Molecular Beam Epitaxy Technique Research Articles

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.

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.

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.

The Origin of the Yellow Luminescence Band in Be-Doped Bulk GaN

Photoluminescence (PL) from Be-doped bulk GaN crystals grown by the High Nitrogen Pressure Solution method was studied and compared with PL from GaN:Be layers on sapphire grown by molecular beam epitaxy and metalorganic chemical vapor deposition techniques. The yellow luminescence band in the latter is caused by the isolated BeGa acceptor (the YLBe band), while the broad yellow band in bulk GaN:Be crystals is a superposition of the YLBe band and another band, most likely the CN-related YL1 band. The attribution of the yellow band in bulk GaN:Be crystals to the BeGaON complex (a deep donor) is questioned.

Pentagonal nanowires from topological crystalline insulators: a platform for intrinsic core-shell nanowires and higher-order topology.

We report on the experimental realization of Pb1-xSnx Te pentagonal nanowires (NWs) with [110] orientation using molecular beam epitaxy techniques. Using first-principles calculations, we investigate the structural stability of NWs of SnTe and PbTe in three different structural phases: cubic, pentagonal with [001] orientation and pentagonal with [110] orientation. Within a semiclassical approach, we show that the interplay between ionic and covalent bonds favors the formation of pentagonal NWs. Additionally, we find that this pentagonal structure is more likely to occur in tellurides than in selenides. The disclination and twin boundary cause the electronic states originating from the NW core region to generate a conducting band connecting the valence and conduction bands, creating a symmetry-enforced metallic phase. The metallic core band has opposite slopes in the cases of Sn and Te twin boundaries, while the bands from the shell are insulating. We finally study the electronic and topological properties of pentagonal NWs unveiling their potential as a new platform for higher-order topology and fractional charge. These pentagonal NWs represent a unique case of intrinsic core-shell one-dimensional nanostructures with distinct structural, electronic and topological properties between the core and the shell region.

Nanomaterials-Based Multiple Quantum Wells for High Photovoltaic Conversion Solar Cells

Using metalorganic chemical vapor deposition (MOCVD), molecular beam epitaxy (MBE) and pulse Laser deposition (PLD) techniques on GaN, Silicon, Silicon Carbide and sapphire substrates, high efficiency InGaN/GaN solar cells are reported with a particular emphasis on the work and achievements made with multi-junction tandem and Nanomaterials (Quantum well (QW), Multiple Quantum Wells (MQW), and Quantum Dots (QD)). An effective method for increasing photon absorption in ultrathin cells made for the best possible photovoltaic response is the InGaN/GaN QW system. To maximize light absorption, the quantum well and barrier thicknesses and number of wells in the MQW active region must be adjusted.

Influence of long- and short-range chemical order on spontaneous magnetization in single-crystalline Fe0.6Al0.4 compound thin films

We systematically investigate the long- and short-range chemical order, lattice volume, and spontaneous magnetization in single-crystalline Fe0.6Al0.4 compound thin films. The vapor-quenching method based on a molecular beam epitaxy technique is utilized to fabricate the single-crystalline Fe0.6Al0.4 compound with the different B2 long-range order parameter S. S was varied by the deposition temperature T d, and it increases with increasing T d. The lattice volume V decreased with increasing T d, while the tetragonal distortion, ∼4%, due to epitaxial strain were observed. The changes in S and V were accompanied with the change in the magnetic moment per Fe, μ Fe. μ Fe showed the monotonic decrease as a function of S whereas μ Fe monotonically increases with V. With considering tetragonal distortion, μ Fe–V relationship has a good agreement with the previous reports. The μ Fe–S relationship showed the steep decrease of μ Fe around S∼ 0.6. In contrast to μ Fe–V relationship, μ Fe–S relationship does not match only from ours to previous studies but also among other reports. It implies the statistical number of the nearest-neighbor Fe–Fe bonds, i.e. S, cannot be an enough explanatory parameter. To clarify the structural origin of change in μ Fe, the short-range order (SRO) parameter inferred from the analysis of superlattice diffractions were introduced. They showed the clear difference for the films with high and low μ Fe. The results suggest that the transition from the long- to the SRO state plays the significant role on μ Fe.

Metastable Co3Mn/Fe/Pb(Mg1/3Nb2/3)O3–PbTiO3 multiferroic heterostructures

Using a molecular beam epitaxy technique, we experimentally demonstrate a multiferroic heterostructure consisting of metastable ferromagnetic Co3Mn on piezoelectric Pb(Mg1/3Nb2/3)O3–PbTiO3 (PMN-PT). Inserting a 2-nm-thick Fe layer between Co3Mn and PMN-PT(001) allows the formation of bcc Co3Mn layers even at an extremely low growth temperature of ∼80°C. Upon increasing this temperature to 200 °C, a bcc Co3Mn/Fe/PMN-PT(001) multiferroic heterostructure with a relatively large saturation magnetization of ∼1680 kA/m and an atomically flat interface is obtained, resulting in an obvious converse magnetoelectric (CME) effect. The large CME effect originates mainly from the strain-induced modulation of the magnetic anisotropy energy, supported by the first-principles calculations.

Intrinsically large effective mass and multi-valley band characteristics of n-type Bi2[sbnd]Bi2Te3 superlattice-like films

Thermoelectric superlattices are expected to decouple the strong correlation between various thermoelectric parameters, and are an important strategy for excellent thermoelectric performances. The superlattices of (Bi2)m(Bi2Te3)n homologous series are well-known for low lattice thermal conductivity and intriguing topological surface states. However, the impacts of electronic structure on the thermoelectric performance were still not well-understood in (Bi2)m(Bi2Te3)n. To cope with this issue, Bi2Bi2Te3 superlattice-like films with adjustable Bi2/(Bi2+Bi2Te3) molar ratio (R) were successfully fabricated by the molecular beam epitaxy technique. Angle-resolved photoemission spectroscopy measurements combined with theoretical calculations revealed the conduction band evolution from single-valley to multi-valley as R ≥ 0.30, leading to intrinsically high carrier effective mass and improved thermoelectric power factor. Also, the superlattice film (R = 0.46) with the structure close to Bi4Te3 possesses the topological surface state feature around the high symmetry point. As a result of the high effective mass of 3.9 m0 and very high electron density of 2.31 × 1021 cm−3, the film with R = 0.46 acquired the highest power factor of 1.49 mW·m−1·K−2 at 420 K, outperforming that of other (Bi2)m(Bi2Te3)n superlattices. This work lays an essential foundation on understanding the electronic structure and further improving thermoelectric performances of (Bi2)m(Bi2Te3)n homologous series.

Tailoring the Structure and Properties of Epitaxial Europium Tellurides on Si(100) through Substrate Temperature Control.

In this study, we improved the growth procedure of EuTe and realized the epitaxial growth of EuTe4. Our research demonstrated a selective growth of both EuTe and EuTe4 on Si(100) substrates using the molecular beam epitaxy (MBE) technique and reveals that the substrate temperature plays a crucial role in determining the structural phase of the grown films: EuTe can be obtained at a substrate temperature of 220 °C while lowering down the temperature to 205 °C leads to the formation of EuTe4. A comparative analysis of the transmittance spectra of these two films manifested that EuTe is a semiconductor, whereas EuTe4 exhibits charge density wave (CDW) behavior at room temperature. The magnetic measurements displayed the antiferromagnetic nature in EuTe and EuTe4, with Néel temperatures of 10.5 and 7.1 K, respectively. Our findings highlight the potential for controllable growth of EuTe and EuTe4 thin films, providing a platform for further exploration of magnetism and CDW phenomena in rare earth tellurides.

Valence Band Dispersion in Bi-Doped (Ga,Mn)As Epitaxial Layers

The impact of incorporating Bi into (Ga,Mn)As layers on their electronic, band structure, magnetic, and structural properties has been studied. The low-temperature molecular beam epitaxy technique was employed to grow homogeneous (Ga,Mn)(Bi,As) layers with high structural perfection. Post-growth annealing treatment resulted in improved structural and magnetic properties, as well as an increase in the hole concentration in the layers. Modulation photoreflectance spectroscopy confirmed modifications to the valence and split-off band in the (Ga,Mn)(Bi,As) layers. The experimental results are consistent with the valence band model of hole-mediated ferromagnetism in the layers. The (Ga,Mn)(Bi,As) compound combines the properties of (Ga,Mn)As and Ga(Bi,As) ternary compounds, offering the possibility of tailoring the bandgap structure to the requirements of novel device functionalities for future spintronic and photonic applications.