Sapphire Substrates Research Articles

Effects of Thickness and Grain Size on Harmonic Generation in Thin AlN Films

High-harmonic generation from solid films is an attractive method for converting infrared laser pulses to ultraviolet and vacuum ultraviolet wavelengths and for examining the films using the generation process. In this work, AlN thin films grown on a sapphire substrate are studied. Below-band-gap third harmonics and above-band-gap fifth harmonics were generated using a Ti:sapphire oscillator running at 800 nm. A strong enhancement of the fifth-harmonic signal in the forward direction was observed from thicker 39 nm and 100 nm films compared to thinner 8 nm and 17 nm films. For the fifth harmonic generated in the backward direction, and also for the third harmonic in both the forward and backward directions, only a weak dependence of the harmonic signal on the film thickness was measured. Using both X-ray diffraction and dependence of the fifth harmonic on the laser polarization measurements, these behaviors are attributed to the crystallization and the grain size of the films, promising fifth-harmonic generation as a suitable tool to study AlN film properties.

Substrate-induced strain upshot on the optical and optoelectronic properties of trilayer MoS2.

The characteristics of 2D layered MoS2 film are highly dependent on the substrate it is grown on which leaves us privileged to achieve unique and tunable properties. In this study, trilayer MoS2 films have been grown on fused quartz, crystalline quartz (z-cut), sapphire (0001), and silicon (100) substrates. MoS2 film grows as freestanding on amorphous fused quartz, while it experiences an in-plane tensile strain on the sapphire and silicon. Unprecedentedly we show that due to a large mismatch in the lattice parameter as well as in the thermal expansion coefficient, MoS2 grows with a significant compressive strain both along both in-plane on the crystalline quartz. The developed strain causes an alteration in its electronic structure, causing a 30 meV blue shift in the photoluminescence peak and an increased band gap in addition to fewer sulphur vacancies. Comparatively, the film on sapphire having tensile strain along the in-plane exhibits more sulphur vacancies increasing the electron density. The photoresponse time, photosensitivity, and charge separation distinctly vary for the MoS2 films depending on the substrates. This study underscores the influence of substrate on MoS2 film opening further research scopes on tunable properties owing to 2D layer-substrate interactions.

Design and Experimental Demonstration of Wavelength‐Selective Metamirrors on Sapphire Substrates

The increasing demand for novel mirror coating designs for new generation of gravitational wave detectors is stimulating significant research interest in investigations of reflective properties of metasurfaces. Given this strong interest, this article details a systematic methodology for fabricating reflecting metasurfaces (metamirrors) designed to operate at target wavelengths of 1064 or 1550 nm. The proposed metasurfaces consist of silicon cylindrical nanoparticles placed on a sapphire substrate. First, the dimensional parameters of the structures are thoroughly selected through numerical simulations combined with material characterization. The configurations are subsequently analyzed analytically to reveal the mirror effect, which arises from the excitation of electric and magnetic dipole moments. Following this, the metasurfaces are fabricated and experimentally characterized, demonstrating reflectivity exceeding 95% around the design wavelengths, which is in good agreement with theoretical predictions. Overall, the work demonstrates the feasibility and detailed methodology for the fabrication of thin, lightweight metamirrors capable of achieving near‐perfect reflectivity at the specified target wavelengths.

Depth Profiles of Crystallinity and Preferential Orientation and Surface Characteristics of Sputter‐Deposited CeO2 Thin Film Buffer Layers on Sapphire Substrates Evaluated Through Two‐Dimensional Grazing‐Incidence X‐Ray Diffraction

ABSTRACTTwo‐dimensional grazing‐incidence wide‐angle X‐ray diffraction data were acquired from CeO2 thin films serving as buffer layers on r‐cut sapphire substrates to investigate the depth profiles of crystallinity and preferential orientation as well as surface conditions. The thin film samples were sputter‐deposited under different conditions. Data were obtained at an X‐ray wavelength of 0.100 nm at 0.02° intervals from 0.06° to 0.30° at the grazing‐incidence angle. A 60‐nm‐thick CeO2 thin film sputter‐deposited under Ar (Ar‐60) and a 100‐nm‐thick CeO2 thin film sputter deposited using 10 vol.% O2 in Ar (O+Ar‐100) were found to have partially oriented three‐dimensional bulk crystal structures with preferential orientation in the (100) direction near the surface. The lattice constant for the Ar‐60 film was found to be approximately 0.30% smaller than that for a CeO2 standard, whereas the lattice constant for the O+Ar‐100 film was approximately 0.50% larger. Lattice mismatch between the CeO and CeO2 on the substrate surface is evidently not an issue based on the lattice constants near the surface. Hence, both films could be considered to represent optimal buffer layers for YBa2Cu3O6+δ thin film growth. However, even in the case of a CeO2 thin film suitable for use as a buffer layer, the difference in lattice constants between the interior and surface of an Ar‐60 film was found to be relatively small, whereas that for an O+Ar‐100 film was relatively large. These results show that it is important to analyze the film surface in detail by reducing the incidence angle to less than 0.1°.

Impact of Temperature and Substrate Type on the Optical and Structural Properties of AlN Epilayers: A Cross-Sectional Analysis Using Advanced Characterization Techniques

AlN, with its ultra-wide bandgap, is highly attractive for modern applications in deep ultraviolet light-emitting diodes and electronic devices. In this study, the surface and cross-sectional properties of AlN films grown on flat and nano-patterned sapphire substrates are characterized by a variety of techniques, including photoluminescence spectroscopy, high-resolution X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and Raman spectroscopy. The results indicate that different sapphire substrates have minimal impact on the photoluminescence spectrum of the epitaxial films. As the temperature increased, the radius of curvature of the AlN films increased, while the warpage decreased. The AlN films grown on nano-patterned substrates exhibited superior quality with less surface oxidation. During the growth of AlN thin films on different types of substrates, slight shifts in the energy bands occurred due to differences in the introduction of carbon-related impurities and intrinsic defects. The Raman shift and full width at half maximum (FWHM) of the E2(low), A1(TO), E2(high), E1(TO), and E1(LO) phonon modes for the cross-sectional AlN films varied with the depth and temperature. The stress state within the film was precisely determined with specific depths and temperatures. The FWHM of the E2(high) phonon mode suggests that the films grown on nano-patterned substrates exhibited better crystalline quality.

Deep Ultraviolet Excitation Photoluminescence Characteristics and Correlative Investigation of Al-Rich AlGaN Films on Sapphire.

AlGaN is attractive for fabricating deep ultraviolet (DUV) optoelectronic and electronic devices of light-emitting diodes (LEDs), photodetectors, high-electron-mobility field-effect transistors (HEMTs), etc. We investigated the quality and optical properties of AlxGa1-xN films with high Al fractions (60-87%) grown on sapphire substrates, including AlN nucleation and buffer layers, by metal-organic chemical vapor deposition (MOCVD). They were initially investigated by high-resolution X-ray diffraction (HR-XRD) and Raman scattering (RS). A set of formulas was deduced to precisely determine x(Al) from HR-XRD data. Screw dislocation densities in AlGaN and AlN layers were deduced. DUV (266 nm) excitation RS clearly exhibits AlGaN Raman features far superior to visible RS. The simulation on the AlGaN longitudinal optical (LO) phonon modes determined the carrier concentrations in the AlGaN layers. The spatial correlation model (SCM) analyses on E2(high) modes examined the AlGaN and AlN layer properties. These high-x(Al) AlxGa1-xN films possess large energy gaps Eg in the range of 5.0-5.6 eV and are excited by a DUV 213 nm (5.8 eV) laser for room temperature (RT) photoluminescence (PL) and temperature-dependent photoluminescence (TDPL) studies. The obtained RTPL bands were deconvoluted with two Gaussian bands, indicating cross-bandgap emission, phonon replicas, and variation with x(Al). TDPL spectra at 20-300 K of Al0.87Ga0.13N exhibit the T-dependences of the band-edge luminescence near 5.6 eV and the phonon replicas. According to the Arrhenius fitting diagram of the TDPL spectra, the activation energy (19.6 meV) associated with the luminescence process is acquired. In addition, the combined PL and time-resolved photoluminescence (TRPL) spectroscopic system with DUV 213 nm pulse excitation was applied to measure a typical AlGaN multiple-quantum well (MQW). The RT TRPL decay spectra were obtained at four wavelengths and fitted by two exponentials with fast and slow decay times of ~0.2 ns and 1-2 ns, respectively. Comprehensive studies on these Al-rich AlGaN epi-films and a typical AlGaN MQW are achieved with unique and significant results, which are useful to researchers in the field.

Sensitive direct converting thin film x-ray detector utilizing β-Ga2O3 fabricated via MOCVD

Ga2O3 has been considered as one of the most suitable materials for x-ray detection, but its x-ray detection performance is still at a low level due to the limitation of its quality and absorbance, especially for hard x-ray. In this work, the effects of growth temperature and miscut angle of the sapphire substrate on the crystal quality of Ga2O3 thin films were investigated based on the MOCVD technique. It was found that the crystal growth mode was transformed from island growth to step-flow growth using miscut sapphire substrates and increasing growth temperature, which was accompanied by the improvement of the crystal quality and the reduction of the density of trapped states. Ga2O3 films with optimal crystal quality were finally prepared on a 4° miscut substrate at 900 °C. The x-ray detector based on this film shows good hard x-ray response with a sensitivity of 3.72 × 105μC·Gyair−1·cm−2. Furthermore, the impacts of Ga2O3 film crystal quality and trap density on the x-ray detector were investigated in depth, and the mechanism of the photoconductive gain of the Ga2O3 thin-film x-ray detector was analyzed.

Transferrable GaN-based Micro-LED heterostructures grown on h-BN for optogenetic applications

Individually transferrable GaN-based MQWs micro-LED structures grown on two-dimensional (2D) hexagonal boron nitride (h-BN) have been demonstrated. Different sizes (60 × 30 µm, 60 × 60 µm, 90 × 60 µm and 90 × 90 µm) of GaN-based LED heterostructures on layered h-BN were grown on dielectric SiN patterned sapphire substrates using Metal Organic Vapor Phase Epitaxy (MOVPE). Scanning electron microscope (SEM) images show micro-LEDs were grown with high selectivity within the mask opening areas. Consistent MQWs emission from micro-LEDs was observed at 452 ± 2 nm by cathodoluminescence (CL) spectroscopy for all micro-LED sizes. The structural and optical quality were similar to the GaN-based-LEDs grown on unpatterned substrates. In addition, we have successfully demonstrated the lift-off and transfer of individual micro-LEDs to arbitrary flexible templates using a transfer printing machine, which can be addressed by full front-end process. These studies highlight the role of combination of van der Waals (vdW) epitaxy and selective area growth (SAG) in facilitating the direct realization of dimensionally defined III-Nitride micro-LED structures and the mechanical release and transfer of these micro-LEDs to templates suitable for flexible display and optogenetics applications.

Thermal atomic layer deposition of Ga2O3 films using trimethylgallium and H2O

The Atomic Layer Deposition (ALD) technique is regarded as an effective method for fabricating high-quality Ga2O3 thin films. Trimethyl gallium (TMG), with its high vapor pressure at room temperature (227 Torr), is widely utilized as a gallium precursor in this technique. For oxygen precursors, common choices include O3 and O2 plasma. However, the impact of H2O as an oxygen precursor on Ga2O3 thin films during Thermal Atomic Layer Deposition (TALD) remains insufficiently explored. This study investigates the temperature window and growth characteristics of Ga2O3 thin films, deposited using TMG and H2O as precursors, on sapphire substrates within the temperature range of 250–500 °C. At 250 °C, deposited Ga2O3 films exhibit an amorphous structure, whereas within the 300–500 °C substrate temperature range, they transition to the α-phase. The half-peak width (FWHM) narrows as the temperature increases, with characteristic peaks of the (0006) facets shifting to higher angles at 500 °C. STEM analysis reveals complete coherence between α-Ga2O3 films and the sapphire substrate, indicating a pseudo-crystalline structure formation. The growth rate of the films at 450 °C is 0.083 Å/cycle. Ga2O3 films prepared with H2O as the oxygen precursor exhibit Ga-rich properties, with (Ga + Al)/O atomic ratios between 0.88 and 0.91 across the 250–500 °C temperature range. The films’ roughness (Ra) ranges from 0.453 to 0.646 nm. Island-like particles form on the film surface within the 400–500 °C range, smoothing out as the temperature rises. The film’s band gap peaks at 5.50 eV at 450 °C. The reaction of TMG with H2O on sapphire substrates yields Ga2O3 films and CH4 by-products, akin to the trimethylaluminum process.

Growth and characterization of n-type Ga2O3 films on sapphire substrates by APMOVPE

Growth and characterization of n-type Ga2O3 films on sapphire substrates by APMOVPE

Orientation-dependent structural properties during growth and growth mechanism of CoO films

The orientation-dependent local structural properties of CoO films on sapphire substrates during growth were investigated through linearly-polarized extended X-ray absorption fine structure (EXAFS) measurements. Specifically, CoO(111) and (100) crystals with a rock-salt structure (Fm3m) were epitaxially grown on α-Al2O3(0001) and (101¯2) substrates, respectively, at 700℃ using a radio-frequency sputtering system. The local structural properties of CoO films in the in-plane and out-of-plane orientations were quantitatively determined using linearly-polarized EXAFS at the Co K-edge during growth. The EXAFS analysis revealed that during the initial stages of growth, the local structural properties exhibit significant differences compared to thick films, with short atomic distances and large (small) Debye-Waller factors observed in the out-of-plane (in-plane) orientations. The local structural strain mostly diminished when approximately 20 CoO layers accumulated on the substrate. Density functional theory (DFT) calculations further supported these findings by confirming that cobalt atoms initially form stable bonds with the sapphire surface, leading to the simultaneous growth of oxygen and cobalt layers in a coordinated manner through layer-by-layer growth.

Ammonia-free quasi-atmospheric MOCVD of InN/Al2O3 (0001)

We demonstrate ammonia-free quasi-atmospheric metal–organic chemical vapor deposition (AFQA-MOCVD) of InN grown on c-plane sapphire (Al2O3) substrate using high-density nitrogen (N2) microstrip-line microwave plasma. Dependence of growth temperature (Tg) and N2 plasma power on structural properties were examined. Increasing Tg and N2 plasma power markedly improved surface morphology of InN. An atomically smooth surface with layer-by-layer growth mode was realized at Tg of 750 °C under N2 plasma power of 80 W. Fully strain-relaxed InN was grown on in-plane crystal rotation by 30° with respect to the Al2O3 (0001). N-polar InN on Al2O3 (0001) was revealed by scanning transmission electron microscopy. AFQA-MOCVD enables to expand growth windows by increasing Tg and V/III ratio compared to the standard MOCVD using NH3.

Structural and optical properties of Eu-doped ZnO epitaxial thin films grown by pulsed-laser deposition

Pulsed-laser deposition was utilized to fabricate Eu-doped ZnO epitaxial films on c-plane sapphire substrates with Eu concentrations ranging from 0.5 to 4.0 at. %. The structural properties were analyzed using x-ray diffraction surface normal radial scans and azimuthal cone scans, which confirmed the epitaxy of the film samples. Reciprocal space mapping was performed on ZnO(101̄1) to visualize the effect of Eu incorporation. X-ray fluorescence mapping confirmed the homogeneous distribution of Zn and Eu, and x-ray absorption near-edge structure spectra directly confirmed the trivalent state of Eu ions. The optical properties were assessed using temperature-dependent photoluminescence (PL). Various defects were identified. With increasing Eu dopant concentration, PL emissions from defects and the Eu 4f-intraband transitions gradually became the predominant features in the PL spectra at low temperatures. Furthermore, PL analysis suggested that Eu ions substituted Zn, occupying sites with lower C3v symmetry due to the distortion caused by Eu incorporation.

4 inch 11 μm high-quality AlN thick films grown on nanopatterned sapphire substrates

A high-quality AlN thick film with 11 μm thickness and low defect density was grown on a 4 inch hexagonal hole nano-patterned sapphire substrate by metal oxide chemical vapor deposition. The density of dislocation etch pits in the AlN heteroepitaxial film reached 1.1 × 107 cm−2. The surface and microstrcutres of the AlN thick film were characterized in detail. The dislocation evolution mechanism and stress evolution of AlN were investigated. Dislocations were mainly generated at the interface between the sapphire and AlN, and the voids above the patterned region were generated by the undesirable grain boundaries caused by the lateral epitaxy of AlN and the substrate during the growth process, which prompted a large number of screw dislocations to bend and merge, and while some mixed dislocations to merge and extend upwards, resulting in a high-quality AlN thick film.

Morphological control for hollow rod crystals of a photochromic diarylethene on spherulites by surface properties of substrates.

Sublimation methods utilizing the surface properties of substrates can address the challenge of controlling hollow morphologies in rod crystals. Spherulites were formed on the hydrophilic surface of the (0001) planes of α-quartz and sapphire substrates by sublimation of 1,2-bis(3,5-dimethyl-2-thienyl)perfluorocyclopentene (1a). Various types of hollow morphologies, distinguished by the size and shape of their cross sections and by the presence or absence of branching structures, were formed separately on α-quartz and sapphire substrates. Such precise control of the hollow morphologies was attributed to the wettability of each substrate, leading to the formation of spherulites of 1a. In addition, it was indicated that the formation process of the surface morphologies of spherulites was associated with the hollow morphologies of rod crystals of 1a.

High-Performance Sol-Gel-Derived CNT-ZnO Nanocomposite-Based Photodetectors with Controlled Surface Wrinkles.

We investigate the effects of incorporating single-walled carbon nanotubes (CNTs) into sol-gel-derived ZnO thin films to enhance their optoelectronic properties for photodetector applications. ZnO thin films were fabricated on c-plane sapphire substrates with varying CNT concentrations ranging from 0 to 2.0 wt%. Characterization techniques, including high-resolution X-ray diffraction, photoluminescence, and atomic force microscopy, demonstrated the preferential growth of the ZnO (002) facet and improved optical properties with the increase in the CNT content. Electrical measurements revealed that the optimal CNT concentration of 1.5 wt% resulted in a significant increase in the dark current (from 0.34 mA to 1.7 mA) and peak photocurrent (502.9 µA), along with enhanced photoresponsivity. The rising and falling times of the photocurrent were notably reduced at this concentration, indicating improved charge dynamics due to the formation of a p-CNT/n-ZnO heterojunction. The findings suggest that the incorporation of CNTs not only modifies the structural and optical characteristics of ZnO thin films but also significantly enhances their electrical performance, positioning CNT-ZnO composites as promising candidates for advanced photodetector technologies in optoelectronic applications.

Wafer-scale vertical injection III-nitride deep-ultraviolet light emitters

A ground-breaking roadmap of III-nitride solid-state deep-ultraviolet light emitters is demonstrated to realize the wafer-scale fabrication of devices in vertical injection configuration, from 2 to 4 inches. The epitaxial device structure is stacked on a GaN template instead of conventionally adopted AlN, where the primary concern of the tensile strain for Al-rich AlGaN on GaN is addressed via an innovative decoupling strategy, making the device structure decoupled from the underlying GaN template. Moreover, the strategy provides a protection cushion against the stress mutation during the removal of substrates. As such, large-sized wafers can be obtained without surface cracks, even after the removal of the sapphire substrates by laser lift-off. Wafer-scale fabrication of 280 nm vertical injection deep-ultraviolet light-emitting diodes is eventually demonstrated, where a light output power of 65.2 mW is achieved at a current of 200 mA, largely thanks to the significant improvement of light extraction. This work will definitely speed up the application of III-nitride solid-state deep-ultraviolet light emitters featuring high performance and scalability.

650 V vertical Al0.51Ga0.49N power Schottky diodes

We report high-Al-composition (HAC) Al0.51Ga0.49N vertical power Schottky barrier diodes (SBDs) on sapphire substrates grown by metal organic chemical vapor deposition. The fabricated vertical HAC AlGaN-on-sapphire SBDs exhibit a low turn-on voltage of 1.31 V, a high on/off ratio of ∼107, a low ideality factor of 1.35, and a high breakdown voltage of 662 V.

Mechanism of Thermodynamically Rationalized Selective Growth of a Two-Dimensional Ternary Ferromagnet on Insulating Substrates.

Two-dimensional (2D) semiconducting ferromagnet Fe3GeTe2 holds great promise for advanced spintronic applications because of its gate-tunable ferromagnetic ordering at room temperature, whereas the controllable growth of large-area single crystals remains very challenging due to its ternary nature and variable stoichiometry inducing many competitive phases. Here, we theoretically probe the mechanism of selective growth of monolayer Fe3GeTe2 on various epitaxial substrates. Thermodynamic analysis shows that the corresponding phase-pure chemical potential windows for the selective growth of Fe3GeTe2 can be reasonably attained in ternary phase space on insulating and chemically inert c-plane sapphire and Ga2O3(0001) substrates by properly modulating the interfacial interaction and employing suitable feedstocks to avoid competitive growth of possible impurity phases with different stoichiometry ratios. It is also revealed that both the weak edge-substrate interaction and interlayer coupling of Fe3GeTe2 together lead to a surface-dominated nucleation behavior and, thereby, energetically favor lateral growth of the monolayer rather than vertical growth of the multilayer. Importantly, straight protocols for the experimentally selective growth of phase-pure ternary Fe3GeTe2 are also provided by establishing the relationship between the feedstock chemical potential and growth parameters on a thermochemical basis. Our insightful study can also be reasonably extended to guide future experimental design for the selective growth of other multicomponent 2D materials.

Twin-free thermal laser epitaxy of Si on sapphire

The heteroepitaxial growth of silicon (Si) is essential for modern electronics. Our study investigates the potential of thermal laser epitaxy (TLE) for Si epitaxy. A systematic study on the evaporation behavior of Si during TLE identifies and addresses the causes of notable flux rate fluctuations, resulting in a Si flux with ±0.3% stability over time. We also demonstrate heteroepitaxy of Si on c-plane sapphire substrates via TLE. High-temperature substrate preparation combined with deposition at a substrate temperature of 1000 °C produced high-quality epitaxial Si (111) films without twin domains.