Heteroepitaxial Growth Research Articles

Optical Properties of Yttrium Ferrite Films Prepared by Pulse Laser Deposition

This study investigates the optical properties of yttrium ferrite thin films fabricated via pulse laser deposition. Yttrium orthoferrite, a ferrimagnetic material known for its potential applications in spintronics and photonics, was deposited on single-crystal substrates under controlled conditions to analyze its optical characteristics. The influence of deposition time on the film quality and optical properties was examined. Atomic force microscopy in contact mode revealed surface roughness variations up to 35 nm, indicating the films’ ability to cover substrate defects. Reflectance measurements determined the optical band gap, which decreased from 3.17 eV for thinner films (44 nm) to 2.91 eV for thicker films (93 nm). Forbidden electronic transitions were also observed, attributed to heteroepitaxial growth and phonon interactions. These results demonstrate the effect of film thickness on morphology and optical properties, making YFeO3 films promising for a range of optoelectronic applications.

Hydrogen‐Driven Phase Differentiation in BN Nucleation on Diamond

AbstractBoron nitride has attracted scientific interest in recent years due to its potential use in electronics, both as hexagonal (hBN) and cubic (cBN) phases. While both are successfully realized through chemical vapor deposition, the heteroepitaxial growth of cBN on another iconic semiconductor, diamond is plagued with mixed‐phase formation. Employing first‐principles computations and a nanoreactor approach, the BN phase preferences are explored on diamond (001) controlled—as it is discovered—by the hydrogen gas concentration. In a limited‐hydrogen environment, the initial BN‐island expands along the diamond surface, forming a 3D metastable cubic phase that grows in the direction normal to the basal plane through kinetically‐limited nucleation, thus overcoming the thermodynamic preference toward the hBN phase. Comparatively, the amorphous phase is favored in the absence of hydrogen, while the hexagonal phase dominates at its high levels, elucidating numerous experimental observations. A obtained kinetic phase diagram connects the phase with hydrogen chemical potential to facilitate targeted phase selection. The results suggest that gas‐mediated nucleation kinetics provide feasible control for the precise synthesis. It also offers valuable guidance for the controllable synthesis of desired BN phases and advances research toward potential BN electronics.

Insights into strain dependent lattice thermal conductivity of α - and κ -Ga2O3

α- and κ-Ga2O3 are promising candidates for high-performance devices such as high-power electronics, but the low thermal conductivity (TC) severely hinders its application. Strain inevitably exists in practical Ga2O3-based devices due to the mismatch of lattice structure and thermal expansion brought by heteroepitaxial growth, and it significantly influences the thermal properties of α- and κ-Ga2O3. By employing first-principles calculations and the phonon Boltzmann transport equation, we have studied the TC at the induced strain and optimized strain axis in free states and 16 different strain states. The TC at the induced strain and optimized strain axis generally decreases with increasing strain. Under −4% XZ-axes biaxial compressive strain, the kzz of α-Ga2O3 can increase to ∼1.7 times its original value, while under −2% XY-axes biaxial compressive strain, the kxx of κ-Ga2O3 can increase to 2.8 times its original value. The improvement of thermal transport properties is attributed to the increase in phonon group velocity and relaxation time caused by the phonon hardening and decrease in three-phonon scattering channels, respectively. However, we observed an exception: under +4% X-axis tensile strain, kyy of α-Ga2O3 increased by 1.1 times. Moreover, atomic bond analysis revealed that under XY-direction strain, the ICOHP values for α-Ga2O3 are −3.94 eV (at −4% strain), −3.76 eV (unstrained state), and −3.63 eV (+4% strain). This discovery elucidates the origin of phonon hardening under compressive strain, indicating that strengthened bonds enhance phonon transport. This study provides essential insights into the mechanisms of α- and κ-Ga2O3 TC under different strains.

Recent progress on heteroepitaxial growth of single crystal diamond films

AbstractDiamond is an ultimate semiconductor with exceptional physical and chemical properties, such as an ultra‐wide bandgap, excellent carrier mobility, extreme thermal conductivity, and stability, making it highly desirable for various applications including power electronics, sensors, and optoelectronic devices. However, the challenge lies in growing the large‐size and high‐quality single‐crystal diamond films, which are crucial for realizing the full potential of this wonder material. Heteroepitaxial growth has emerged as a promising approach to achieve single‐crystal diamond wafers with large sizes of up to 3 inches and controlled electrical properties. This review provides an overview of the advancements in diamond heteroepitaxy using microwave plasma‐assisted chemical vapor deposition, including the mechanism of heteroepitaxial growth, selection of substrates, film optimization, chemistry of defects, and doping. Moreover, recent progress on the device applications and perspectives is also discussed.

High-quality heteroepitaxial growth of β-Ga2O3 with NiO buffer layer based on Mist-CVD

The heteroepitaxial growth of β-Ga2O3 on the commonly used sapphire substrate presents great challenges due to their large lattice mismatch. To address this, a NiO buffer layer is proposed to improve the quality of the heteroepitaxial β-Ga2O3, as it has a lower lattice mismatch (0.46 %) with β-Ga2O3 compared to sapphire (6.6 %). Traditional epitaxial growth methods for Ga2O3 are not compatible with NiO growth, so an inexpensive, non-vacuum, and convenient Mist-CVD technology is used for heterogeneous β-Ga2O3 growth in this study. XRD and TEM results demonstrate the high quality of β-Ga2O3 sample with the clear interface between materials. Introducing a NiO buffer layer enables the Full Width at Half Maximum (FWHM) and root-mean-square (RMS) roughness of β-Ga2O3 to reduce from 0.726° to 0.514° and from 7.47 nm to 3.34 nm respectively. Additionally, through the UDM analysis model, micro-strain within the film is found to significantly decrease. This work proposes a novel approach to improve the quality of β-Ga2O3 heteroepitaxial growth on sapphire substrate, contributing to the advancement of Ga2O3 materials and devices.

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.

Atomic structure of self-buffered BaZr(S, Se)3 epitaxial thin film interfaces

Understanding and controlling the growth of chalcogenide perovskite thin films through interface design is important for tailoring film properties. Here, the film and interface structure of BaZr(S,Se)3 thin films grown on LaAlO3 by molecular beam epitaxy and postgrowth anion exchange is resolved using aberration-corrected scanning transmission electron microscopy. Epitaxial films are achieved from self-assembly of an interface “buffer” layer, which accommodates the large film/substrate lattice mismatch of nearly 40% for the alloy film studied here. The self-assembled buffer layer, occurring for both the as-grown sulfide and post-selenization alloy films, is shown to have rock-salt-like atomic stacking akin to a Ruddlesden–Popper phase. These results provide insights into oxide-chalcogenide heteroepitaxial film growth, illustrating a process that yields relaxed, crystalline, epitaxial chalcogenide perovskite films that support ongoing studies of optoelectronic and device properties.

Direct-bonded diamond membranes for heterogeneous quantum and electronic technologies

Diamond has superlative material properties for a broad range of quantum and electronic technologies. However, heteroepitaxial growth of single crystal diamond remains limited, impeding integration and evolution of diamond-based technologies. Here, we directly bond single-crystal diamond membranes to a wide variety of materials including silicon, fused silica, sapphire, thermal oxide, and lithium niobate. Our bonding process combines customized membrane synthesis, transfer, and dry surface functionalization, allowing for minimal contamination while providing pathways for near unity yield and scalability. We generate bonded crystalline membranes with thickness as low as 10 nm, sub-nm interfacial regions, and nanometer-scale thickness variability over 200 by 200 μm2 areas. We measure spin coherence times T2 for nitrogen vacancy centers in 150 nm-thick bonded membranes of up to 623 ± 21 μs, suitable for advanced quantum applications. We demonstrate multiple methods for integrating high quality factor nanophotonic cavities with the diamond heterostructures, highlighting the platform versatility in quantum photonic applications. Furthermore, we show that our ultra-thin diamond membranes are compatible with total internal reflection fluorescence (TIRF) microscopy, which enables interfacing coherent diamond quantum sensors with living cells while rejecting unwanted background luminescence. The processes demonstrated herein provide a full toolkit to synthesize heterogeneous diamond-based hybrid systems for quantum and electronic technologies.

All Oxide-Based Magnetic Tunnel Junctions Fabricated by Focused Ion Beam Nanomachining Technique

This study offers a comprehensive investigation into the fabrication of all-oxide-based magnetic tunnel junctions (MTJs) utilizing the focused ion beam (FIB) nanomachining method. The oxide thin films of SrTiO3 (STO), La[Formula: see text]CaxMnO3 (LCMO) and La[Formula: see text]SrxMnO3 (LSMO) were grown using pulsed laser deposition (PLD). Magnetization measurements at 5K revealed a notable difference in coercivity between LCMO and LSMO films, highlighting their suitability as electrodes in MTJ device fabrication. The deposited trilayer structure of LCMO/STO/LSMO exhibited heteroepitaxial growth, enabling the independent magnetic switching of electrode layers in the MTJ with the STO barrier layer. Conventional photolithography and ion milling were used to create a series of 4[Formula: see text][Formula: see text]m Hall bar tracks in the deposited films. Nanopillar devices, sized 250[Formula: see text]nm[Formula: see text]×[Formula: see text]250[Formula: see text]nm, were successfully fabricated on these 4[Formula: see text][Formula: see text]m tracks by optimizing the FIB nanomachining technique. The fabricated MTJs demonstrated a high tunnel magnetoresistance (TMR) response, leading to the conclusion that the FIB nanomachining technique holds significant promise for the development of high-performance oxide-based spintronic devices.

Polarity Effect on the Heteroepitaxial Growth of B<sub>x</sub>C on 4H-SiC by CVD

The chemical vapor deposition (CVD) growth of boron carbide (BxC) layers on 4H-SiC, 4°off substrates was studied. Depending on the polarity of the substrate, different results were obtained. On Si face, the direct CVD growth at 1600°C under a mixture of BCl3+C3H8 systematically led to polycrystalline BxC films, whatever the C/B ratio in the gas phase. On the C face, heteroepitaxial growth was obtained for C/B ratios = 12 or higher with a step bunched morphology. If a boridation step (10 min at 1200°C under BCl3 flow) was used before the CVD growth, then heteroepitaxy was successful on both substrate polarities. To explain these results, a mechanism is proposed which involves the nature of the chemical bonds at the early stage of nucleation. It is suggested that a full B coverage of the SiC surface should favor the nucleation of the B-rich (0001) plane of BxC, promoting thus the heteroepitaxial growth along this direction.

Ultra-low-defect homoepitaxial micro-LEDs with enhanced efficiency and monochromaticity for high-PPI AR/MR displays

The issue of brightness in strong ambient light conditions is one of the critical obstacles restricting the application of augmented reality (AR) and mixed reality (MR). Gallium nitride (GaN)-based micro-LEDs, renowned for their exceptional brightness and stability, are considered the foremost contenders for AR applications. Nevertheless, conventional heteroepitaxial growth micro-LED devices confront formidable challenges, including substantial wavelength shifts and efficiency droop. In this paper, we firstly demonstrated the high-quality homoepitaxial GaN-on-GaN micro-LEDs micro-display, and thoroughly analyzed the possible benefits for free-standing GaN substrate from the material-level characterization to device optoelectronic properties and micro-display application compared with sapphire substrate. The GaN-on-GaN structure exhibits a superior crystal quality with ultra-low threading dislocation densities (TDDs) of ~ 105 cm−2, which is three orders of magnitude lower than that of GaN-on-Sapphire. Through an in-depth size-dependent optoelectronic analysis of blue/green emission GaN-on-GaN/ Sapphire micro-LEDs from 100 × 100 shrink to 3 × 3 μm2, real that a lower forward voltage and series resistance, a consistent emission wavelength (1.21 nm for blue and 4.79 nm for green @ 500 A/cm2), coupled with a notable reduction in efficiency droop ratios (15.6% for blue and 28.5% for green @ 500 A/cm2) and expanded color gamut (103.57% over Rec. 2020) within GaN-on-GaN 10 μm micro-LEDs. Last but not least, the GaN-on-GaN micro-display with 3000 pixels per inch (PPI) showcased enhanced display uniformity and higher luminance in comparison to its GaN-on-Sapphire counterpart, demonstrating significant potentials for high-brightness AR/MR applications under strong ambient light.

Surface morphology of 3C–SiC layers grown on 4H–SiC substrates using TCS as silicon precursor

The hetero-epitaxial growth of 3C–SiC layers on on-axis 4H–SiC substrates has been demonstrated in a hot-wall CVD reactor using trichlorosilane and ethylene as precursors. The additional chlorine is supplied by hydrogen chloride for variation of Cl/Si ratio. The influence of temperature, C/Si ratio and Cl/Si ratio process parameters on the morphology is studied. Double-position-boundaries free 3C–SiC epitaxial layers have been successfully grown at the optimized condition, which is at a temperature of 1340 °C, with C/Si = 0.6 and Cl/Si = 6 using a carbon-rich pretreatment. Low temperature near bandgap photoluminescence shows a good optical property of the obtained 3C–SiC epitaxial layers. Compared to the standard chemistry, a higher growth rate of 12 μm/h could be achieved by utilizing the chlorinated precursors. This study provides a feasible way to grow double-position-boundaries free 3C–SiC epitaxial layers using TCS as silicon precursor.

Magneto-optical Kerr effect of noncollinear antiferromagnetic Mn3Ir films

We present the magneto-optical Kerr effect (MOKE) of (111)-oriented antiferromagnetic L12-Mn3Ir films epitaxially grown on MgO (111) substrates. We observed that the amplitude and sign of the polar MOKE change depending on the growth temperature. The Mn3Ir films grown at 800 and 600 °C have rotation angles of 41.6 and −4.6 mdeg and ellipticity angles of −15.3 and 9.1 mdeg, respectively. Residual strains owing to heteroepitaxial growth on the order of a few tenths of a percent can play a critical role in determining the amplitude and sign of the MOKE of a noncollinear antiferromagnet, unlike ferromagnets.

Microstructure and reflectance of porous GaN distributed Bragg reflectors on silicon substrates

Distributed Bragg reflectors (DBRs) based on alternating layers of porous and non-porous GaN have previously been fabricated at the wafer-scale in heteroepitaxial GaN layers grown on sapphire substrates. Porosification is achieved via the electrochemical etching of highly Si-doped layers, and the etchant accesses the n+-GaN layers through nanoscale channels arising at threading dislocations that are ubiquitous in the heteroepitaxial growth process. Here, we show that the same process applies to GaN multilayer structures grown on silicon substrates. The reflectance of the resulting DBRs depends on the voltage at which the porosification process is carried out. Etching at higher voltages yields higher porosities. However, while an increase in porosity is theoretically expected to lead to peak reflectance, in practice, the highest reflectance is achieved at a moderate etching voltage because etching at higher voltages leads to pore formation in the nominally non-porous layers, pore coarsening in the porous layers, and in the worst cases layer collapse. We also find that at the high threading dislocation densities present in these samples, not all dislocations participate in the etching process at low and moderate etching voltages. However, the number of dislocations involved in the process increases with etching voltage.

Light B Doping by Ion Implantation into High‐Purity Heteroepitaxial Diamond

The low‐concentration boron doping is performed from 1016 to 1018 cm−3 by ion implantation into heteroepitaxially synthesized large‐area diamond and electrical properties are investigated. Photoluminescence analysis is first carried out to clarify the optical properties of the heteroepitaxial diamond substrate. As a result, defect complexes of nitrogen‐vacancy and silicon‐vacancy are hardly detected in this substrate, suggesting that optically high‐purity diamond can be accomplished by heteroepitaxial growth. Then, the electrical properties of resistivity, mobility, carrier concentration, and conductive type by Hall effect measurements are investigated. For the samples with doping concentrations higher than 1016 cm−3, the electrical activation of implanted B acting as acceptors is confirmed. The compensation ratio for the sample with 3.5 × 1017 cm−3 concentration reaches 76%, indicating the presence of compensating donor‐like centers. With increasing the doping concentration to 3.5 × 1018 cm−3, the compensation ratio is significantly reduced to 35%. The observed mobility of the higher doped sample takes almost the ideal value observed for the sample doped by chemical vapor deposition process. It is suggested that the heteroepitaxial synthesis of large‐area and high‐purity substrates should contribute to the further development of the application to electronic, optical, and sensing devices in the future.

Concentric hollow multi-hexagonal platelets from a small molecule

The creation of well-defined hollow two-dimensional structures from small organic molecules, particularly those with controlled widths and numbers of segments, remains a formidable challenge. Here we report the fabrication of the well-defined concentric hollow two-dimensional platelets with programmable widths and numbers of segments through constructing a concentric multiblock two-dimensional precursor followed by post-processing. The fabrication of concentric multi-hexagons two-dimensional platelets is realized by the alternative heteroepitaxial growth of two donor-acceptor molecules. Upon ultraviolet irradiation, one of the two donor-acceptor molecules can be selectively oxidized by singlet oxygen generated during the process, and the oxidized product becomes more soluble due to increased polarity. This allows for selective removal of the oxidized segments simply by solvent dissolution, yielding hollow multiblock two-dimensional structures. The hollow two-dimensional platelets can be utilized as templates to lithograph complex electrodes with precisely controlled gap sizes, thereby offering a platform for examining the optoelectronic performance of functional materials.

A High‐Speed Image Sensor Based on Large‐Area MoTe2/Si Photodiode Arrays

AbstractThe market demand for optoelectronic devices is increasing, leading to a need for low‐cost, high‐performance image sensors that can operate effectively in challenging environments such as darkness and fog. The emerging 2D transition metal dichalcogenides (TMDs) have garnered significant interest due to their exceptional optoelectronic properties and compatibility with silicon (Si) complementary metal oxide semiconductor (CMOS) technology. However, the large‐scale synthesis of TMD films and uniform preparation of photodiode arrays remain challenging. This paper reports a synthesis method for heteroepitaxial growth of 2H‐ molybdeum diyelluride (MoTe2) semiconducting films on 3D wafer‐level Si substrates. Using this method, arrays of 2H‐MoTe2/Si heterojunction photodiodes are prepared that demonstrate excellent uniformity and 100% device yield. The photodiodes exhibit satisfactory optoelectronic properties, including a small dark current maintained within a range of 1–3 nA and a maximum responsivity of 521.1 mAW−1 under near‐infrared light at 800 nm, with rise and fall times of less than 4 ms. To demonstrate the image‐sensing capabilities of the photodiode array under visible and near‐infrared (NIR) light illumination, a complete imaging system is designed.The MoTe2/Si photodiode arrays examined in this study offer a practical solution for integrating Si‐based readout circuits and photodetector arrays on a single chip.

Heteroepitaxial growth of Ga2O3 thin films on Al2O3(0001) by ion beam sputter deposition

Deposition of epitaxial oxide semiconductor films using physical vapor deposition methods requires a detailed understanding of the role of energetic particles to control and optimize the film properties. In the present study, Ga2O3 thin films are heteroepitaxially grown on Al2O3(0001) substrates using oxygen ion beam sputter deposition. The influence of the following relevant process parameters on the properties of the thin films is investigated: substrate temperature, oxygen background pressure, energy of primary ions, ion beam current, and sputtering geometry. The kinetic energy distributions of ions in the film-forming flux are measured using an energy-selective mass spectrometer, and the resulting films are characterized regarding crystalline structure, microstructure, surface roughness, mass density, and growth rate. The energetic impact of film-forming particles on the thin film structure is analyzed, and a noticeable decrease in crystalline quality is observed above the average energy of film-forming Ga+ ions around 40 eV for the films grown at a substrate temperature of 725 °C.

Quasi-Homoepitaxial Growth of Highly Strained Alkali-Metal Ultrathin Films on Kagome Superconductors.

Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high-quality thin films, its application to studying strain-induced structural phases is limited. Contrary to this general belief, here the quasi-homoepitaxial growth of Cs and Rb thin films is reported with substantial in-plane compressive strain. This is achieved by utilizing the alkali-metal layer existing in bulk crystal of kagome metals AV3Sb5 (A=Cs and Rb) as a structural template. The angle-resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness-dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face-centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi-homoepitaxy, and pave the way for investigating many-body interactions in Fermi liquids with tunable dimensionality.

Red-Emitting CsPbI3/ZnSe Colloidal Nanoheterostructures with Enhanced Optical Properties and Stability.

Producing heterostructures of cesium lead halide perovskites and metal-chalcogenides in the form of colloidal nanocrystals can improve their optical features and stability, and also govern the recombination of charge carriers. Herein, the synthesis of red-emitting CsPbI3/ZnSe nanoheterostructures is reported via an insitu hot injection method, which provides the crystallization conditions for both components, subsequently leading to heteroepitaxial growth. Steady-state absorption and photoluminescence studies alongside X-ray photoelectron spectroscopy and ultraviolet photoelectron spectroscopy analysis evidence on a type-I band alignment for CsPbI3/ZnSe nanoheterostructures, which exhibit photoluminescence quantum yield of 96% due to the effective passivation of surface defects, and an enhancement in carrier lifetime. Furthermore, the heterostructure growth of ZnSe domains leads to significant improvement in the stability of the CsPbI3 nanocrystals under ambient conditions and against thermal and UV irradiation stress.