Growth of GaN and AlN thin films by laser induced molecular beam epitaxy

Hexagonal GaN and AlN thin films were grown by laser induced molecular beam epitaxy using Al or Ga metal as target material and N₂as nitrogen source. The films were deposited on sapphire (0001) and SiC (0001) substrates. Epitaxial growth of GaN has been achieved at 730°C and 10⁻³ mbar N₂ pressure. The AlN films were polycrystalline with predominant (0001) orientation.     

Growth and characterization of group-III impurity-doped semiconducting BaSi2 films grown by molecular beam epitaxy

Ga- or In-doped BaSi₂ films were grown on Si(111) by molecular beam epitaxy (MBE). The Ga-doped BaSi₂ showed n-type conductivity. The electron concentration and resistivity of the Ga-doped BaSi₂ depended on the Ga temperature; however, the electron concentration and resistivity could not be controlled properly. In contrast, the In-doped BaSi₂ showed p-type conductivity and its hole concentration was controlled in the range between 10¹⁶ and 10¹⁷ cm^− 3 at RT.     

Si(100)衬底上激光分子束外延制备高质量TiN薄膜

采用激光分子束外延(LMBE)技术在Si(100)上制备了高质量的TiN薄膜.对N2分压和激光脉冲能量对TiN薄膜晶体结构、生长模式和表面形貌影响的研究表明,TiN单晶薄膜呈(200)择优取向,在N2分压为10-1 Pa时,薄膜的结晶度高且表面平整致密.随着N2分压的增加,TiN(200)衍射峰向低角度移动.激光脉冲能...     

Deposition and characterization of MgO/Si gate stacks grown by molecular beam epitaxy

In this article, the deposition and characterization of amorphous MgO films grown on Si (001) using molecular beam epitaxy is reported. In order to ensure amorphous films, low substrate temperatures (200 °C) and high oxygen pressures were used (up to 5 × 10^− 3 Pa). Both atomic and molecular oxygen species were used at different pressures. Films ranging in thickness from 3 nm till 30 nm were grown and characterized using structural and electrical methods.The dielectric constant deduced from this thickness series corresponds to 8.74 close to the bulk value of 9.8. The best equivalent oxide thickness value observed for this series - grown under high oxygen pressure - corresponds to 1.2 nm for a current density measured at V_FB − 1 V of 0.1 A/cm². The films grown with atomic oxygen display a lower capacitance and lower leakage compared to the films grown using molecular oxygen. This is due to the appearance of a thin SiO₂ interface layer which is also responsible for the high defect density observed in the capacitance-voltage measurements. Upon annealing both types of films in forming gas for 15 min at 450 °C, the capacitance decreases further while the leakage increases. This change is assigned to the appearance of the lower bandgap (6.6 eV), lower dielectric constant (6.6) phase of silicate, MgSiO₃. Furthermore a V_FB shift of − 0.6 V is observed and is related to the appearance of oxygen vacancies as Mg diffuses into the SiO₂ interface layer.     

Growth of stoichiometric TiO2 thin films on Au(100) substrates by molecular beam epitaxy

The present study reports on the growth of thin TiO₂ films onto Au(100) single crystals by Ti evaporation in a reactive O₂ atmosphere at two different substrate temperatures: room temperature (RT) and 300 °C. The growth of the oxide films was monitored by means of X-ray photoemission spectroscopy, while the valence and conduction band electronic structure was investigated by UV and inverse photoemission spectroscopy, respectively.The TiO₂ film grows epitaxially on the Au(100) substrate at 300 °C exhibiting the rutile (100) surface. The evolution of the Ti 2p lineshape with the oxide coverage shows the presence of reduced oxide species (characterized by Ti^3 + ions) at the Au(100) interface. A crystalline and stoichiometric TiO₂ oxide is produced at high substrate temperature, while growth at RT gives a measurable concentration of defects. Post growth annealing in ultra-high vacuum of the RT grown film increases this concentration, while subsequent annealing in O₂ atmosphere restores the sample to the as-grown conditions.     

LMBE法生长ZnO薄膜的结构和光学性能

利用激光分子束外延方法(LMBE)在单晶Si(100)和玻璃基片上生长了ZnO薄膜.通过XRD谱、拉曼光谱和光致发光(PL)谱研究了ZnO薄膜的结构和光学性能.结果表明,ZnO薄膜具有六方纤锌矿结构,(002)衍射峰较强,c轴择优取向良好.在可见光范围,ZnO薄膜的平均透射率＞80%,而在紫外范围,平均透射率急剧降低.拟合得到ZnO薄膜的禁带宽度为3.31eV.随激发波长增加,PL谱峰位没有变化,但强度发生了变化.同时,随测量温度升高,紫外发光峰强度减弱,峰位红移,半高宽展宽.理论拟合得到ZnO薄膜的活化能为59meV,接近于ZnO体材料的激子束缚能(60meV),说明紫外发光是由自由激子辐射复合引起的.     

MgxZn1-xO单晶薄膜的分子束外延生长及结构表征

用等离子辅助分子束外延(P-MBE)的方法,在蓝宝石c-平面上外延生长了MgxZn1-xO合金薄膜.在0≤x≤0.2范围内MgxZn1-xO薄膜保持着六角纤锌矿结构不变.原位反射式高能电子衍射图样和X射线双晶衍射谱的结果表明生长的样品是单晶薄膜.随着x值逐渐增大,Mg2+离子逐渐进入ZnO的晶格,X射线双晶衍射测得样品的(002)取向的半高宽度从0.249°增加到0.708°,表明结晶质量逐渐下降,(002)方向的X射线衍射峰向大角度方向移动,晶格常数c由5.205(A)减小到5.185(A).透射光谱的结果表明,合金薄膜的吸收边随着Mg离子的掺入逐渐向高能侧移动,室温光致发光谱出现很强的紫外发光(NBE)峰,没有观察到深能级(DL)发射,且随着Mg掺入量的增加,紫外发光峰有明显的蓝移,这与透射光谱的结果是相吻合的.     

Growth and characterization of InP ringlike quantum-dot molecules grown by solid-source molecular beam epitaxy

In this paper, we have studied the fabrication of InP ringlike quantum-dot molecules on GaAs(001) substrate grown by solid-source molecular beam epitaxy using droplet epitaxy technique and the effect of In deposition rate on the physical and optical properties of InP ringlike quantum-dot molecules. The In deposition rate is varied from 0.2 ML/s to 0.4, 0.8 and 1.6 ML/s. The surface morphology and cross-section were examined by ex-situ atomic force microscope and transmission electron microscope, respectively. The increasing of In deposition rate results in the decreasing of outer and inner diameters of InP ringlike quantum-dot molecules and height of InP quantum dots but increases the InP quantum dot and ringlike quantum-dot molecule densities. The photoluminescence peaks of InP ringlike quantum-dot molecules are blue-shifted and FWHM is narrower when In deposition rate is bigger.     

Growth of germanium nanowires on silicon(111) substrates by molecular beam epitaxy

Heteroepitaxial growth of Ge nanowires was carried out on Si(111) substrates by MBE. Au seeds were used as precursor for the VLS growth of the nanowires. Even if the Au droplets do not act as catalyst for the dissociation of gas, they are local preferential areas where the energetic barrier of Ge nucleation is lowered compare to the remaining non activated surface. Two sets of Au seeds were used as precursors for the VLS process. The first set have an average diameter of 125 nm and the second of 25 nm. In-situ RHEED monitoring showed a Au wetting layer between these seeds before the nanowires growth as well as at the end of the Ge nanowires growth. It means that the wetting layer acted as a surfactant from the Si(111) surface to the Ge grown layer between the nanowires. Analysis of SEM images brought the fact that the diffusion of gold from the droplets on the surface and the sidewalls of the nanowires via the Ostwald ripening is a key parameter of the growth of the nanowires.     

Growth of β-FeSi2 thin films on β-FeSi2 (110) substrates by molecular beam epitaxy

We have investigated the preparation of β-FeSi₂ substrate and growth condition of β-FeSi₂ thin film on β-FeSi₂ (110) substrate by molecular beam epitaxy. The surface of the substrate was prepared by a wet-etching using HF(50%):HNO₃(60%):H₂O = 1:1:5 solution at 25 °C. It is clear that the optimal etching period to obtain a flat surface was 3 min. The β-FeSi₂ thin film with streak RHEED pattern was obtained at Si/Fe flux ratio of 2.9. Average surface roughness (Ra) of the β-FeSi₂ film was about 0.5 nm in 5 × 5 μm² area.     

Growth of columnar aluminum nitride layers on Si(111) by molecular beam epitaxy

Single crystalline aluminum nitride (AlN) thin films are deposited by molecular beam epitaxy (MBE) using thermally evaporated aluminum and RF-plasma excited nitrogen gas. In this paper we report on films grown on Si(111) at substrate temperatures of 800° with growth rates between 65 and 350 nm h⁻¹. All layers consist of hexagonal and exactly c-axis oriented AlN crystals with column-like structure. For the smoothest layers surface roughness (rms) around 1 nm is obtained. In the XRD-spectra (ω-scan) we have achieved a minimum FWHM of 0.4° (=25′) for the AlN(00.2) reflex. At maximum growth rates (350 nm h⁻¹) for AlN a transition zone of about 200 nm is formed with high defect density compared to the subsequent growth. For lower growth rates (65 nm h⁻¹) no transition zone exists. Application of a substrate nitridation leads to a partial loss of epitaxial relation between AlN layer and Si(111)-substrate.     

Combinatorial screening of halide perovskite thin films and solar cells by mask-defined IR laser molecular beam epitaxy

Abstract

As an extension of combinatorial molecular layer epitaxy via ablation of perovskite oxides by a pulsed excimer laser, we have developed a laser molecular beam epitaxy (MBE) system for parallel integration of nano-scaled thin films of organic–inorganic hybrid materials. A pulsed infrared (IR) semiconductor laser was adopted for thermal evaporation of organic halide (A-site: CH₃NH₃I) and inorganic halide (B-site: PbI₂) powder targets to deposit repeated A/B bilayer films where the thickness of each layer was controlled on molecular layer scale by programming the evaporation IR laser pulse number, length, or power. The layer thickness was monitored with an in situ quartz crystal microbalance and calibrated against ex situ stylus profilometer measurements. A computer-controlled movable mask system enabled the deposition of combinatorial thin film libraries, where each library contains a vertically homogeneous film with spatially programmable A- and B-layer thicknesses. On the composition gradient film, a hole transport Spiro-OMeTAD layer was spin-coated and dried followed by the vacuum evaporation of Ag electrodes to form the solar cell. The preliminary cell performance was evaluated by measuring I-V characteristics at seven different positions on the 12.5 mm × 12.5 mm combinatorial library sample with seven 2 mm × 4 mm slits under a solar simulator irradiation. The combinatorial solar cell library clearly demonstrated that the energy conversion efficiency sharply changes from nearly zero to 10.2% as a function of the illumination area in the library. The exploration of deposition parameters for obtaining optimum performance could thus be greatly accelerated. Since the thickness ratio of PbI₂ and CH₃NH₃I can be freely chosen along the shadow mask movement, these experiments show the potential of this system for high-throughput screening of optimum chemical composition in the binary film library and application to halide perovskite solar cell.     

Thickness distribution of films fabricated by the molecular beam epitaxy technique

The thickness distribution of the film deposited on a rotating substrate holder depends on both the geometrical parameters of the molecular-beam-epitaxy apparatus and the angular distribution of molecular flux from the evaporation furnace. First, Deppisch's formulation for calculation of the thickness distribution is generalized so that it can be applied to a more practical case when the furnace is inclined relative to the axis of rotation of the holder. Next, the angular distributions are calculated for several types of furnaces of practical use by means of the test-particle Monte Carlo method. They are expressed in simple analytical forms. Lastly, example calculations are made to show how to determine such geometrical parameters as are optimum for yielding uniformly thick films.     

Epitaxial growth of ZnO layers on (111) GaAs substrates by laser molecular beam epitaxy

ZnO layers were grown on (111) GaAs substrates by laser molecular epitaxy at substrate temperatures between 200 and 550 °C. X-ray diffraction analysis revealed that c-axis of ZnO epilayer with a wurtzite structure is perpendicular to the substrate surface. X-ray rocking curves and Raman spectroscopy showed that the crystal quality of ZnO epilayers depends on the substrate temperature during the growth. Strong near-band-edge emission in the UV region without any deep-level emissions was observed from the ZnO epilayers at room temperature. The results indicate that laser molecular beam epitaxy is a promising growth method for obtaining high-quality ZnO layers on (111) GaAs substrates.     

Magnetization reversal in YIG/GGG(111) nanoheterostructures grown by laser molecular beam epitaxy

Abstract

Thin (4–20 nm) yttrium iron garnet (Y₃Fe₅O₁₂, YIG) layers have been grown on gadolinium gallium garnet (Gd₃Ga₅O₁₂, GGG) 111-oriented substrates by laser molecular beam epitaxy in 700–1000 °C growth temperature range. The layers were found to have atomically flat step-and-terrace surface morphology with step height of 1.8 Å characteristic for YIG(111) surface. As the growth temperature is increased from 700 to 1000 °C the terraces become wider and the growth gradually changes from layer by layer to step-flow regime. Crystal structure studied by electron and X-ray diffraction showed that YIG lattice is co-oriented and laterally pseudomorphic to GGG with small rhombohedral distortion present perpendicular to the surface. Measurements of magnetic moment, magneto-optical polar and longitudinal Kerr effect (MOKE), and X-ray magnetic circular dichroism (XMCD) were used for study of magnetization reversal for different orientations of magnetic field. These methods and ferromagnetic resonance studies have shown that in zero magnetic field magnetization lies in the film plane due to both shape and induced anisotropies. Vectorial MOKE studies have revealed the presence of an in-plane easy magnetization axis. In-plane magnetization reversal was shown to occur through combination of reversible rotation and abrupt irreversible magnetization jump, the latter caused by domain wall nucleation and propagation. The field at which the flip takes place depends on the angle between the applied magnetic field and the easy magnetization axis and can be described by the modified Stoner–Wohlfarth model taking into account magnetic field dependence of the domain wall energy. Magnetization curves of individual tetrahedral and octahedral magnetic Fe³⁺ sublattices were studied by XMCD.     

Electrical, optical and structural characterization of high-k dielectric ZrO2 thin films deposited by the pyrosol technique

High-k dielectric zirconium oxide (ZrO₂) thin films have been deposited on silicon substrates at temperatures from 400 to 600 °C using the spray pyrolysis technique. The films were deposited from two spraying solution concentrations (0.033 and 0.066 M) of zirconium acetylacetonate dissolved in N,N-dimethylformamide. These films were stoichiometric, transparent and with a very low surface roughness (5–40 ). The refractive index of these films was of the order of that obtained for a bulk material (2.12). Films deposited with high molar concentration presented the best electrical characteristic, have a dielectric constant in the range 12.5–17.5, depending on the deposition temperature, and can stand electric fields up to 3 MV cm^–1 without observing destructive dielectric breakdown. Transmission electron microscopy measurements, indicate that the films consist of nano-crystallites of the tetragonal ZrO₂ crystalline phase embedded into an amorphous matrix. Infrared spectroscopy measurements of the films show peaks associated with ZrO₂ and a peak related to silicon dioxide (SiO₂). The analysis of spectroscopic ellipsometry measurements on these films indicates the existence of a layer at the ZrO₂/Si interface composed of SiO₂ as well as ZrO₂ and crystalline silicon.     

Annealing temperature dependence on the structural and optical properties of sputtering-grown high-k HfO2 gate dielectrics

High-k gate dielectric HfO₂ thin films have been deposited on Si and quartz substrates by radio frequency magnetron sputtering. The structural characteristics, surface morphology, and optical properties of the HfO₂/Si gate stacks at various post-annealing temperatures were examined by X-ray diffraction (XRD), atomic force microscopy (AFM), fourier transform infrared spectroscopy (FTIR), ultraviolet–visible spectroscopy (UV–Vis spectroscopy), and spectroscopic ellipsometry (SE). XRD measurement indicates that the 80 W-deposited HfO₂ films demonstrate a polycrystalline structure. AFM measurements illustrate that the root mean square of the HfO₂ thin films demonstrates an apparent increase with increasing the annealing temperature. Analysis from FTIR indicates that the Si–O–Si bonds vibration peak position shift toward lower wave numbers with increasing the annealing temperature. Combined with UV–Vis spectroscopy and SE measurements, it can be noted reduction in band gap with an increase in annealing temperature has been confirmed. Additionally, increase in refractive index (n) has been confirmed by SE.     

Growth of M-plane GaN on (100) LiGaO2 by plasma-assisted molecular beam epitaxy

Growth of M-plane GaN on (100) LiGaO₂ was achieved using plasma-assisted molecular beam epitaxy. Thermal annealing of the LiGaO₂ wafer was found to lead to a substrate surface suitable for growth. Structural and morphological analysis was performed using x-ray and reflective high energy electron diffraction, scanning electron and atomic force microscopy. X-ray diffraction results show very high phase purity and a relaxation state of the GaN film close to 80%. The surface morphology, showing characteristic M-plane streaks, is flat and smooth.     

Growth and characterization of Hg1-xCdxTe epitaxial films by isothermal vapour phase epitaxy (ISOVPE)

Growth of Hg_1-xCd_xTe epitaxial films by a new technique called asymmetric vapour phase epitaxy (ASVPE) has been carried out on CdTe and CZT substrates. The critical problems faced in normal vapour phase epitaxy technique like poor surface morphology, composition gradient and dislocation multiplication have been successfully solved. The epitaxial films have been electrically characterized by using the Hall effect and capacitance-voltage (C-V) measurements.