Molecular Beam Epitaxy Technique Research Articles

Barrier heights and strong fermi-level pinning at epitaxially grown ferromagnet/ZnO/metal Schottky Interfaces for opto-spintronics applications

Schottky contacts at the ferromagnet/ZnO interface are good candidates for the realization and control of several semiconductor emerging magnetic phenomena such spin injection and spin-controlled photonics. In this work, we demonstrate the epitaxial growth of single-phase and wurtzite-ZnO thin films on fcc Pt/Co0.30Pt0.70 (111) electrodes by molecular beam epitaxy technique. While the magnetic properties of the Pt/Co0.30Pt0.70 buffer remain unchanged after the ZnO growth, the electric measurements of back-to-back Schottky diodes reveal Schottky barrier heights at the metal/ZnO interfaces in the range of 590–690 meV using Cu, Pt and Co0.30Pt0.70 contacts. A pinning factor S and a charge neutrality level (CNL) ΦCNL of 0.08 and 4.94 eV, respectively, are obtained indicating a strong Fermi-level pining with a CNL level that lies 0.64 eV bellow the conductance band of ZnO semiconductor. These experimental findings indicate that Co0.30Pt0.70/ZnO interface follows the metal-induced gap states model and can open a pathway for the realization of opto-spintronics applications such spin-LEDs.

Interfacial characteristics dependence on interruption times in InGaAs/InAlAs superlattice grown by molecular beam epitaxy

This study delves into the impact of interruption times on the interfacial characteristics of strain-balanced InGaAs/InAlAs superlattice structures. The structures were grown epitaxially using molecular beam epitaxy technique and subsequently analyzed through atomic probe tomography. Based on our findings, interruption times significantly influence the characteristics of layers and interfaces, as well as the composition of layers. Notably, interruption times significantly influence the interface length in the InAlAs layers, with changes of up to 10 % of its thickness. In contrast, the interface length in the InGaAs layers remains unaffected by variations in interruption time. These insights into the evolution of interface lengths, which are influenced by the growth modes of layers, adatom mobility, and interruption times, present a promising opportunity for enhancing epitaxial growth methods for quantum devices.

Kinetics-controlled epitaxial growth and bipolar transport properties of semimetal Bi4Se3

(Bi2)m(Bi2Se3)n (m, n: integers) compounds with an infinitely adaptive superlattice structure exhibit several fascinating topological phases. Here, we study kinetics-controlled epitaxial growth of Bi4Se3 on mica by co-evaporating Bi and Se using molecular beam epitaxy technique, as well as the transport properties of Bi4Se3. By precisely controlling the beam fluxes of Bi and Se and growth temperature, we can tune the growth modes from van der Waals' condensation to spiral growth, thus achieving single-crystalline Bi4Se3 of dislocation-free microplate or mounded thin-film morphologies. This reflects a transition from near-thermodynamic-equilibrium to non-thermodynamic-equilibrium growth processes of single-crystalline Bi4Se3. Thin-film Bi2+xSe3 (1.7 < x < 2) solid-solution phases consisting of randomly stacked Bi2 and Bi2Se3 units are also prepared as comparative samples. Hall and thermopower properties suggest that the as-grown Bi4Se3 films exhibit semimetallic bipolar conduction behaviors while the Bi2+xSe3 films present typical semiconducting transport characteristics with a n-type polarity. Due to semiconductor band structures, the Bi2+xSe3 films show superior thermopower to that of semimetal Bi4Se3.

Molecular beam epitaxy growth and doping modulation of topological semimetal NiTe2

In this study, high-quality thin films of the topological semimetal phase NiTe2 were prepared using the molecular beam epitaxy technique, confirmed through x-ray diffraction with pronounced Laue oscillations. Electrical transport experiments reveal that thick films have properties similar to bulk materials. By employing co-deposition, we introduced either magnetic or non-magnetic elements during the growth of thinner films, significantly altering their electrical properties. Notably, the magnetic element Cr induces long-range ferromagnetic ordering, leading to the observation of a significant anomalous Hall effect in NiTe2 thin films. The Hall conductivity remains nearly constant well below the Curie temperature, indicating the correlation with the intrinsic topological nature of the band structure. Theoretical first principles band calculations support the generation of the Weyl semimetal state in the material through magnetic doping. These findings pave the way for exploring more magnetic Weyl semimetals and related low-dimensional quantum devices based on topological semimetals.

InGaAs quantum dot chains grown by twofold selective area molecular beam epitaxy

Increasing quantum confinement in semiconductor quantum dot (QD) systems is essential to perform robust simulations of many-body physics. By combining molecular beam epitaxy and lithographic techniques, we developed an approach consisting of a twofold selective area growth to build QD chains. Starting from 15 nm-thick and 65 nm-wide in-plane In0.53Ga0.47As nanowires on InP substrates, linear arrays of In0.53Ga0.47As QDs were grown on top, with tunable lengths and separations. Kelvin probe force microscopy performed at room temperature revealed a change of quantum confinement in chains with decreasing QD sizes, which was further emphasized by the spectral shift of quantum levels resolved in the conduction band with low temperature scanning tunneling spectroscopy. This approach, which allows the controlled formation of 25 nm-thick QDs with a minimum length and separation of 30 nm and 22 nm respectively, is suitable for the construction of scalable fermionic quantum lattices.

Epitaxial Growth of Large-Area Monolayers and van der Waals Heterostructures of Transition-Metal Chalcogenides via Assisted Nucleation.

The transition-metal chalcogenides include some of the most important and ubiquitous families of 2D materials. They host an exceptional variety of electronic and collective states, which can in principle be readily tuned by combining different compounds in van der Waals heterostructures. Achieving this, however, presents a significant materials challenge. The highest quality heterostructures are usually fabricated by stacking layers exfoliated from bulk crystals, which - while producing excellent prototype devices - is time consuming, cannot be easily scaled, and can lead to significant complications for materials stability and contamination. Growth via the ultra-high vacuum deposition technique of molecular-beam epitaxy (MBE) should be a premier route for 2D heterostructure fabrication, but efforts to achieve this are complicated by non-uniform layer coverage, unfavorable growth morphologies, and the presence of significant rotational disorder of the grown epilayer. This work demonstrates a dramatic enhancement in the quality of MBE grown 2D materials by exploiting simultaneous deposition of a sacrificial species from an electron-beam evaporator during the growth. This approach dramatically enhances the nucleation of the desired epi-layer, in turn enabling the synthesis of large-area, uniform monolayers with enhanced quasiparticle lifetimes, and facilitating the growth of epitaxial van der Waals heterostructures.

Rapid identification and quantitative analysis of malachite green in fish via SERS and 1D convolutional neural network

Rapid and quantitative detection of malachite green (MG) in aquaculture products is very important for safety assurance in food supply. Here, we develop a point-of-care testing (POCT) platform that combines a flexible and transparent surface-enhanced Raman scattering (SERS) substrate with deep learning network for achieving rapid and quantitative detection of MG in fish. The flexible and transparent SERS substrate was prepared by depositing silver (Ag) film on the polydimethylsiloxane (PDMS) film using laser molecular beam epitaxy (LMBE) technique. The wrinkled Ag NPs@PDMS film exhibits high SERS activity, excellent reproducibility and good mechanical stability. Additionally, the fast in situ detection of MG residues onfishscales was achieved by using the wrinkled Ag NPs/PDMS film and a portable Raman spectrometer, with a minimum detectable concentration of 10-6 M. Subsequently, a one-dimensional convolutional neural network (1D CNN) model was constructed for rapid quantification of MG concentration. The results demonstrated that the 1D CNN quantitative analysis model possessed superior predictive performance, with a coefficient of determination (R2) of 0.9947 and a mean squared error (MSE) of 0.0104. The proposed POCT platform, integrating a transparent flexible SERS substrate, a portable Raman spectrometer and a 1D CNN model, provides an efficient strategy for rapid identification and quantitative analysis of MG in fish.

The Quest for High-Temperature Superconductivity in Nickelates under Ambient Pressure.

Recently, superconductivity with Tc ≈ 80 K was discovered in La3Ni2O7 under extreme hydrostatic pressure (>14 GPa). For practical applications, we needed to stabilize this state at ambient pressure. It was proposed that this could be accomplished by substituting La with Ba. To put this hypothesis to the test, we used the state-of-the-art atomic-layer-by-layer molecular beam epitaxy (ALL-MBE) technique to synthesize (La1-xBax)3Ni2O7 films, varying x and the distribution of La (lanthanum) and Ba (barium). Regrettably, none of the compositions we explored could be stabilized epitaxially; the targeted compounds decomposed immediately into a mixture of other phases. So, this path to high-temperature superconductivity in nickelates at ambient pressure does not seem promising.

Ferromagnetic Order in 2D Layers of Transition Metal Dichlorides.

Magnetism in two dimensions is traditionally considered an exotic phase mediated by spin fluctuations, but far from collinearly ordered in the ground state. Recently, 2D magnetic states have been discovered in layered van der Waals compounds. Their robust and tunable magnetic state by material composition, combined with reduced dimensionality, foresee a strong potential as a key element in magnetic devices. Here, a class of 2D magnets based on metallic chlorides is presented. The magnetic order survives on top of a metallic substrate, even down to the monolayer limit, and can be switched from perpendicular to in-plane by substituting the metal ion from iron to nickel. Using functionalized STM tips as magnetic sensors, local exchange fields are identified, even in the absence of an external magnetic field. Since the compounds are processable by molecular beam epitaxy techniques, they provide a platform with large potential for incorporation into current devicetechnologies.

Application of femtosecond mode-locked SnTe thin films and generation of bound-state solitons

In the realm of ultrafast laser technology, the exploration of two-dimensional materials as saturable absorbers (SA) has garnered significant research interest. Our research investigates the characteristics of SnTe thin films, a topological crystalline insulator material, as a potential saturable absorber for ultrafast lasers. Using the molecular beam epitaxy (MBE) technique, we analyze the films’ morphology and composition through atomic force microscopy (AFM) and successfully deposit SnTe epilayers on Au(111)/mica substrates. Through the utilization of SnTe-SA, an erbium-doped fiber laser is fabricated, demonstrating a pulse output with a width of 276 fs and a center wavelength of 1560 nm, highlighting the potential of SnTe films in manufacturing ultrafast optical devices. Additionally, tightly bound solitons with a soliton interval of 1.01 ps are observed, contributing to the exploration of soliton nonlinear dynamics.

Effect of Energy-driven Molecular Precursor Decomposition on the Crystal Orientation of Antimony Selenide Film and Solar Cell Efficiency.

Antimony selenide (Sb2Se3) consists of 1D (Sb4Se6)n ribbons, along which the carriers exhibit high transport efficiency. By adjusting the deposition parameters of vacuum-deposited methods, such as evaporation temperature, chamber pressure, and vapor concentration, it is possible to grow the (Sb4Se6)n ribbons vertically or highly inclined towards the substrate, resulting in films with [hk1] orientation. However, the specific mechanisms by which these deposition parameters affect the orientation of thin films require a deeper understanding. Herein, a molecular beam epitaxy technique is developed for the preparation of highly [hk1]-oriented Sb2Se3 films, and the effect of evaporation parameters on the film orientation is investigated. It is found that the evaporation temperature can affect the decomposition degree of Sb2Se3, which in turn determines the vapor composition and film orientation. Additionally, the decomposition of Sb2Se3 related to evaporation temperature leads to significant changes in the elemental composition of the film, thereby passivating deep-level defects under Se-rich conditions. Consequently, the Sb2Se3 films with highly [hk1] orientation achieve a power conversion efficiency of 8.42% for the solar cells. This study provides new insights into the control of orientation in antimony-based chalcogenide films and points out new directions for improving the photovoltaic performance of solar cells.

Composition-dependent optical, dielectric and d-orbital electron characteristic of high-throughput horizontal composition gradient Li1-xMgxTi2O4 combinatorial film

The unique physical properties of LiTi2O4 and MgTi2O4 attracted extensive research interest in various fields, including new type batteries and high-temperature superconductors. However, the intricate mechanism governing the d-orbital electron within this system still awaits further excavation. Herein, we employed the combinatorial laser molecular beam epitaxy technique to fabricate a high-quality composition-spread Li1-xMgxTi2O4 film and evaluated its structure, composition, surface morphology and phonon modes by X-ray diffraction, X-ray photoelectron spectroscopy, atomic force microscopy, and Raman scattering spectroscopy. The optical constants and dielectric properties of diverse microregions with varying Li/Mg content over a wide spectral range (189–1658 nm) were measured nondestructively using spectroscopic ellipsometry, revealing the composition-dependent optical properties of Li1-xMgxTi2O4. By fitting the second derivative spectra (d2ε/dE2) using the standard critical point model, five transitions within the detected spectral range were observed. Combining previous analyses and first-principles calculation, we attribute the critical points to crystal field (CF) transition 4A2 →4T1 originating from the spin state of tetrahedral Li/Mg ions, the binding of Ti-related pairs and electron transitions between O-2p to Ti-3d orbits. This exploration of the precise structure of the d-metal band provides a positive reference for the regulation and application of relevant devices.

Distance-Dependent Evolution of Electronic States in Kagome-Honeycomb Lateral Heterostructures in FeSn.

In this work, we demonstrate the formation and electronic influence of lateral heterointerfaces in FeSn containing Kagome and honeycomb layers. Lateral heterostructures offer spatially resolved property control, enabling the integration of dissimilar materials and promoting phenomena not typically observed in vertical heterostructures. Using the molecular beam epitaxy technique, we achieve a controllable synthesis of lateral heterostructures in the Kagome metal FeSn. With scanning tunneling microscopy/spectroscopy in conjunction with first-principles calculations, we provide a comprehensive understanding of the bonding motif connecting the Fe3Sn-terminated Kagome and Sn2-terminated honeycomb surfaces. More importantly, we reveal a distance-dependent evolution of the electronic states in the vicinity of the heterointerfaces. This evolution is significantly influenced by the orbital character of the flat bands. Our findings suggest an approach to modulate the electronic properties of the Kagome lattice, which should be beneficial for the development of future quantum devices.

Achieving high carrier mobility and thermoelectric performance in nearly twin-free rhombohedral GeTe (00l) films

GeTe-based thermoelectric (TE) films have garnered significant attentions due to their promising TE performance near room temperature. However, it is challenging to further optimizing the TE performance due to the inferior carrier mobility (μ) and the excessively high hole density (p). Herein, we developed a novel method based on molecular beam epitaxy technique to successfully fabricate nearly twin-free GeTe (00l) films via incorporating Bi2Te3 buffer layers to alleviate epitaxial strain. Consequently, μ was significantly enhanced. Additionally, through comprehensively investigating the processing conditions, we found that substrate temperature and Te/GeTe flux ratio can shape intrinsic atomic defects and further decrease p. With the optimal synthesis and processing conditions, the GeTe film achieves optimized p of 3.44 × 1020 cm−3 and a high μ of 73.31 cm2/V/s, which lead to the highest room-temperature power factor of 2.67 mWm/K2, outperforming the values of other GeTe films. This work provides important guidance on fabricating twin-free GeTe films and on further improving their TE performance.

MBE-grown tetragonal FeTe consisting of c-axis-aligned nanocrystals

Tetragonal FeTe grown on c-plane sapphire by the molecular beam epitaxy technique is found to result in a new structural phase consisting of c-axis-aligned nanocrystals. Their reflection high-energy electron diffraction patterns display two sets of streaks simultaneously at all rotation angles of the sample. High-resolution x-ray diffraction studies confirm that the nanocrystals are tetragonal FeTe with their c-axes aligned to the growth direction. Atomic force microscopy imaging reveals that further growth of these nanocrystals involves a cannibalism process resulting in nanocrystal pillars with sizes of about 0.5–1 µm. The temperature-dependent resistance of these thin films displays an overall semiconducting behavior, however, with a non-measurable state or jumps and falls depending on their nominal thickness, which can be attributed to the thermal responses of the nanocrystals during cooling and heating processes. This discovery provides an approach to form inhomogeneous heterostructures with all possible twisted angles.

Role of Surface Chemistry of Ta Metal Foil on the Growth of GaN Nanorods by Laser Molecular Beam Epitaxy and Their Field Emission Characteristics.

This study investigates the influence of surface nitridation of Ta metal foil substrates on the growth of GaN nanorods using the laser molecular beam epitaxy (LMBE) technique and the field emission characteristics of the grown GaN nanorod ensemble. Surface morphology examinations underscore the pivotal role of Ta foil nitridation in shaping the dimensions and densities of GaN nanorods. Bare Ta foil fosters the formation of high-density, vertically self-aligned GaN nanorods at a growth temperature of 700 °C. Furthermore, the density of these nanorods is directly related to the duration of Ta foil nitridation, with increased duration leading to a reduced nanorod density. X-ray Photoelectron Spectroscopy (XPS) studies reveal that the transition of the Ta foil surface from tantalum oxide to tantalum nitride during nitridation emerges as a crucial factor influencing GaN nanorod growth. Photoluminescence (PL) spectroscopy at ambient temperature reveals a strong near-band-edge (NBE) emission peak with negligible defect-related peaks, displaying the high optical quality of the GaN nanorods. The highly dense vertically aligned GaN nanorod ensemble growth without Ta prenitridation exhibits the most favorable field emission performance, featuring a turn-on field of 2.1 V/μm, a field enhancement factor of 2480, and a stable long-term operation at the emission current density of 2.26 mA/cm2. This study advances the understanding of the role of the surface chemistry of metal foil in determining GaN nanorod growth and opens up exciting possibilities for tailoring advanced optoelectronic devices for specific application requirements.

Study of dielectric polarization and electrical transport in Bi1·2Sb0·8Te0·4Se2.6 nanofilms

Studying the dielectric response of topological insulators (TIs) can unveil their unique physical mechanisms such as charge transport and spin-orbit coupling effects. However, due to the manifestation of material's topological nature and band structure primarily in nanofilm, such thickness poses challenges for dielectric testing. To date, research on TI dielectric aspects remains relatively unexplored. Therefore, this paper successfully synthesizes nanofilm of quaternary topological insulator Bi1·2Sb0·8Te0·4Se2.6 (BSTS) using laser molecular beam epitaxy (LMBE) technique. Utilizing a wide-frequency dielectric spectrometer and a comprehensive physical properties measurement system (PPMS), we measured and thoroughly analyzed the dielectric polarization and charge transport characteristics of BSTS. We observed various polarization responses in the frequency range of 101–103 Hz, with the dipole orientation gradually failing to keep pace with the frequency increase in the range of 103–105 Hz, and the relaxation polarization unable to establish itself in the range of 105–107 Hz, with polarization primarily contributed by displacement polarization. Subsequently, we further analyzed the dependence of BSTS dielectric polarization response on temperature and film thickness, which will help reveal the influence of external factors on TI dielectric response, providing crucial insights for controlling TI materials' dielectric response. This not only deepens our understanding of the fundamental physical properties of this novel material but also offers important scientific basis and technological support for its applications in quantum computing, photonics, spintronics, and other fields.

Revealing the temperature-driven Lifshitz transition in p-type Mg3Sb2-based thermoelectric materials

The manipulation of native atomic defects and their thermal excitations plays vital roles in the thermoelectric performance of Mg3Sb2-based materials. While native defects manipulation has been intensively studied in p-type Mg3Sb2, there exists interesting unsolved issue regarding the abnormal semiconducting electrical behavior in most of samples. In this work, high quality Mg3Sb2 and Mg3Bi2 (00l) films are fabricated by molecular beam epitaxy technique, while variable temperature angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy measurements are utilized for resolving the aforementioned issue. The thermal excitation of Mg interstitials (the electron donor) results in an obvious downshift of valence bands with rising temperature in both the p-type Mg3Sb2 and Mg3Bi2. Meanwhile, the interesting temperature-driven Lifshitz transition is discovered in the p-type Mg3Sb2, as indicated by the change of Fermi surface topology. Above the Lifshitz transition temperature, the Fermi level of p-type Mg3Sb2 will enter the bandgap, which leads to the abnormal semiconducting electrical behavior. This work discloses the excitation of native defects and temperature-driven Lifshitz transition, which are the main causes for the anomalies in electrical transport of p-type Mg3Sb2-based materials, and also provides valuable insights for further improving their thermoelectric performance.

Highly oriented crystalline si on epitaxial Gd2O3/Si(111) substrate using low-cost Radio Frequency sputtering for Silicon on Insulator application

Silicon-on-Insulator (SOI) technology has been the center of attraction with the advancement in Radio Frequency (RF) technology and the advent of Internet-of-Things due to its low-power operation with reduced parasitic and short-channel effects. However, the state-of-the-art smart-cut method used for the SOI wafer is costly. Alternatively, the notion of using the Si channel layer on epitaxial rare-earth oxide has been proposed. In literature, the existing techniques used to achieve the same, such as Molecular beam Epitaxy or reduced-pressure chemical vapor deposition technique, are either costly or non-high-volume manufacturable. In this context, we propose a method to fabricate the highly oriented crystalline Si(111) channel layer (Top-Si) on an epitaxial Gd2O3/Si(111) virtual substrate (SOXI) utilizing the solid phase epitaxy using the high-volume manufacturing friendly (HVM), low-cost RF magnetron sputtering technique. First, we have shown the multicrystalline Si and epitaxial Gd2O3 layer grown on Si(111) substrate, as confirmed using high-resolution X-ray diffraction (HRXRD) and Transmission Electron Microscopy (TEM). Second, we investigated the impact of rapid thermal annealing at 850 °C on the heterostructure using HRXRD and TEM. It is observed that the high-temperature annealing transforms the Top-Si layer into the highly oriented crystalline Si(111) layer by fusing smaller grains towards larger grains. Hence, we demonstrate a low-cost, HVM-friendly technique for the fabrication of SOXI wafers.

Migration-Enhanced Epitaxial Growth of InAs/GaAs Short-Period Superlattices for THz Generation

The low-temperature-grown InGaAs (LT-InGaAs) photoconductive antenna has received great attention for the development of highly compact and integrated cheap THz sources. However, the performance of the LT-InGaAs photoconductive antenna is limited by its low resistivity and mobility. The generated radiated power is much weaker compared to the low-temperature-grown GaAs-based photoconductive antennas. This is mainly caused by the low abundance of excess As in LT-InGaAs with the conventional growth mode, which inevitably gives rise to the formation of As precipitate and alloy scattering after annealing. In this paper, the migration-enhanced molecular beam epitaxy technique is developed to grow high-quality (InAs)m/(GaAs)n short-period superlattices with a sharp interface instead of InGaAs on InP substrate. The improved electron mobility and resistivity at room temperature (RT) are found to be 843 cm2/(V·s) and 1648 ohm/sq, respectively, for the (InAs)m/(GaAs)n short-period superlattice. The band-edge photo-excited carrier lifetime is determined to be ~1.2 ps at RT. The calculated photocurrent intensity, obtained by solving the Maxwell wave equation and the coupled drift–diffusion/Poisson equation using the finite element method, is in good agreement with previously reported results. This work may provide a new approach for the material growth towards high-performance THz photoconductive antennas with high radiation power.