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.

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.

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.

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.

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.

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.

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.

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.

Characteristics of In_(0.52)Al_(0.48)As Grown on InP(100) Substrates by Molecular Beam Epitaxy: Growth Optimisation and Effects of Si Doping

Growth of In0.52Al0.48As epilayers on InP (100) substrates by molecular beam epitaxy at a wide range of substrate tempreatures (470~550℃) and at different Si doping levels has been carried out. Low temperature photoluminescence (PL) and double-axis X-ray diffraction (XRD) analyses shaw a strong dependence of the PL and XRD linewidths, XRD intensity ratio (Lepi/Isub), and lattice-mismatch on the substrate temperature. The X-ray diffraction peaks of samples grown at law temperatures show a composition of smaller peaks, indicating the presence of disorder due to alloy clustering. Raman scattering measurements of the same samples show an additional higher energy mode at 273 cm-1 in addition to the InAs-like and AlAs-like longitudinal-optic (LO) phonon modes. Samples doped with Si show an inverted S-shaped dependence of the PL peak energy variation with the temperature which weakens at high doping levels due to a possible reduction in the donor binding energy. Supported be observations of a reduction in both the AlAs-like and InAs-like LO phonon frequencies and a broadening of the LO phonon line shape as the doping level is increased, the PL intensity also shows in increasing degrees at higher doping levels, a temperature dependence which is characteristic of disordered and amorphous materials.

Growth and Characterization of AlInAs on InP Substrate by Molecular Beam Epitaxy

AlxIn1-xAs with 0.47&lex&le0.62 onto (100) oriented InP substrate was grown by molecular beam epitaxy (MBE) and characterized with X-ray double crystal diffraction, low temperature photoluminescence and an electron probe. Results show their high qualities. Strain and residual stress were studied in detail.

Growth of high-crystallinity uniform GaAs nanowire arrays by molecular beam epitaxy

The self-catalyzed growth of Ga As nanowires(NWs)on silicon(Si)is an effective way to achieve integration between group III–V elements and Si.High-crystallinity uniform Ga As NW arrays were grown by solid-source molecular beam epitaxy(MBE).In this paper,we describe systematic experiments which indicate that the substrate treatment is crucial to the highly crystalline and uniform growth of one-dimensional nanomaterials.The influence of natural oxidation time on the crystallinity and uniformity of Ga As NW arrays was investigated and is discussed in detail.The Ga As NW crystallinity and uniformity are maximized after 20 days of natural oxidation time.This work provides a new solution for producing high-crystallinity uniform III–V nanowire arrays on wafer-scale Si substrates.The highly crystalline uniform NW arrays are expected to be useful for NW-based optical interconnects and Si platform optoelectronic devices.

Molecular beam epitaxy and superconductivity of stoichiometric FeSe and K_x Fe_(2-y)Se_2 crystalline films

Our recent progress in the fabrication of FeSe and KxFe2_ySe2 ultra thin films and the understanding of their superconductivity properties is reviewed. The growth of high-quality FeSe and KxFe2_ySe2 films is achieved in a well controlled manner by molecular beam epitaxy. The high-quality stoichiometric and superconducting crystalline thin films allow us to investigate the intrinsic superconductivity properties and the interplay between the superconductivity and the film thickness, the local structure, the substrate, and magnetism. In situ low-temperature scanning tunneling spectra reveal the nodes and the twofold symmetry in FeSe, high-temperature superconductivity at the FeSe/SrTiO3 interface, phase separation and magnetic order in KxFe2_ySe2, and the suppression of superconductivity by twin boundaries and Fe vacancies. Our findings not only provide fundamental information for understanding the mechanism of unconventional superconductivity, but also demonstrate a powerful way of engineering superconductors and raising the transition temperature.

Growth and structural characteristics of metastableβ-In2Se3 thin films on H-terminated Si(111)substrates by molecular beam epitaxy

Epitaxial growth and structural characteristics of metastableβ-In2Se3 thin films on H-terminated Si(111)substrates are studied.The In2Se3 thin films grown below theβ-to-αphase transition temperature(453 K)are characterized to be strainedβ-In2Se3 mixed with significantγ-In2Se3 phases.The pure-phased single-crystallineβ-In2Se3 can be reproducibly achieved by in situ annealing the as-deposited poly-crystalline In2Se3 within the phase equilibrium temperature window ofβ-In2Se3.It is suggeted that the observedγ-to-βphase transition triggered by quite a low annealing temperature should be a rather lowered phase transition barrier of the epitaxy-stabilized In2Se3 thin-film system at a state far from thermodynamic equilibrium.

Effects of N_2 Pressure on the Structural and Electrical Properties of TiN Films Deposited by Laser Molecular Beam Epitaxy

Titanium nitride （TiN） films were deposited on Si（100） substrates by laser molecular beam epitaxy（LMBE）,and their properties of structure and resistivity with varying N2 pressure were investigated.The results showed that atomically flat TiN films with layer-by-layer growth mode were successfully grown on Si（100） substrates,and （200） was the preferred orientation.With the increasing of N2 pressure,the N/Ti ratio gradually increased and the diffraction peak progressively shifted towards lower diffraction angle.At pressure of 0.1 Pa,stoichiometric TiN film was formed which exhibited the characteristic diffraction angle of （200） plane.All films showed high reflectance to infrared spectrum and the films with overstoichiometry and understoichiometry had a higher resistivity owing to the surface particles and lattice distortion,while the stoichiometric TiN film depicted the minimum resistivity,around 19 μΩ·cm.