Development of in situ characterization techniques in molecular beam epitaxy

Ex situ characterization techniques in molecular beam epitaxy(MBE)have inherent limitations,such as being prone to sample contamination and unstable surfaces during sample transfer from the MBE chamber.In recent years,the need for improved accuracy and reliability in measurement has driven the increasing adoption of in situ characterization techniques.These techniques,such as reflection high-energy electron diffraction,scanning tunneling microscopy,and X-ray photoelectron spectroscopy,allow direct observation of film growth processes in real time without exposing the sample to air,hence offering insights into the growth mechanisms of epitaxial films with controlled properties.By combining multiple in situ characterization techniques with MBE,researchers can better understand film growth processes,realizing novel materials with customized properties and extensive applications.This review aims to overview the benefits and achievements of in situ characterization techniques in MBE and their applications for material science research.In addition,through further analysis of these techniques regarding their challenges and potential solutions,particularly highlighting the assistance of machine learning to correlate in situ characterization with other material information,we hope to provide a guideline for future efforts in the development of novel monitoring and control schemes for MBE growth processes with improved material properties.

Pit density reduction for AlN epilayers grown by molecular beam epitaxy using Al modulation method

We have investigated homoepitaxy of AlN films grown by molecular beam epitaxy on AlN/sapphire templates byadopting both the continuous growth method and the Al modulation epitaxy(AME)growth method.The continuous growthmethod encounters significant challenges in controlling the growth mode.As the precise Al/N=1.0 ratio is difficult toachieve,either the excessive Al-rich or N-rich growth mode occurs.In contrast,by adopting the AME growth method,sucha difficulty has been effectively overcome.By manipulating the supply time of the Al and nitrogen sources,we were able toproduce AlN films with much improved surface morphology.The first step of the AME method,only supplying Al atoms,is important to wet the surface and the Al adatoms can act as a surfactant.Optimization of the initial Al supply time caneffectively reduce the pit density on the grown AlN surface.The pits density dropped from 12 pits/μm^(2)to 1 pit/μm^(2)andthe surface roughness reduced from 0.72 nm to 0.3 nm in a 2×2μm^(2)area for the AME AlN film homoepitaxially grownon an AlN template.

Electrical properties and structural optimization of GaN/InGaN/GaN tunnel junctions grown by molecular beam epitaxy

The InGaN films and GaN/InGaN/GaN tunnel junctions(TJs)were grown on GaN templates with plasma-assisted molecular beam epitaxy.As the In content increases,the quality of InGaN films grown on GaN templates decreases and the surface roughness of the samples increases.V-pits and trench defects were not found in the AFM images.p++-GaN/InGaN/n++-GaN TJs were investigated for various In content,InGaN thicknesses and doping concentration in the InGaN insert layer.The InGaN insert layer can promote good interband tunneling in GaN/InGaN/GaN TJ and significantly reduce operating voltage when doping is sufficiently high.The current density increases with increasing In content for the 3 nm InGaN insert layer,which is achieved by reducing the depletion zone width and the height of the potential barrier.At a forward current density of 500 A/cm^(2),the measured voltage was 4.31 V and the differential resistance was measured to be 3.75×10^(−3)Ω·cm^(2)for the device with a 3 nm p++-In_(0.35)Ga_(0.65)N insert layer.When the thickness of the In_(0.35)Ga_(0.65)N layer is closer to the“balanced”thickness,the TJ current density is higher.If the thickness is too high or too low,the width of the depletion zone will increase and the current density will decrease.The undoped InGaN layer has a better performance than n-type doping in the TJ.Polarization-engineered tunnel junctions can enhance the functionality and performance of electronic and optoelectronic devices.

Strain compensated type Ⅱ superlattices grown by molecular beam epitaxy

We investigate a strain compensation method for the growth of complex interband cascade laser structures. For thick In As/Al Sb superlattice clad layers, the sublayer thicknesses were adjusted so that the tensile strain energy in the In As sublayer was equal to the compressive strain energy in the Al Sb sublayer. For the four-constituent active region, as the compressive strain in the Ga0.65In0.35Sb alloy layer was large, a tensile strain was incorporated in the chirped In As/Al Sb superlattice region for strain compensation to the Ga0.65In0.35Sb alloy. A laser structure of thickness 6 μm was grown on the Ga Sb substrate by molecular beam epitaxy. The wafer exhibited good surface morphology and high crystalline quality.

Characterization of Ga NAs/ Ga As and Ga In NAs/ Ga As Quantum Wells Grown by Plasma-Assisted Molecular Beam Epitaxy: Effects of Ion Damage

The effects of ion damage on Ga NAs/Ga As and Ga In NAs/Ga As quantum wells ( QWs) grown by plas- ma- assisted molecular beam epitaxy have been investigated. Itis found thation damage is a key factor affecting the quality of Ga NAs and Ga In NAs QWs. Obvious appearance of pendello¨ sung fringes in X- ray diffraction pattern and remarkable im provement in the optical properties of the samples grown with ion removal magnets are observed.By removing nitrogen ions,the PL intensity of the Ga In NAs QW is improved so as to be comparable with that of Ga In As QW. The stronger is the magnetic field,the m ore obvious the PL intensity im provement would be.

Highly-Strained InGaAs/GaAs Single-Quantum-Well Lasers Grown by Molecular Beam Epitaxy

Highly stained InGaAs/GaAs Quantum Wells (QW) are grown by using molecular beam epitaxy.The room-temperature photoluminescence (PL) peak wavelength as long as 1160nm is obtained from QW with the In composition of 38% and the well width of 6 8nm.The full-width at half-maximum of the PL peak is 22meV,indicating a good quality.InGaAs/GaAs QW ridge-waveguide lasers with emission wavelength of 1120nm are demonstrated.For 100-μm-wide ridge-waveguide lasers with a cavity length of 800μm,the kink-free output power up to 200mW is achieved with the slope efficiency of 0 84mW/mA under the continue-wave operation.For 10μm-wide ridge-waveguide lasers,the lowest threshold current density of 450A/cm2 and the characteristic temperature of 90K are obtained.

MBE脱氧条件与InGaAs/InP APD性能的相关性

InP基InGaAs/InP雪崩光电二极管(APD)对近红外光具有高敏感度,使其成为微弱信号和单光子探测的理想光电器件。然而随着先进器件结构越来越复杂,厚度尺寸从量子点到几微米不等,性能越来越受材料中晶格缺陷的影响和工艺条件的制约。采用固态源分子束外延(MBE)技术分别在As和P气氛保护下对InP衬底进行脱氧处理并外延生长晶格匹配的In_(0.53)Ga_(0.47)As薄膜和APD结构材料。实验结果表明,As脱氧在MBE材料质量方面比P脱氧具有明显的优势,可获得陡直明锐的异质结界面,降低载流子浓度,提高霍尔迁移率,延长少子寿命,并抑制器件中点缺陷或杂质缺陷引起的暗电流。因此,As脱氧可以有效提高MBE材料的质量,这项工作优化了InP衬底InGaAs/InP外延生长参数和器件制造条件。

Distribution of carriers in gradient-doping transmission-mode GaAs photocathodes grown by molecular beam epitaxy

The gradient-doping structure is first applied to prepare the transmission-mode GaAs photocathode and the integral sensitivity of the sealed image tube achieves 1420μA/lm. This paper studies the inner carrier concentration distribution of the gradient-doping transmission-mode GaAs photocathode after molecular beam epitaxy （MBE） growth using the electrochemical capacitance-voltage profiling. The results show that an ideal gradient-doping structure can be obtained by using MBE growth. The total band-bending energy in the gradient-doping GaAs active-layer with doping concentration ranging from 1×10^19 cm-3 to 1×1018 cm-3 is calculated to be 46.3 meV, which helps to improve the photoexcited electrons movement toward surface for the thin epilayer. In addition,by analysis of the band offsets, it is found that the worse carrier concentration discrepancy between GaAs and GaA1As causes a lower back interface electron potential barrier which decreases the amount of high-energy photoelectrons and affects the short-wave response.

Comparison of blue–green response between transmission-mode GaAsP-and GaAs-based photocathodes grown by molecular beam epitaxy

In order to develop the photodetector for effective blue-green response, the 18-mm-diameter vacuum image tube combined with the transmission-mode Alo.7Gao.3Aso.9Po.1/GaAso.9Po.1 photocathode grown by molecular beam epitaxy is tentatively fabricated. A comparison of photoelectric property, spectral characteristic and performance parameter be- tween the transmission-mode GaAsP-based and blue-extended GaAs-based photocathodes shows that the GaAsP-based photocathode possesses better absorption and higher quantum efficiency in the blue-green waveband, combined with a larger surface electron escape probability. Especially, the quantum efficiency at 532 nm for the GaAsP-based photocathode achieves as high as 59%, nearly twice that for the blue-extended GaAs-based one, which would be more conducive to the underwater range-gated imaging based on laser illumination. Moreover, the simulation results show that the favorable blue-green response can be achieved by optimizing the emission-layer thickness in a range of 0.4 μm-0.6 μm.

High Lattice Match Growth of InAsSb Based Materials by Molecular Beam Epitaxy

High lattice match growth of InAsSb based materials on GaSb substrates is demonstrated. The present results indicate that a stable substrate temperature and the optimal flux ratios are of critical importance in achieving a homogeneous InAsSb based material composition throughout the growth period. The quality of these epilayers is assessed using a high-resolution x-ray diffraction and atomic force microscope. The mismatch between the GaSb substrate and InAsSb alloy achieves almost zero, and the rms surface roughness of InAsSb alloy achieves around 1.7A over an area of 28μm × 28μm. At the same time, the mismatches between GaSb and InAs/InAs0.73Sb0.27 superlattices （SLs） achieve approximately 100 arcsec （75 periods） and zero （300 periods）, with the surface rms roughnesses of InAs/InAs0.73Sb0.27 SLs around 1.8 A （75 periods） and 2.1A （300 periods） over an area of 20 μm×20 μm, respectively. After fabrication and characterization of the devices, the dynamic resistance of the n-barrier-n InAsSb photodetector near zero bias is of the order of 10^6Ω·cm^2. At 77K, the positive-intrinsic-negative photodetectors are demonstrated in InAsSb and InAs/InAsSb SL （75 periods） materials, exhibiting fifty-percent cutoff wavelengths of 3.8μm and 5.1μm, respectively.

Molecular Beam Epitaxy of Zero Lattice-Mismatch InAs/GaSb Type-Ⅱ Superlattice

Type-Ⅱ InAs/GaSb superlattiees made of 13 InAs monolayers （MLs） and 7 GaSb MLs are grown on GaSb substrates by solid source molecular beam epitaxy. To obtain lattice-matched structures, thin InSb layers are inserted between InAs and GaSb layers. We complete a series of experiments to investigate the influence of the InSb deposition time, Ⅴ/Ⅲ beam-equivalent pressure ratio and interruption time between each layer, and then characterize the superlattice （SL） structures with high-resolution x-ray diffraction and atomic force microscopy. The optimized growth parameters are applied to grow the 100-period SL structure, resulting in the full-width half-maximum of 29.55 arcsee for the first SL satellite peak and zero lattice-mismatch between the zero-order SL peak and the GaSb substrate peak.

Interface effect on superlattice quality and optical properties of InAs/GaSb type-Ⅱ superlattices grown by molecular beam epitaxy

We systematically investigate the influence of InSb interface(IF)engineering on the crystal quality and optical properties of strain-balanced InAs/GaSb type-Ⅱsuperlattices(T2SLs).The type-Ⅱsuperlattice structure is 120 periods InAs(8 ML)/GaSb(6 ML)with different thicknesses of InSb interface grown by molecular beam epitaxy(MBE).The highresolution x-ray diffraction(XRD)curves display sharp satellite peaks,and the narrow full width at half maximum(FWHM)of the 0th is only 30-39 arcsec.From high-resolution cross-sectional transmission electron microscopy(HRTEM)characterization,the InSb heterointerfaces and the clear spatial separation between the InAs and GaSb layers can be more intuitively distinguished.As the InSb interface thickness increases,the compressive strain increases,and the surface“bright spots”appear to be more apparent from the atomic force microscopy(AFM)results.Also,photoluminescence(PL)measurements verify that,with the increase in the strain,the bandgap of the superlattice narrows.By optimizing the InSb interface,a high-quality crystal with a well-defined surface and interface is obtained with a PL wavelength of 4.78μm,which can be used for mid-wave infrared(MWIR)detection.

The scanning tunneling microscopy and spectroscopy of GaSb_(1-x)Bi_(x) films of a few-nanometer thickness grown by molecular beam epitaxy

The ultrahigh vacuum scanning tunneling microscope(STM)was used to characterize the GaSb_(1-x)Bi_(x) films of a few nanometers thickness grown by the molecular beam epitaxy(MBE)on the GaSb buffer layer of 100 nm with the GaSb(100)substrates.The thickness of the GaSb_(1-x)Bi_(x) layers of the samples are 5 and 10 nm,respectively.For comparison,the GaSb buffer was also characterized and its STM image displays terraces whose surfaces are basically atomically flat and their roughness is generally less than 1 monolayer(ML).The surface of 5 nm GaSb_(1-x)Bi_(x) film reserves the same terraced morphology as the buffer layer.In contrast,the morphology of the 10 nm GaSb_(1-x)Bi_(x) film changes to the mound-like island structures with a height of a few MLs.The result implies the growth mode transition from the two-dimensional mode as displayed by the 5 nm film to the Stranski-Krastinov mode as displayed by the 10 nm film.The statistical analysis with the scanning tunneling spectroscopy(STS)measurements indicates that both the incorporation and the inhomogeneity of Bi atoms increase with the thickness of the GaSb_(1-x)Bi_(x) layer.

Nanoelectronic devices resonant tunnelling diodes grown on InP substrates by molecular beam epitaxy with peak to valley current ratio of 17 at room temperature

This paper reports that InAs/In0.53Ga0.47As/AlAs resonant tunnelling diodes have been grown on InP substrates by molecular beam epitaxy. Peak to valley current ratio of these devices is 17 at 300K. A peak current density of 3kA/cm^2 has been obtained for diodes with AlAs barriers of ten monolayers, and an Ino.53Ga0.47As well of eight monolayers with four monolayers of InAs insert layer. The effects of growth interruption for smoothing potential barrier interfaces have been investigated by high resolution transmission electron microscope.

Plasma assisted molecular beam epitaxial growth of GaN with low growth rates and their properties

A systematic investigation on PA-MBE grown GaN with low growth rates(less than 0.2μm/h)has been conducted in a wide growth temperature range,in order to guide future growth of sophisticated fine structures for quantum device applications.Similar to usual growths with higher growth rates,three growth regions have been revealed,namely,Ga droplets,slightly Ga-rich and N-rich 3D growth regions.The slightly Ga-rich region is preferred,in which GaN epilayers demonstrate optimal crystalline quality,which has been demonstrated by streaky RHEED patterns,atomic smooth surface morphology,and very low defect related yellow and blue luminescence bands.The growth temperature is a critical parameter to obtain high quality materials and the optimal growth temperature window(~700-760℃)has been identified.The growth rate shows a strong dependence on growth temperatures in the optimal temperature window,and attention must be paid when growing fine structures at a low growth rate.Mg and Si doped GaN were also studied,and both p-and n-type materials were obtained.

Growth of high quality InSb thin films on GaAs substrates by molecular beam epitaxy method with AlInSb/GaSb as compound buffer layers

A series of In Sb thin films were grown on Ga As substrates by molecular beam epitaxy(MBE).Ga Sb/Al In Sb is used as a compound buffer layer to release the strain caused by the lattice mismatch between the substrate and the epitaxial layer,so as to reduce the system defects.At the same time,the influence of different interface structures of Al In Sb on the surface morphology of buffer layer is explored.The propagation mechanism of defects with the growth of buffer layer is compared and analyzed.The relationship between the quality of In Sb thin films and the structure of buffer layer is summarized.Finally,the growth of high quality In Sb thin films is realized.

High quality PdTe_2 thin films grown by molecular beam epitaxy

PdTe2, a member of layered transition metal dichalcogenides （TMDs）, has aroused significant research interest due to the coexistence of superconductivity and type-II Dirac fermions. It provides a promising platform to explore the inter- play between superconducting quasiparticles and Dirac fermions. Moreover, PdTe2 has also been used as a substrate for monolayer antimonene growth. Here in this paper, we report the epitaxial growth of high quality PdTe2 films on bilayer graphene/SiC（0001） by molecular beam epitaxy （MBE）. Atomically thin films are characterized by scanning tunneling microscopy （STM）, X-ray photoemission spectroscopy （XPS）, low-energy electron diffraction （LEED）, and Raman spec- troscopy. The band structure of 6-layer PdTe2 film is measured by angle-resolved photoemission spectroscopy （ARPES）. Moreover, our air exposure experiments show excellent chemical stability of epitaxial PdTe2 film. High-quality PdTe2 films provide opportunities to build antimonene/PdTe2 heterostructure in ultrahigh vacuum for future applications in electronic and optoelectronic nanodevices.

Influence of Ⅴ/Ⅲ ratio on the structural and photoluminescence properties of In_(0.52) AlAs/In_(0.53) GaAs metamorphic high electron mobility transistor grown by molecular beam epitaxy

A series of metamorphic high electron mobility transistors （MMHEMTs） with different Ⅴ/Ⅲ flux ratios are grown on CaAs （001） substrates by molecular beam epitaxy （MBE）. The samples are analysed by using atomic force microscopy （AFM）, Hall measurement, and low temperature photoluminescence （PL）. The optimum Ⅴ/Ⅲ ratio in a range from 15 to 60 for the growth of MMHEMTs is found to be around 40. At this ratio, the root mean square （RMS） roughness of the material is only 2.02 nm; a room-temperature mobility and a sheet electron density are obtained to be 10610.0cm^2/（V.s） and 3.26×10^12cm^-2 respectively. These results are equivalent to those obtained for the same structure grown on InP substrate. There are two peaks in the PL spectrum of the structure, corresponding to two sub-energy levels of the In0.53Ga0.47As quantum well. It is found that the photoluminescence intensities of the two peaks vary with the Ⅴ/Ⅲ ratio, for which the reasons are discussed.

Molecular-beam epitaxy of topological insulator Bi_2Se_3(111) and (221) thin films

This paper presents an overview of the growth of Bi2Se3, a prototypical three-dimensional topological insulator, by molecular-beam epitaxy on various substrates. Comparison is made between the growth of Bi2 Se3 （111） on van der Waals （vdW） and non-vdW substrates, with attention paid to twin suppression and strain. Growth along the [221] direction of Bi2Se3 on InP （001） and GaAs （001） substrates is also discussed.