. The performed modeling indicates that the formation of the core–shell structure is substantially driven by the precursors’ abundance and their preferential bonding onto the growing edge of the nanoclusters/islands initiated by phase separation from the beginning of the NR growth. The cohesive energies and the band gaps of the NRs show decreasing trends with an increment in the In concentration of the NRs’ core and with an increment in the overall thickness (diameter) of the NRs. These results reveal the energy and electronic reasons behind the limited growth (up to ∼25% of In atoms of all metal atoms, i.e., InxAl1–xN, x ∼ 0.25) in the NR core and may be qualitatively perceived as a limiting factor for the thickness of the grown NRs (typically <50 nm).
Indium segregation in a narrow InGaN single quantum well creates quantum dot (QD) like exciton localization centers. Cross-section transmission electron microscopy reveals varying shapes and lateral sizes in the range ∼1–5 nm of the QD-like features, while scanning near field optical microscopy demonstrates a highly inhomogeneous spatial distribution of optically active individual localization centers. Microphotoluminescence spectroscopy confirms the spectrally inhomogeneous distribution of localization centers, in which the exciton and the biexciton related emissions from single centers of varying geometry could be identified by means of excitation power dependencies. Interestingly, the biexciton binding energy (Ebxx) was found to vary from center to center, between 3 to −22 meV, in correlation with the exciton emission energy. Negative binding energies are only justified by a three-dimensional quantum confinement, which confirms QD-like properties of the localization centers. The observed energy correlation is proposed to be understood as variations of the lateral extension of the confinement potential, which would yield smaller values of Ebxx for reduced lateral extension and higher exciton emission energy. The proposed relation between lateral extension and Ebxx is further supported by the exciton and the biexciton recombination lifetimes of a single QD, which suggest a lateral extension of merely ∼3 nm for a QD with strongly negative Ebxx = −15.5 meV.
Zinc aluminogallate, Zn(AlxGa1−x)2O4 (ZAGO), a single-phase spinel structure, offers considerable potential for high-performance electronic devices due to its expansive compositional miscibility range between aluminum (Al) and gallium (Ga). Direct growth of high-quality ZAGO epilayers however remains problematic due to the high volatility of zinc (Zn). This work highlights a novel synthesis process for high-quality epitaxial quaternary ZAGO thin films on sapphire substrates, achieved through thermal annealing of a ZnGa2O4 (ZGO) epilayer on sapphire in an ambient air setting. In-situ annealing x-ray diffraction measurements show that the incorporation of Al in the ZGO epilayer commenced at 850 °C. The Al content (x) in ZAGO epilayer gradually increased up to around 0.45 as the annealing temperature was raised to 1100 °C, which was confirmed by transmission electron microscopy (TEM) and energy dispersive x-ray spectroscopy. X-ray rocking curve measurement revealed a small full width at half maximum value of 0.72 °, indicating the crystal quality preservation of the ZAGO epilayer with a high Al content. However, an epitaxial intermediate �–(AlxGa1−x)2O3 layer (� - AGO) was formed between the ZAGO and sapphire substrate. This is believed to be a consequence of the interdiffusion of Al and Ga between the ZGO thin film and sapphire substrate. Using density functional theory, the substitution cost of Ga in sapphire was determined to be about 0.5 eV lower than substitution cost of Al in ZGO. Motivated by this energetically favorable substitution, a formation mechanism of the ZAGO and AGO layers was proposed. Spectroscopic ellipsometry studies revealed an increase in total thickness of the film from 105.07 nm (ZGO) to 147.97 nm (ZAGO/AGO) after annealing to 1100 °C, which were corroborated using TEM. Furthermore, an observed increase in the direct (indirect) optical bandgap from 5.06 eV (4.7 eV) to 5.72 eV (5.45 eV) with an increasing Al content in the ZAGO layer further underpins the formation of a quaternary ZAGO alloy with a tunable composition.
Electronic grade ZnGa2O4 epitaxial thin films were grown on c-plane sapphire substrates by metal-organic chemical vapor deposition and investigated using spectroscopic ellipsometry. Their thickness, roughness and optical properties were determined using a Multiple Sample Analysis based approach by the regression analysis of optical model and measured data. These samples were then compared to samples which had undergone ion etching, and it was observed that etching time up to four minutes had no discernible impact on its optical properties. Line shape analysis of resulting absorption coefficient dispersion revealed that ZnGa(2)O(4 )exhibited both direct and indirect interband transitions. The modified Cody formalism was employed to determine their optical bandgaps. These values were found to be in good agreement with values obtained using other popular bandgap extrapolation procedures. Published by Optica Publishing Group under the terms of the Creative Commons Attribution 4.0 License. Further distribution of this work must maintain attribution to the author(s) and the published articles title, journal citation, and DOI.
Glancing angle deposition (GLAD) of AlN nanostructures was performed at room temperature by reactive magnetron sputtering in a mixed gas atmosphere of Ar and N-2. The growth behavior of nanostructures shows strong dependence on the total working pressure and angle of incoming flux. In GLAD configuration, the morphology changed from coalesced, vertical nanocolumns with faceted terminations to highly inclined, fan-like, layered nanostructures (up to 38 degrees); while column lengths decreased from around 1743 to 1068 nm with decreasing pressure from 10 to 1.5 mTorr, respectively. This indicates a change in the dominant growth mechanism from ambient flux dependent deposition to directional ballistic shadowing deposition with decreasing working pressures, which is associated with the change of energy and incident angle of incoming reactive species. These results were corroborated using simulation of metal transport (SiMTra) simulations performed at similar working pressures using Ar and N separately, which showed the average particle energy and average angle of incidence decreased while the total average scattering angle of the metal flux arriving at substrate increased with increasing working pressures. Observing the crystalline orientation of GLAD deposited wurtzite AlN nanocolumns using X-ray diffraction (XRD), pole-figure measurements revealedc-axis growth towards the direction of incoming flux and a transition from fiber-like to biaxial texture took place with increasing working pressures. Under normal deposition conditions, AlN layer morphology changed from {0001} to {10 (1) over bar1} with increasing working pressure because of kinetic energy-driven growth.
Photoconduction (PC) properties were investigated for ternary indium aluminium nitride (InxAl1-xN) nanorods (NRs) with different indium compositions (x) from 0.35 to 0.68, as grown by direct-current reactive magnetron sputter epitaxy. Cross-sectional scanning transmission electron microscopy (STEM) reveals single-crystal quality of the vertically aligned InxAl1-xN NRs. Single-rod photodetector devices with good ohmic contacts were fabricated using the focused-ion-beam technique (FIB), where the In-rich In0.68Al0.32N NR exhibits an optimal photocurrent responsivity of 1400 A W-1 and photoconductive gain of 3300. A transition from a positive photoresponse to a negative photoresponse was observed, while increasing the In composition x from 0.35 to 0.57. The negative PC was further enhanced by increasing x to 0.68. A model based on the coexistence and competition of deep electron trap states and recombination centers was proposed to explain the interesting composition-dependent PC in these ternary III-nitride 1D nanostructures.
Tritantalum pentanitride (Ta3N5) semiconductor is a promising material for photoelectrolysis of water with high efficiency. Ta3N5 is a metastable phase in the complex system of TaN binary compounds. Growing stabilized single-crystal Ta3N5 films is correspondingly challenging. Here, we demonstrate the growth of a nearly single-crystal Ta3N5 film with epitaxial domains on c-plane sapphire substrate, Al2O3(0001), by magnetron sputter epitaxy. Introduction of a small amount ~2% of O2 into the reactive sputtering gas mixed with N2 and Ar facilitates the formation of a Ta3N5 phase in the film dominated by metallic TaN. In addition, we indicate that a single-phase polycrystalline Ta3N5 film can be obtained with the assistance of a Ta2O5 seed layer. With controlling thickness of the seed layer smaller than 10 nm and annealing at 1000 °C, a crystalline β phase Ta2O5 was formed, which promotes the domain epitaxial growth of Ta3N5 films on Al2O3(0001). The mechanism behind the stabilization of the orthorhombic Ta3N5 structure resides in its stacking with the ultrathin seed layer of orthorhombic β-Ta2O5, which is energetically beneficial and reduces the lattice mismatch with the substrate.
Direct growth of orthorhombic Ta3N5-type Ta-O-N compound thin films, specifically Ta3-xN5-yOy, on Si and sapphire substrates with various atomic fractions is realized by unbalanced magnetron sputtering. Low-degree fiber-textural Ta3-xN5-yOy films were grown through reactive sputtering of Ta in a gas mixture of N-2, Ar, and O-2 with keeping a partial pressure ratio of 3:2:0.1 in a total working pressure range of 5-30 mTorr. With increasing total pressure from 5 to 30 mTorr, the atomic fraction of O in the as-grown Ta3-xN5-yOy films was found to increase from 0.02 to 0.15 while that of N and Ta decrease from 0.66 to 0.54 and 0.33 to 0.31, respectively, leading to a decrease in b lattice constant up to around 1.3%. Metallic TaNx phases were formed without oxygen. For a working pressure of 40 mTorr, an amorphous, O-rich Ta-N-O compound film with a high O fraction of similar to 0.48, was formed, mixed with non-stoichiometric TaON and Ta2O5. By analyzing the plasma discharge, the increasing O incorporation is associated with oxide formation on top of the Ta target due to a higher reactivity of Ta with O than with N. The increase of O incorporation in the films also leads to a optical bandgap widening from similar to 2.22 to similar to 2.96 eV, which is in agreement with the compositional and structural changes from a crystalline Ta3-xN5-yOy to an amorphous O-rich Ta-O-N compound.
Gallium nitride (GaN) epitaxial films on sapphire (Al2O3) substrates have been grown using reactive magnetron sputter epitaxy with a liquid Ga target. Threading dislocations density (TDD) of sputtered GaN films was reduced by using an inserted high-quality aluminum nitride (AlN) buffer layer grown by reactive high power impulse magnetron sputtering (R-HiPIMS) in a gas mixture of Ar and N2. After optimizing the Ar/N2 pressure ratio and deposition power, a high-quality AlN film exhibiting a narrow full-width at half-maximum (FWHM) value of the double-crystal x-ray rocking curve (DCXRC) of the AlN(0002) peak of 0.086° was obtained by R-HiPIMS. The mechanism giving rise the observed quality improvement is attributed to the enhancement of kinetic energy of the adatoms in the deposition process when operated in a transition mode. With the inserted HiPIMS-AlN as a buffer layer for direct current magnetron sputtering (DCMS) GaN growth, the FWHM values of GaN(0002) and (10 1‾ 1) XRC decrease from 0.321° to 0.087° and from 0.596° to 0.562°, compared to the direct growth of GaN on sapphire, respectively. An order of magnitude reduction from 2.7 × 109 cm−2 to 2.0 × 108 cm−2 of screw-type TDD calculated from the FWHM of the XRC data using the inserted HiPIMS-AlN buffer layer demonstrates the improvement of crystal quality of GaN. The result of TDD reduction using the HiPIMS-AlN buffer was also verified by weak beam dark-field (WBDF) cross-sectional transmission electron microscopy (TEM).
The electronic transport properties of the wide-bandgap aluminum indium nitride (AlInN) nanorods (NRs) grown by ultrahigh-vacuum magnetron sputter epitaxy (MSE) have been studied. The conductivities of the ternary compound nanostructure locates at the value of 15 Q-1 cm -1, which is respectively one and two orders of magnitude lower than the binary GaN and InN counterparts grown by chemical vapor deposition (CVD). The very shallow donor level/band with the activation energy at 11 + 2 meV was obtained by the temperature-dependent measurement. In addition, the photoconductivity has also been investigated. The photoconductive (PC) gain of the NRs device can reach near 2400 under a low bias at 0.1 V and the light intensity at 100W m-2 for ultraviolet response in vacuum. The power-insensitive gain and ambience-dependent photocurrent are also observed, which is attributed to the probable surfacecontrolled PC mechanism in this ternary nitride nanostructure.
We present a study on the role of dislocations and impurities for the unintentional n-type conductivity in high-quality InN grown by molecular beam epitaxy. The dislocation densities and H profiles in films with free electron concentrations in the low 10(17) cm(-1) and mid 10(18) cm(-3) range are measured, and analyzed in a comparative manner. It is shown that dislocations alone could not account for the free electron behavior in the InN films. On the other hand, large concentrations of H sufficient to explain, but exceeding substantially, the observed free electron densities are found. Furthermore, enhanced concentrations of H are revealed at the film surfaces, resembling the free electron behavior with surface electron accumulation. The low-conductive film was found to contain C and it is suggested that C passivates the H donors or acts as an acceptor, producing compensated material in this case. Therefore, it is concluded that the unintentional impurities play an important role for the unintentional n-type conductivity in InN. We suggest a scenario of H incorporation in InN that may reconcile the previously reported observations for the different role of impurities and dislocations for the unintentional n-type conductivity in InN.
Novel hybrid organic-inorganic nanostructures fabricated to utilize non-radiative resonant energy transfer mechanism are considered to be extremely attractive for a variety of light emitters for down converting of ultaviolet light and for photovoltaic applications since they can be much more efficient compared to devices grown with common design. Organic-inorganic hybrid structures based on green polyfluorene (F8BT) and GaN (0001) nanorods grown by magnetron sputtering on Si (111) substrates are studied. In such nanorods, stacking faults can form periodic polymorphic quantum wells characterized by bright luminescence. In difference to GaN exciton emission, the recombination rate for the stacking fault related emission increases in the presence of polyfluorene film, which can be understood in terms of Forster interaction mechanism. From comparison of dynamic properties of the stacking fault related luminescence in the hybrid structures and in the bare GaN nanorods, the pumping efficiency of non-radiative resonant energy transfer in hybrids was estimated to be as high as 35% at low temperatures.
Optical and structural properties are presented for GaN nanorods grown in the [0001]direction on Si(111) substrates by direct-current reactive magnetron sputter epitaxy.Transmission electron microscopy reveals clusters of dense stacking faults (SFs) regularlydistributed along the c-axis. A strong emission at ~3.42 eV associated with basal plane SFsdemonstrates thermal stability up to room temperatures together with a relatively shortrecombination time suggesting carrier localization in the system similar to multiple quantumwells.
The demand for highly sensitive and selective gas sensors has been steadily increasing, driven by applications in various fields such as environmental monitoring, healthcare, and industrial safety. In this context, ternary alloy indium aluminum nitride (InAlN) semiconductors have emerged as a promising material for gas sensing due to their unique properties and tunable material characteristics. This work focuses on the fabrication and characterization of InAlN nanorods grown on sapphire substrates using an ultra-high vacuum magnetron sputter epitaxy with precise control over indium composition and explores their potential for acetone-gas-sensing applications. Various characterization techniques, including XRD, SEM, and TEM, demonstrate the structural and morphological insights of InAlN nanorods, making them suitable for gas-sensing applications. To evaluate the gas-sensing performance of the InAlN nanorods, acetone was chosen as a target analyte due to its relevance in medical diagnostics and industrial processes. The results reveal that the InAlN nanorods exhibit a remarkable sensor response of 2.33% at 600 ppm acetone gas concentration at an operating temperature of 350 degrees C, with a rapid response time of 18 s. Their high sensor response and rapid response make InAlN a viable candidate for use in medical diagnostics, industrial safety, and environmental monitoring.
ZnGa2O4 epilayers have been grown on sapphire using the metalorganic chemical vapor deposition system. However, there is a trade-off between high conductivity and large defect density (oxygen vacancies) with the growth time of the growth of ZnGa2O4 epilayers. The ultraviolet (UV)-ozone treatment on the ZnGa2O4 epilayer at 100. C was proposed to reduce the number of oxygen vacancies in ZnGa2O4. The effect of UV-ozone treatment on the performance of ZnGa2O4 metal-semiconductor-metal (MSM) photodetector (PD) was evaluated. X-ray photoelectron spectroscopy analysis showed a decrease in the number of oxygen vacancies after UV-ozone treatment of ZnGa2O4. The measured lattice parameter near the surface around 10 nm of untreated ZnGa2O4 was 8.3434 +/- 0.0120 angstrom and increased slightly to 8.3775 +/- 0.0083 A. after UV-ozone treatment due to the decrease in oxygen vacancies. The dark current (at 5 V) of ZnGa2O4 PD was significantly reduced from 251 to 20.2 pA before and after UV-ozone treatment; it resulted in a substantial one-order enhancement in the on/off ratio of the PDs from 2.7 x 10(5) and 2.15 x 10(6) after the UV-ozone treatment. Furthermore, the rejection ratio also improved between 240 and 470 nm from 35 to 84 after UV-ozone treatment. The relationship between photocurrent and light intensity and the improvement in raising and falling time also showed the reduced density of trap states by UV-ozone treatment. This indicates that UV-ozone treatment can enhance the characteristics of ZnGa2O4 PDs for UV sensing applications.
We fabricated a gas sensor with a wide-bandgap ZnGa2O4 (ZGO) epilayer grown on a sapphire substrate by metalorganic chemical vapor deposition. The ZGO presented (111), (222) and (333) phases demonstrated by an X-ray diffraction system. The related material characteristics were also measured by scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy. This ZGO gas sensor was used to detect nitric oxide (NO) in the parts-per-billion range. In this study, the structure effect on the response of the NO gas sensor was studied by altering the sensor dimensions. Two approaches were adopted to prove the dimension effect on the sensing mechanism. In the first approach, the sensing area of the sensors was kept constant while both channel length (L) and width (W) were varied with designed dimensions (L x W) of 60 x 200, 80 x 150, and 120 x100 mu m(2). In the second, the dimensions of the sensing area were altered (60, 40, and 20 mu m) with W kept constant. The performance of the sensors was studied with varying gas concentrations in the range of 500 ppb similar to 10 ppm. The sensor with dimensions of 20 x 200 mu m(2) exhibited a high response of 11.647 in 10 ppm, and 1.05 in 10 ppb for NO gas. The sensor with a longer width and shorter channel length exhibited the best response. The sensing mechanism was provided to explain the above phenomena. Furthermore, the reaction between NO and the sensor surface was simulated by O exposure of the ZGO surface in air and calculated by first principles.
In this study, the Si-ions implantation technique with different doses from 1 x 1014 to 1 x 1015 cm-2 and dose energy 30, 40 and 50 keV was used to tune the electrical properties in unintentionally doped (UID) 8-Ga2O3 epilayers grown on the sapphire substrates by metalorganic chemical vapor deposition (MOCVD). A high quality UID 8-Ga2O3 epilayers were fabricated using the optimized growth parameters of MOCVD. The UID and Si-ions implanted 8-Ga2O3 epilayers were examined and results were compared with the help of X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy. Si-ions implantation parameters were also simulated by stopping and range of ions in matter software (SRIM) and actual Si-ions concentration was measured by secondary ions mass spectroscopy. The electrical properties of the implanted 8-Ga2O3 epilayers were measured by transmission length method and Hall measurements. The sheet resistivity for the 8-Ga2O3epilayers with Si-ion dose of 1 x 1014, 6 x 1014 and 1 x 1015 cm-2 were found as 2.047, 0.158 and 0.144 Cd cm, respectively measured by Hall measurements and the electron carrier concentrations for the above doses were 4.39 x 1018, 6.86 x 1018 and 7.98 x 1019 cm-3. From the above results, the ion implantation was demonstrated to effectively reduce the resistivity with the high carrier concentrations.
In this study, monoclinic gallium oxide (beta-Ga2O3) epilayer was successfully grown on c-plane, (0001), sapphire substrate by metalorganic chemical vapor deposition (MOCVD) with interplaying growth temperature, TEGa flow rate, and growth time. X-ray diffraction 20 scans show only three narrow diffraction peaks referred to beta-Ga2O3 ((2) over bar 01), ((4) over bar 02), and ((6) over bar 03) in all epilayers, indicating a superior crystalline quality. Current-voltage (I-V) measurement reveals that these beta-Ga2O3 films are insulating and exhibit high resistance in a range of 10(12)-10(14) Omega. The crystallization characteristics of the epilayers can be effectively improved with thickness through increasing TEGa flow rate and growth time, which was evidenced by X-ray rocking curves and I-V measurements. However, the surface roughness of beta-Ga2O3 film increases with growth time and TEGa flow rate. When the growth temperature increases above 825 degrees C, the thickness of beta-Ga2O3 film decreases clearly. Furthermore, it can be found that the growth rate decreased as the growth time increasing. The growth mechanism based on first-principles calculation was proposed as that 3D growth induced by the lattice mismatch between beta-Ga2O3 and sapphire starts at nucleation stage, and follows up a lateral growth promoting a 2D growth after the thick epilayer being grown. In addition, the complex chemical reaction between TEGa and oxygen precursors was unraveled by density function theory calculation. (c) 2022 Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http:// creativecommons.org/licenses/by-nc-nd/4.0/).
Chirality, tailored by external morphology and internal composition, has been realized by controlled curved-lattice epitaxial growth (CLEG) of uniform coatings of single-crystalline InxAl1-xN nanospirals. The nanospirals are formed by sequentially stacking segments of curved nanorods on top of each other, where each segment is incrementally rotated around the spiral axis. By controlling the growth rate, segment length, rotation direction, and incremental rotation angle, spirals are tailored to predetermined handedness, pitch, and height. The curved morphology of the segments is a result of a lateral compositional gradient across the segments while maintaining a preferred crystallographic growth direction, implying a lateral gradient in optical properties as well. Left- and right-handed nanospirals, tailored with 5 periods of 200 nm pitch, as confirmed by scanning electron microscopy, exhibit uniform spiral diameters of ~80 nm (local segment diameters of ~60 nm) with tapered hexagonal tips. High resolution electron microscopy, in combination with nanoprobe energy dispersive X-ray spectroscopy and valence electron energy loss spectroscopy, show that individual nanospirals consist of an In-rich core with ~15 nm-diameter hexagonal cross-section, comprised of curved basal planes. The core is surrounded by an Al-rich shell with a thickness asymmetry spiraling along the core. The ensemble nanospirals, across the 1 cm2 wafers, show high in-plane ordering with respect to shape, crystalline orientation, and direction of compositional gradient. Mueller matrix spectroscopic ellipsometry shows that the tailored chirality is manifested in the polarization state of light reflected off the CLEG nanospiral-coated wafers. In that, the polarization state is shown to be dependent on the handedness of the nanospirals and the wavelength of the incident light in the ultraviolet-visible region.
Despite of using chiral metamaterials to manipulate light polarization states has been demonstrated their great potential for applications such as invisible cloaks, broadband or wavelength-tunable circular polarizers, microreflectors, etc. in the past decade [1-6], operating wavelength in ultraviolet-visible range is still a challenge issue. Since these chiral structures often consist of metallic materials, their operation is designed for the infrared and microwave regions [2-4]. Here, we show how a controlled curved-lattice epitaxial growth (CLEG) of wide-bandgap AlInN semiconductor curved nanocrystals [7] can be exploited as a novel route for tailoring chiral nanostructures in the form of twisted nanorods (TNRs). The fabricated TNRs are shown to reflect light with a high degree of polarization as well as a high degree of circular polarization (that is, nearly circularly polarized light) in the ultravioletvisible region. The obtained polarization is shown to be dependent on the handedness of the TNRs.
Self-assembled ternary Al1-xInxN nanorod arrays with variable In concentration, 0.10 ≤ x ≤ 0.32 have been realized onto c-plane sapphire substrates by ultra-high-vacuum magnetron sputter epitaxy with Ti0.21Zr0.79N or VN seed layers assistance. The formation of nanorods was very sensitive to the applied seed layer. Without proper seed layer assistance a continuous Al1-xInxN film was grown. The nanorods exhibit hexagonal crosssections with preferential growth along the c axis. A coaxial rod structure with higher In concentration in the core was observed by (scanning) transmission electron microscopy in combination with low-loss electron energy loss spectroscopy and energy dispersive xray spectroscopy. 5 K cathodoluminescence spectroscopy of Al0.86In0.14N nanorods revealed band edge emission at ~5.46 eV, which was accompanied by a strong defectrelated emission at ~ 3.38 eV.
Al1-xInxN heteroepitaxial layers covering the full composition range have been realized by magnetron sputter epitaxy on basal-plane AlN, GaN, and ZnO templates at room temperature (RT). Both Al1-xInxN single layers and multilayers grown on these isostructural templates show single phase, single crystal wurtzite structure. Even at large lattice mismatch between the film and the template, for instance InN/AlN (similar to 13% mismatch), heteroepitaxy is achieved. However, RT-grown Al1-xInxN films directly deposited on non-isostructural c-plane sapphire substrate exhibit a polycrystalline structure for all compositions, suggesting that substrate surface structure is important for guiding the initial nucleation. Degradation of Al1-xInxN structural quality with increasing indium content is attributed to the formation of more point-and structural defects. The defects result in a prominent hydrostatic tensile stress component, in addition to the biaxial stress component introduced by lattice mismatch, in all RT-grown Al1-xInxN films. These effects are reflected in the measured in-plane and out-of-plane strains. The effect of hydrostatic stress is negligible compared to the effects of lattice mismatch in high-temperature grown AlN layers thanks to their low amount of defects. We found that Vegards rule is applicable to determine x in the RT-grown Al1-xInxN epilayers if the lattice constants of RT-sputtered AlN and InN films are used instead of those of the strain-free bulk materials.
The spontaneous formation of AlInN core–shell nanorod arrays with variable In concentration has been realized by ultrahigh-vacuum magnetron sputter epitaxy with Ti0.21Zr0.79N or VN seed layer assistance. The nanorods exhibit hexagonal cross sections with preferential growth along the c-axis. A core–shell rod structure with a higher In concentration in the core was observed by (scanning) transmission electron microscopy in combination with low-loss electron energy loss spectroscopy and energy dispersive X-ray spectroscopy. 5 K cathodoluminescence spectroscopy of Al0.86In0.14N nanorods revealed band edge emission at ∼5.46 eV, which was accompanied by a strong defect-related emission at ∼3.38 eV
Nucleation of self-induced nanorod and core-shell structure formation by surface-induced phase separation have been studied at the initial growth stage. The growth of well-separated core shell nanorods is only found in a transition temperature region (600 degrees C amp;lt;= T amp;lt;= 800 degrees C) in contrast to the result of thin film growth outside this region (T amp;lt; 600 degrees C or T amp;gt; 800 degrees C). Formation of multiple compositional domains, due to phase separation, after similar to 20 nm InxAl1-xN epilayer growth from sapphire substrate promotes the core-shell nanorod growth, showing a modified Stranski-Krastanov growth mode. The use of VN seed layer makes the initial growth of the nanorods directly at the substrate interface, revealing a Volmer-Weber growth mode. Different compositional domains are found on VN template surface to support that the phase separation takes place at the initial nucleation process and forms by a self-patterning effect. The nanorods were grown from In-rich domains and initiated the formation of core-shell nanorods due to spinodal decomposition of the InxAl1-xN alloy with a composition in the miscibility gap.
Gallium oxide (Ga2O3) has especially become popular because of its established applications in semiconductors. Of five polymorphs, monoclinic beta-Ga2O3 is the most thermodynamically stable phase. However, orthorhombic Ga2O3 (also known as epsilon-Ga2O3 or kappa-Ga2O3) is gaining increasing interest due to its high lattice symmetry and peculiar ferroelectricity. Although the structural approach for estimating Ga2O3 has been studied both theoretically and experimentally, epsilon-Ga2O3 and kappa-Ga2O3 are still confused. In this study, epsilon-Ga2O3 epilayers are grown on c-plane sapphire by metal-organic chemical vapor deposition with a multistep growth process. A thin annealed epsilon-Ga2O3 buffer layer is grown in the first step. The sequent growth steps with slow, fast, or combination of slow then fast growth rate significantly influence the quality of epilayers compared with that of directly grown Ga2O3. Through a detailed transmission electron microscopy (TEM) characterization of these Ga2O3 epilayers, the structural relationship between orthorhombic kappa-Ga2O3 and hexagonal epsilon-Ga2O3 is elucidated. A series of first-principles density functional theory calculations are also carried out to confirm the argument.
GaN nanorods, essentially free from crystal defects and exhibiting very sharp band-edge luminescence, have been grown by reactive direct-current magnetron sputter epitaxy onto Si (111) substrates at a low working pressure of 5 mTorr. Upon diluting the reactive N2 working gas with a small amount of Ar (0.5 mTorr), we observed an increase in the nanorod aspect ratio from 8 to ~35, a decrease in the average diameter from 74 to 35 nm, and a two-fold increase in nanorod density. With further dilution (Ar = 2.5 mTorr), the aspect ratio decreased to 14, while the diameter increased to 60 nm and the nanorod density increased to a maximum of 2.4 × 109 cm−2. Yet, lower N2 partial pressures eventually led to the growth of continuous GaN films. The observed morphological dependence on N2 partial pressure is explained by a change from N-rich to Ga-rich growth conditions, combined with reduced GaN-poisoning of the Ga-target as the N2 gas pressure is reduced. Nanorods grown at 2.5 mTorr N2 partial pressure exhibited a high intensity 4 K photoluminescence neutral donor bound exciton transitions (D0XA) peak at ~3.479 eV with a full-width-at-half-maximum of 1.7 meV. High-resolution transmission electron microscopy corroborated the excellent crystalline quality of the nanorods.
Electronic-grade GaN (0001) epilayers have been grown directly on Al2O3 (0001) substrates by reactive DC-magnetron sputter epitaxy (MSE) from a liquid Ga sputtering target in an Ar/N2 atmosphere. The as-grown GaN epitaxial film exhibit low threading dislocation density on the order of ≤ 1010 cm-2 obtained by transmission electron microscopy and modified Williamson-Hall plot. X-ray rocking curve shows narrow fullwidth at half maximum (FWHM) of 1054 arcsec of the 0002 reflection. A sharp 4 K photoluminescence peak at 3.474 eV with a FWHM of 6.3 meV is attributed to intrinsic GaN band edge emission. The high structural and optical qualities indicate that MSEgrown GaN epilayers can be used for fabricating high-performance devices without the need of any buffer layer.
Epitaxial GaN (0001) thin films were grown on Al2O3 (0001) substrates by reactive high power impulse magnetron sputtering of liquid Ga targets in a mixed N2/Ar discharge. A combination of x-ray diffraction, electron microscopy, atomic force microscopy, μ-Raman mapping and spectroscopy, μ-photoluminescence, time of flight elastic recoil detection, and cathodoluminescence showed the formation of relaxed and strained domains in the same films. While the strained domains form due to ion bombardment during growth, the relaxed domains exhibit
The Mueller matrix elements mij representing the polarization response from a nanostructured materialis determined by the constituent materials optical properties and the superstructure. Here, we investigate how chiral structures in form of helicoidally stacked uniaxial layers determine mij as a functionof polarization state, wavelength, incidence angle and azimuthal angle of the incoming light. The studied parameters include the layer materials ordinary/extraordinary optical properties, Euler angle values, and layer thickness as well as the thickness and pitch of the helicoidal superstructure. Sub- and superstructure inhomogeneity is also introduced. From the Fresnel-based calculations, mij aswell as the degree of polarization, ellipticity and azimuth of the polarization ellipse are obtained and presented as contour and trace plots to give a complete view of the polarization behavior. The results from the calculations are compared with Mueller matrix spectroscopic ellipsometry measurements of both natural and synthesized helicoidal structures. The measurements were performed with a dualrotating compensator system (RC2, J.A. Woollam Co., Inc.) for wavelengths in the range from 245 to 1000 nm and incident angles from 20 to 75°. For some measurements the azimuthal angle of the incident light was varied. The investigated natural chiral structures were exoskeletons from several beetles in the scarab subfamilies Cetoniinae and Rutelinae. As predicted from the calculations it isobserved that the reflection from these beetles can have a high degree of polarization and high ellipticity (near-circular polarization). Both left- and right-polarization was observed. The synthesized structures are helicoidal nanorods of Al1−xInxN grown on sapphire substrates with metal-nitride seedlayers using UHV magnetron sputtering. Due to an internal composition gradient (a variation of x) in the crystalline structure, the nanorods will tilt away from the substrate normal. Helicoidal structures can thus be obtained by rotating the substrate around its normal during deposition. Samples with different pitch and layer thickness with right-handed as well as left-handed chirality were grown. Also for these structures both left and right near-circular polarized light is observed. By combining calculations, ellipsometry measurements and scanning electron microscopy characterization we get agood input to build layered models of the natural and synthetic samples. After regression fitting agood agreement between calculated and measured optical data were obtained.
The influence of structural configurations of indium aluminum nitride (InA1N) nanospirals, grown by reactive magnetron sputter epitaxy, on the transformation of light polarization are investigated in terms of varying structural chirality, growth temperatures, titanium nitride (TiN) seed (buffer) layer thickness, nanospiral thickness, and pitch. The handedness of reflected circularly polarized light in the ultraviolet-visible region corresponding to the chirality of nanospirals is demonstrated. A high degree of circular polarization (P-c) value of 0.75 is obtained from a sample consisting of 1.2 mu m InA1N nanospirals grown at 650 degrees C. A film-like structure is formed at temperatures lower than 450 degrees C. At growth temperatures higher than 750 degrees C, less than 0.1 In-content is incorporated into the InA1N nanospirals. Both cases reveal very low P-c-A red shift of wavelength at P-c peak is found with increasing nanospiral pitch in the range of 200-300 nm. The P-c decreases to 0.37 for two-turn nanospirals with total length of 0.7 mu m, attributed to insufficient constructive interference. A branch-like structure appears on the surface when the nanospirals are grown longer than 1.2 mu m, which yields a low P-c around 0.5, caused by the excessive scattering of incident light.
The phase evolution of reactive radio frequency (RF) magnetron sputtered Cr0.28Zr0.10O0.61 coatings has been studied by in situ synchrotron X-ray diffraction during annealing under air atmosphere and vacuum. The annealing in vacuum shows t-ZrO2 formation starting at similar to 750-800 degrees C, followed by decomposition of the alpha-Cr2O3 structure in conjunction with bcc-Cr formation, starting at similar to 950 degrees C. The resulting coating after annealing to 1140 degrees C is a mixture of t-ZrO2, m-ZrO2, and bcc-Cr. The air-annealed sample shows t-ZrO2 formation starting at similar to 750 degrees C. The resulting coating after annealing to 975 degrees C is a mixture of t-ZrO2 and alpha-Cr2O3 (with dissolved Zr). The microstructure coarsened slightly during annealing, but the mechanical properties are maintained, with no detectable bcc-Cr formation. A larger t-ZrO2 fraction compared with alpha-Cr2O3 is observed in the vacuum-annealed coating compared with the air-annealed coating at 975 degrees C. The results indicate that the studied pseudo-binary oxide is more stable in air atmosphere than in vacuum.
A free-standing high-output power density polymeric thermoelectric (TE) device is realized based on a highly conductive (approximate to 2500 S cm(-1)) structure-ordered poly(3,4-ethylenedioxythiophene):polystyrene sulfonate film (denoted as FS-PEDOT:PSS) with a Seebeck coefficient of 20.6 mu V K-1, an in-plane thermal conductivity of 0.64 W m(-1) K-1, and a peak power factor of 107 mu W K-2 m(-1) at room temperature. Under a small temperature gradient of 29 K, the TE device demonstrates a maximum output power density of 99 +/- 18.7 mu W cm(-2), which is the highest value achieved in pristine PEDOT:PSS based TE devices. In addition, a fivefold output power is demonstrated by series connecting five devices into a flexible thermoelectric module. The simplicity of assembling the films into flexible thermoelectric modules, the low out-of-plane thermal conductivity of 0.27 W m(-1) K-1, and free-standing feature indicates the potential to integrate the FS-PEDOT:PSS TE modules with textiles to power wearable electronics by harvesting human bodys heat. In addition to the high power factor, the high thermal stability of the FS-PEDOT:PSS films up to 250 degrees C is confirmed by in situ temperature-dependent X-ray diffraction and grazing incident wide angle X-ray scattering, which makes the FS-PEDOT:PSS films promising candidates for thermoelectric applications.
beta-Ga2O3 thin films with both a 45 nm Si-doped conductive epilayer and unintentionally doped epilayer were grown on c-plane sapphire substrate by metalorganic chemical vapor deposition. beta-Ga2O3 based metal-oxide-semiconductor field-effect transistors (MOSFETs) were fabricated with gate recess depths of 20 nm and 40 nm (it indicated gate depth with 70 nm and 50 nm, respective), respectively, and without said recessing process. The conductivity of beta-Ga2O3 epilayers was improved through low in situ doping using a tetraethoxysilane precursor to increase MOSFET forward current density. After recessing, MOSFET operation was transferred from depletion to enhanced mode. In this study, the maximum breakdown voltage of the recessed 40 nm transistor was 770 V. The etching depth of a recessed-gate device demonstrates its influence on device electrical performance.
The scarab beetle Cetonia aurata is known to reflect light with brilliant colors and a high degree of circular polarization. Both color and polarization effects originate from the beetles exoskeleton and have been attributed to a Bragg reflection of the incident light due to a twisted laminar structure. Our strategy for mimicking the optical properties of the Cetonia aurata was therefore to design and fabricate transparent, chiral films. A series of films with tailored transparent structures of helicoidal InxAl1-xN nanorods were grown on sapphire substrates using UHV magnetron sputtering. The value of x is tailored to gradually decrease from one side to the other in each nanorod normal to its growth direction. This introduces an in-plane anisotropy with different refractive indices in the direction of the gradient and perpendicular to it. By rotating the sample during film growth the in-plane optical axis will be rotated from bottom to top and thereby creating a chiral film. Based on Muellermatrix ellipsometry, optical modeling has been done suggesting that both the exoskeleton of Cetonia aurata and our artificial material can be modeled by an anisotropic film made up of a stack of thin layers, each one with its in-plane optical axis slightly rotated with respect to the previous layer. Simulations based on the optical modeling were used to investigate how pitch and thickness of the film together with the optical properties of the constitutive materials affects the width and spectral position of the Bragg reflection band.
Metamaterials in the form of chiral nanostructures have shown great potential for applications such as chemical and biochemical sensors and broadband or wavelength tunable circular polarizers. Here we demonstrate a method to produce tailored transparent chiral nanostructures with the wide-bandgap semiconductor AlxIn1 − xN. A series of anisotropic and transparent films of AlxIn1 − xN were produced using curved-lattice epitaxial growth on metallic buffer layers. By controlling the sample orientation during dual magnetron sputter deposition, nanospirals with right-handed or left-handed chirality were produced. Using a dual rotating compensator ellipsometer in reflection mode, the full Mueller matrix was measured in the spectral range 245–1700 nm at multiple angles of incidence. The samples were rotated one full turn around their normal during measurements to provide a complete description of the polarization properties in all directions. For certain wavelengths, unpolarized light reflected off these films becomes highly polarized with a polarization state close to circular. Nanostructured films with right- and left-handed chirality produce reflections with right- and left-handed near-circularly polarized light, respectively. A model with a biaxial layer in which the optical axes are rotated from bottom to top was fitted to the Mueller-matrix data. Hence we can perform non-destructive structural analysis of the complex thin layers and confirm the tailored structure. In addition, the refractive index, modeled with a biaxial Cauchy dispersion model, is obtained for the AlxIn1 − xN films.
Optical properties of chiral nanostructured films made of Al1-xInxN using a new growth mechanism - curved-lattice epitaxial growth - are reported. Using this technique, chiral films with right- and left-handed nanospirals were produced. The chiral properties of the films, originating mainly from an internal anisotropy and to a lesser extent from the external helical shape of the nanospirals, give rise to selective reflection of circular polarization which makes them useful as narrow-band near-circular polarization reflectors. The chiral nanostructured films reflect light with high degree of circular polarization in the ultraviolet part of the spectrum with left- and right-handedness depending on the handedness of the nanostructures in the films.
Direct current magnetron sputter epitaxy with a liquid Ga sputtering target hasbeen used to grow single-crystal GaN(0001) nanorods directly on Si(111)substrates at different working pressures ranging from 5 to 20 mTorr of pure N2,.The as-grown GaN nanorods exhibit very good crystal quality from bottom to topwithout stacking faults, as determined by transmission electron microscopy. Thecrystal quality is found to increase with increasing working pressure. X-raydiffraction results show that all the rods are highly (0001)-oriented. Thenanorods exhibit an N-polarity, as determined by convergent beam electrondiffraction methods. Sharp and well-resolved 4 K photoluminescence peaks at ~3.474 eV with a FWHM ranging from 1.7 meV to 35 meV are attributed to theintrinsic GaN band edge emission and corroborate the superior structuralproperties of the material. Texture measurements reveal that the rods haverandom in-plane orientation when grown on Si(111) with native oxide, while theyhave an in-plane epitaxial relationship of GaN[110] // Si[110] when grown onsubstrates without surface oxide.
We study the effect of high power pulses in reactive magnetron sputter epitaxy on the structural properties of GaN (0001) thin films grown directly on Al2O3 (0001) substrates. The epilayers are grown by sputtering from a liquid Ga target, using a high power impulse magnetron sputtering power supply in a mixed N2/Ar discharge. X-ray diffraction, micro-Raman, micro-photoluminescence, and transmission electron microscopy investigations show the formation of two distinct types of domains. One almost fully relaxed domain exhibits superior structural and optical properties as evidenced by rocking curves with a full width at half maximum of 885 arc sec and a low temperature band edge luminescence at 3.47 eV with the full width at half maximum of 10 meV. The other domain exhibits a 14 times higher isotropic strain component, which is due to the higher densities of the point and extended defects, resulting from the ion bombardment during growth. Voids form at the domain boundaries. Mechanisms for the formation of differently strained domains, along with voids during the epitaxial growth of GaN are discussed.
We study the real time stress evolution, by in-situ curvature measurements, during magnetron sputter epitaxy of GaN (0001) epilayers at different growth temperatures, directly on Al2O3 (0001) substrates. The epilayers are grown by sputtering from a liquid Ga target in a mixed N2/Ar discharge. For 600 °C, a tensile biaxial stress evolution is observed, while for 700 °C and 800 °C, compressive stress evolutions are observed. Structural characterization by crosssectional transmission electron microscopy, and atomic force microscopy revealed that films grew at 700 °C and 800 °C in a layer-by-layer mode while a growth temperature of 600 °C led to an island growth mode. High resolution Xray diffraction data showed that edge and screw threading dislocation densities decreased with increasing growth temperature with a total density of 5.5×1010 cm-2. The observed stress evolution and growth modes are explained by a high adatom mobility during magnetron sputter epitaxy at 700 - 800 °C. Also other possible reasons for the different stress evolutions are discussed.
The thermal stability and spinodal decomposition of thin Al0.3In0.7N layers was studied in-situ by scanning transmission electron microscopy following annealing in a temperature range from 700 oC to 900 oC. The results show that for increasing layer thicknesses (from ~4 nm to ~22 nm) surface directed spinodal decomposition is initiated at Al0.3In0.7N/AlN interfaces and columnar boundaries in the Al0.3In0.7N layers. In the thin layers (~10 nm) annealing caused a single composition layer to split into doubly modulated layers with a compositional undulation perpendicular to the interfaces, while for the thicker layers (~22 nm) the spinodally decomposed structure is more random.
The thermal stability of Al1−xInxN (0 ⩽ x ⩽ 1) layers was investigated by scanning transmission electron microscopy (STEM) imaging, electron diffraction, and monochromated valence electron energy loss spectroscopy during in situ annealing from 750 to 950 °C. The results show two distinct decomposition paths for the layers richest in In (Al0.28In0.72N and Al0.41In0.59N) that independently lead to transformation of the layers into an In-deficient, nanocrystalline and a porous structure. The In-richest layer (Al0.28In0.72N) decomposes at 750 °C, where the decomposition process is initiated by In forming at grain boundaries and is characterized by an activation energy of 0.62 eV. The loss of In from the Al0.41In0.59N layer was initiated at 800 °C through continuous desorption. No In clusters were observed during this decomposition process, which is characterized by an activation energy of 1.95 eV. Finally, layers richest in Al (Al0.82In0.18N and Al0.71In0.29N) were found to resist thermal annealing, although the initial stages of decomposition were observed for the Al0.71In0.29N layer.
We have examined the early stages of self-induced InAlN core-shell nanorod (NR) formation processes on amorphous carbon substrates in plan-view geometry by means of transmission electron microscopy methods. The results show that the grown structure phase separates during the initial moments of deposition into a majority of Al-rich InAlN and a minority of In-enriched InAlN islands. The islands possess polygonal shapes and are mainly oriented along a crystallographic c-axis. The growth proceeds with densification and coalescence of the In-enriched islands, resulting in a base for the In-enriched NR cores with shape transformation to hexagonal. The Al-rich shell formation around such early cores is observed at this stage. The matured core-shell structure grows axially and radially, eventually reaching a steady growth state which is dominated by the axial NR growth. We discuss the NR formation mechanism by considering the adatom surface kinetics, island surface energy, phase separation of InAlN alloys, and incoming flux directions during dual magnetron sputter epitaxy.
The spinodal decomposition and thermal stability of thin In0.72Al0.28N layers and In0.72Al0.28N/AlN superlattices with AlN(0001) templates on Al2O3(0001) substrates was investigated by in-situ heating up to 900 degrees C. The thermally activated structural and chemical evolution was investigated in both plan-view and cross-sectional geometries by scanning transmission electron microscopy in combination with valence electron energy loss spectroscopy. The plan-view observations demonstrate evidence for spinodal decomposition of metastable In0.72Al0.28N after heating at 600 degrees C for 1 h. During heating compositional modulations in the range of 2-3 nm-size domains are formed, which coarsen with applied thermal budgets. Cross-sectional observations reveal that spinodal decomposition begin at interfaces and column boundaries, indicating that the spinodal decomposition has a surface-directed component.
Low-loss EELS was used to acquire information about the strain state in group III-nitrides. Experimental and theoretical simulation results show that the bulk plasmon peak position varies near linearly with unit cell volume variations due to strain. A unit cell volume change of 1% results in a bulk plasmon peak shift of 0.159 eV, 0.168 eV, and 0.079 eV for AlN, GaN, and InN, respectively, according to simulations. The AlN peak shift was experimentally corroborated with a peak shift of 0.156 eV, where the applied strain caused a 1% volume change. It is also found that while the bulk plasmon energy can be used as a measure of the composition in a III-nitride alloy for relaxed structures, the presence of strain significantly affects such a measurement. The strain has a lower impact on the peak shift for Al(1-x)InxN (3% compositional error per 1 % volume change) and In(1-x)GaxN alloys compared to significant variations for Al(1-x)GaxN (16% compositional error for 1% volume change). Hence low-loss studies off III-nitrides, particularly for confined structures, must be undertaken with care and understanding.
We demonstrate a standard-free method to retrieve compositional information in Alx In1–xN thin films by measuring the bulk plasmon energy (Ep), employing electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM). Two series of samples were grown by magnetron sputter epitaxy (MSE) and metal organic vapor phase epitaxy (MOVPE), which together cover the full com- positional range 0 ≤ x ≤ 1. Complementary compositional measurements were obtained using Rutherford backscattering spectroscopy (RBS) and the lattice parameters were obtained by X-ray diffraction (XRD). It is shown that Ep follows a linear relation with respect to composition and lattice parameter between the alloying elements from AlN to InN allowing for straightforward compositional analysis.
Currently, self-induced InAlN core-shell nanorods enjoy an advanced stage of accumulation of experimental data from their growth and characterization as well as a comprehensive understanding of their formation mechanism by the ab initio modeling based on Synthetic Growth Concept. However, their electronic and optical properties, on which most of their foreseen applications are expected to depend, have not been investigated comprehensively. GW and the Bethe-Salpeter equation (BSE) are regarded as the state-of-the-art ab initio methodologies to study these properties. However, one of the major drawbacks of these methods is the computational cost, much higher than density-functional theory (DFT). Therefore, in many applications, it is highly desirable to answer the question of how well approaches based on DFT, such as e.g. the local density approximation (LDA), LDA-1/2, the modified Becke-Johnson (mBJ) and the Heyd-Scuseria-Ernzerhof (HSE06) functionals, can be employed to calculate electronic and optical properties with reasonable accuracy. In the present paper, we address this question, investigating how effective the DFT-based methodologies LDA, LDA-1/2, mBJ and HSE06 can be used as approximate tools in studies of the electronic and optical properties of scaled down models of core-shell InAlN nanorods, thus, avoiding GW and BSE calculations.
Magnetron sputter epitaxy (MSE) is a promising processing route for group-III nitride semiconductors, with the potential to enable high-quality and low cost GaN growth for widespread use. However, fundamental techno-logical hurdles must be overcome to enable the adoption of MSE in industrial production. Here, we present a new UHV-compatible magnetron design with high-performance cooling, enabling high GaN growth rates at high growth temperatures using a solid Ga target. The magnetron is tested with a wide range of process parameters and a stable process is feasible while maintaining the solid state of the Ga target. High GaN growth rates of up to 5 mu m/h are achieved at room temperature and a growth rate of 4 mu m/h at high temperature, which is one order of magnitude higher compared to MSE with a liquid target. We grow GaN on c-plane sapphire substrates and show the impact of partial pressure ratio and target-to-substrate distance (TSD) on growth rate, film morphology and crystal quality of GaN films with scanning electron microscopy and X-ray diffraction. While the growth rate and film morphology are strongly impacted by the process parameter variation, the crystal quality is further impacted by the overall film thickness. For a 2 mu m thick GaN film a full width at half maximum of X-ray rocking curve (omega-FWHM) of GaN 10 1 1 reflection of 0.32 degrees is achieved. We demonstrate a process window for growth of dense and smooth GaN films with high crystal quality using low N2 flow rates and high TSD. By introducing a 20 nm AlN nucleation layer prior to the growth of 390 nm GaN, the omega-FWHM of GaN 0002 reflection of 0.19 degrees is achieved. The epitaxially grown crystalline structure is precisely examined by transmission electron microscopy.
Linear polarization properties of light emission are presented for GaN nanorods (NRs) grown along [0001] direction on Si(111) substrates by direct-current magnetron sputter epitaxy. The near band gap photoluminescence (PL) measured at low temperature for a single NR demonstrated an excitonic line at similar to 3.48 eV and the stacking faults (SFs) related transition at similar to 3.43 eV. The SF related emission is linear polarized in direction perpendicular to the NR growth axis in contrast to a non-polarized excitonic PL. The results are explained in the frame of the model describing basal plane SFs as polymorphic heterostructure of type II, where anisotropy of chemical bonds at the interfaces between zinc blende and wurtzite GaN subjected to in-built electric field is responsible for linear polarization parallel to the interface planes. (C) 2017 Author(s).
Magnetron sputter epitaxy (MSE) offers several advantages compared to alternative GaN epitaxy growth methods, including mature sputtering technology, the possibility for very large area deposition, and low-temperature growth of high-quality electronic-grade GaN. In this article, we review the basics of reactive sputtering for MSE growth of GaN using a liquid Ga target. Various target biasing schemes are discussed, including direct current (DC), radio frequency (RF), pulsed DC, and high-power impulse magnetron sputtering (HiPIMS). Examples are given for MSE-grown GaN thin films with material quality comparable to those grown using alternative methods such as molecular-beam epitaxy (MBE), metal-organic chemical vapor deposition (MOCVD), and hydride vapor phase epitaxy (HVPE). In addition, successful GaN doping and the fabrication of practical devices have been demonstrated. Beyond the planar thin film form, MSE-grown GaN nanorods have also been demonstrated through self-assembled and selective area growth (SAG) method. With better understanding in process physics and improvements in material quality, MSE is expected to become an important technology for the growth of GaN.
We demonstrate the versatility of magnetron sputter epitaxy by achieving high-quality GaN nanorods on different substrate/template combinations, specifically Si, SiC, TiN/Si, ZrB2/Si, ZrB2/SiC, Mo, and Ti. Growth temperature was optimized on Si, TiN/Si, and ZrB2/Si, resulting in increased nanorod aspect ratio with temperature. All nanorods exhibit high purity and quality, proved by the strong bandedge emission recorded with cathodoluminescence spectroscopy at room temperature as well as transmission electron microscopy. These substrates/templates are affordable compared to many conventional substrates, and the direct deposition onto them eliminates cumbersome post-processing steps in device fabrication. Thus, magnetron sputter epitaxy offers an attractive alternative for simple and affordable fabrication in optoelectronic device technology.