High-resolution X-ray Reciprocal Space Research Articles

Formation of strain reduced In0.54Al0.34Ga0.12As layer of vertically coupled QDs arrays for O-band telecom single photon sources

We demonstrate the correlative research on the multi-stacked vertically coupled InAs quantum dots (VCQDs) capped by 15 nm combinational capping layer of In(0.21)Al(0.21)Ga(0.58)As and GaAs layer through Atom probe tomography (APT), Transmission Electron Microscopy (TEM), Secondary Ion Mass Spectroscopy (SIMS), High-Resolution X-Ray Diffraction (HRXRD) and Reciprocal Space Mapping (RSM). From the comparative studies, we observed a strain reduction of ∼ 2.3 ± 0.05% in the system, leading to the formation of strain-reduced (SR) In0.54Al0.34Ga0.12As layer with a lattice constant of 5.88 Å, which will work as a shielding layer. We found that the middle portion of the 3rd to 8th layer QDs structure was constant in size, shape, composition, and density, which enhances the carrier confinement in QDs. The computed strain energy values contributed to the overall growth structure of the 30 - layers VCQDs were recorded to be 2.2 meV/atoms. We report the detailed analogy of the in-out flow of In/Ga adatoms in the In0.54Al0.34Ga0.12As layer leading to the evolution of fully developed bigger InAs QDs size. To support the APT results, we also present the outcomes studies of the HRXRD Out-plane and In-Plane symmetric RSM experiment at (002), (004), and (006) reflections to investigate the compressive strain contribution in the SR In0.54Al0.34Ga0.12As shielding layer. This 30-layer VCQDs structure can be employed to fabricate high thermal stability operating at 1.3 µm O-band telecom Single Photon Sources (SPSs).

Properties of topological crystalline insulator Pb0.5Sn0.5Te epitaxial films doped with bismuth

We report here on the properties of topological crystalline insulator Pb0.5Sn0.5Te epitaxial films doped with bismuth at levels from 0% (undoped) to 0.15%. The undoped film exhibits a p-type character due to metal vacancies. As the doping level rises, the hole concentration reduces. At a level of 0.06%, the electrical character inverts to n-type and the electron density continues to increase for rising doping level up to 0.15%. This result demonstrates an effective extrinsic n-type doping of Pb0.5Sn0.5Te crystal with bismuth due to substitutional Bi atoms in metal sites. High-resolution x-ray diffraction and reciprocal space mapping show that fully relaxed high-quality films are obtained. A pristine (111) film surface is revealed after removal of the Te cover layer using a method combining Ar+ sputtering and thermal desorption. Angle-resolved photoemission spectroscopy (ARPES) data acquired at 30 K near the Γ¯ point of the undoped film surface show a parabolic-like dispersion of the bulk valence band close to the Fermi level. Now, the ARPES data for a sample doped with 0.1% of Bi reveal that the chemical potential is shifted by 40 meV upwards in the direction of the conduction band. The ARPES results also indicate that there might be a discrepancy between surface and bulk chemical potential in the doped sample. This divergence suggests that Te atoms diffuse into the surface during the thermal process to desorb the protective layer, inverting the surface to p-type.

Bulk heterogeneity in barium titanate above the Curie temperature

We use dark-field x-ray microscopy to reveal evidence of subtle structural heterogeneity in BaTiO3 single crystals at temperatures of 150 °C—well above the Curie temperature of 125 °C. The heterogeneity exhibits domain-like ordering on the scale of several micrometers, pronounced curvature, and a preference for ⟨110⟩ lattice directions. Complementary high-resolution x-ray reciprocal space measurements suggest that the features originate from point defects (most likely oxygen vacancies) that coalesce along pre-existing domain walls during aging. A simple thermodynamic model suggests that the weak elastic strains associated with the heterogeneity are likely to locally raise the Curie temperature in their vicinity, creating nucleation sites for the ferroelectric phase upon cooling through the ferroelectric phase transition.

Design and growth of InAsP metamorphic buffers for InGaAs thermophotovoltaic cells

The structural and optical properties of InAsxP1-x metamorphic buffers grown by metal–organic chemical vapor deposition on InP (100) substrates have been investigated. High-resolution X-ray reciprocal space mapping around the (115) InP lattice point reveals that the strain relaxations of the InAsxP1-x with x = 0.5, 0.55, and 0.7 are 98%, 92%, and 96%, while the lateral correlation lengths are 17, 62, and 28 nm, respectively. The optical bandgap energy of the InAsP derived from photoreflectance (PR) measurements decreases from 0.819 to 0.621 eV at 300 K when increasing As composition from x = 0.5 to 0.7. The bowing parameter for the optical bandgap of the InAsP is increased with increasing As composition, which is attributable to the increased spontaneous CuPt-type ordering in InAsP. It is found from the excitation power-dependent PR measurement that the InAsxP1-x layers have different degrees of the bandgap redshift due to the reduced thermal conductivity caused by crystal imperfections generated during the strain relaxation process.

Interface-driven magnetic anisotropy in relaxed La0.7Sr0.3CrO3/La0.7Sr0.3MnO3 heterostructures on MgO

We investigate the structural and magnetic properties of La0.7Sr0.3CrO3 (LSCO)/La0.7Sr0.3MnO3 (LSMO) heterostructures grown on (001)-oriented MgO by molecular beam epitaxy. Due to the large film-substrate lattice mismatch, strain relaxation is found to occur within the first 2–3 unit cells (uc) of the film as evidenced by reflection high energy electron diffraction and high-resolution synchrotron x-ray reciprocal space mapping. We find that the presence of the LSCO spacer and capping layers leads to ferromagnetism in ultra-thin LSMO layers with thicknesses of the order of 2 uc with the magnetic easy axis oriented in the film plane. Net magnetic moments of 1.4 and 2.4 μB/Mn are measured for (2 uc LSCO/2 uc LSMO) and (2 uc LSCO/4 uc LSMO) superlattices, respectively, by superconducting quantum interference device magnetometry. The effective magnetic anisotropy of the relaxed (2 uc LSCO/4 uc LSMO) heterostructure is found to be an order of magnitude higher than bulk LSMO highlighting the critical role of interfacial interactions in tuning magnetic anisotropy at complex oxide interfaces.

Influence of Growth Temperature of the Nucleation Layer on the Growth of InP on Si (001)

InP layers grown on Si (001) were achieved by the two-step growth method using gas source molecular beam epitaxy. The effects of growth temperature of nucleation layer on InP/Si epitaxial growth were investigated systematically. Cross-section morphology, surface morphology and crystal quality were characterized by scanning electron microscope images, atomic force microscopy images, high-resolution X-ray diffraction (XRD), rocking curves and reciprocal space maps. The InP/Si interface and surface became smoother and the XRD peak intensity was stronger with the nucleation layer grown at 350 °C. The Results show that the growth temperature of InP nucleation layer can significantly affect the growth process of InP film, and the optimal temperature of InP nucleation layer is required to realize a high-quality wafer-level InP layers on Si (001).

Strain-stress study of AlxGa1\u2212xN/AlN heterostructures on c-plane sapphire and related optical properties

This work presents a systematic study of stress and strain of AlxGa1−xN/AlN with composition ranging from GaN to AlN, grown on a c-plane sapphire by metal-organic chemical vapor deposition, using synchrotron radiation high-resolution X-ray diffraction and reciprocal space mapping. The c-plane of the AlxGa1−xN epitaxial layers exhibits compressive strain, while the a-plane exhibits tensile strain. The biaxial stress and strain are found to increase with increasing Al composition, although the lattice mismatch between the AlxGa1−xN and the buffer layer AlN gets smaller. A reduction in the lateral coherence lengths and an increase in the edge and screw dislocations are seen as the AlxGa1−xN composition is varied from GaN to AlN, exhibiting a clear dependence of the crystal properties of AlxGa1−xN on the Al content. The bandgap of the epitaxial layers is slightly lower than predicted value due to a larger tensile strain effect on the a-axis compared to the compressive strain on the c-axis. Raman characteristics of the AlxGa1−xN samples exhibit a shift in the phonon peaks with the Al composition. The effect of strain on the optical phonon energies of the epitaxial layers is also discussed.

Liquid Phase Epitaxy growth of Tm3+-doped CaF2 thin-films based on LiF solvent

Single-crystalline Tm3+-doped calcium fluoride (Tm3+:CaF2) films were grown onto (100) oriented undoped bulk CaF2 substrates by Liquid Phase Epitaxy method using LiF as a solvent. The growth was performed at the temperatures of 853–865 °C. Crack-free transparent films with a high doping concentration of ∼6 at.% and a thickness up to ∼100 μm were obtained. The film structure and morphology were characterized by confocal microscopy, X-ray diffraction and scanning electron microscopy. High resolution X-ray diffraction and reciprocal space mapping confirmed the high crystallinity and the low mosaicity of the films. Energy-Dispersive X-ray spectroscopy revealed a uniform distribution of Tm3+ ions in the films. The Tm3+:CaF2 films exhibit a broadband emission at ∼2 μm and are of interest for waveguide lasers. The use of CaF2–LiF binary system is also promising for fabrication of other rare-earth-doped CaF2 layers.

Highly polarized photoluminescence from c-plane InGaN/GaN multiple quantum wells on stripe-shaped cavity-engineered sapphire substrate

Highly polarized photoluminescence (PL) from c-plane InGaN/GaN multiple quantum wells (MQWs) grown on stripe-shaped cavity-engineered sapphire substrate (SCES) was realized. The polarization ratio was as high as 0.74 at room temperature. High-resolution X-ray reciprocal space mapping measurements revealed that the InGaN quantum wells on GaN/SCES template were under considerable anisotropic in-plane strain states of −1.178% and −1.921% along the directions perpendicular and parallel to the stripe-pattern, respectively. The anisotropic strain states were attributed to the anisotropic alignment of cavity-incorporated sapphire nano-membranes, which accommodated both anisotropic elastic relaxation in the InGaN quantum well plane as well as the graded elastic relaxation along the vertical direction in the GaN template adjacent to the InGaN/GaN MQWs. The partial strain relaxation in the InGaN wells also contributed to reduction of quantum confined Stark effect, resulting in four times higher PL intensity than InGaN/GaN MQWs on planar sapphire substrate. From theoretical calculations based on k∙p perturbation theory, it was found that fundamental origin of the polarized optical emission was strain-induced modification of valence band structures of the InGaN/GaN MQWs on the SCES. This study will allow us to realize light emitting diodes with highly polarized emission with conventional c-plane sapphire substrates by strain-induced valence band modification.

Optimization of MBE Growth Conditions of In0.52Al0.48As Waveguide Layers for InGaAs/InAlAs/InP Quantum Cascade Lasers.

We investigate molecular beam epitaxy (MBE) growth conditions of micrometers-thick In0.52Al0.48As designed for waveguide of InGaAs/InAlAs/InP quantum cascade lasers. The effects of growth temperature and V/III ratio on the surface morphology and defect structure were studied. The growth conditions which were developed for the growth of cascaded In0.53Ga0.47As/In0.52Al0.48As active region, e.g., growth temperature of Tg = 520 °C and V/III ratio of 12, turned out to be not optimum for the growth of thick In0.52Al0.48As waveguide layers. It has been observed that, after exceeding ~1 µm thickness, the quality of In0.52Al0.48As layers deteriorates. The in-situ optical reflectometry showed increasing surface roughness caused by defect forming, which was further confirmed by high resolution X-ray reciprocal space mapping, optical microscopy and atomic force microscopy. The presented optimization of growth conditions of In0.52Al0.48As waveguide layer led to the growth of defect free material, with good optical quality. This has been achieved by decreasing the growth temperature to Tg = 480 °C with appropriate increasing V/III ratio. At the same time, the growth conditions of the cascade active region of the laser were left unchanged. The lasers grown using new recipes have shown lower threshold currents and improved slope efficiency. We relate this performance improvement to reduction of the electron scattering on the interface roughness and decreased waveguide absorption losses.

Epitaxial strain adaptation in chemically disordered FeRh thin films

Strain and strain adaption mechanisms in modern functional materials are of crucial importance for their performance. Understanding these mechanisms will advance innovative approaches for material properties engineering. Here we study the strain adaption mechanism in a thin film model system as function of epitaxial strain. Chemically disordered FeRh thin films are deposited on W-V buffer layers, which allow for large variation of the preset lattice constants, e.g. epitaxial boundary condition. It is shown by means of high resolution X-ray reciprocal space maps and transmission electron microscopy that the system reacts with a tilting mechanism of the structural units in order to adapt to the lattice constants of the buffer layer. This response explained by density functional theory calculations, which evidence an energetic minimum for structures with a distortion of c/a =0.87. The experimentally observed tilting mechanism is induced by this energy gain and allows the system to remain in the most favorable structure. In general, it is shown that the use of epitaxial model heterostructures consisting of alloy buffer layers of fully miscible elements and the functional material of interest allows to study strain adaption behaviors in great detail. This approach makes even small secondary effects observable, such as the directional tilting of the structural domains identified in the present case study.

Terahertz excitation spectra of GaAsBi alloys

Terahertz excitation spectroscopy was used for the determination of energy separation between the main (Γ) and subsidiary (L and X) conduction band valleys of GaAs1−xBix. The samples used in this study were 1 µm–1.5 µm thick bismide layers grown by Molecular Beam Epitaxy on GaAs substrates. They contained up to 8% of bismuth as determined by high resolution x-ray diffraction (HR-XRD) and reciprocal space mapping (RSM), taking into account the layer relaxation. It was found that both subsidiary conduction band valleys at L and X points of the Brillouin zone move away from the conduction band minimum at rates of 18 meV/%Bi and 25 meV/%Bi, respectively, with increasing Bi content in the alloy.

Linearly polarized photoluminescence of anisotropically strained c-plane GaN layers on stripe-shaped cavity-engineered sapphire substrate

Anisotropic in-plane strain and resultant linearly polarized photoluminescence (PL) of c-plane GaN layers were realized by using a stripe-shaped cavity-engineered sapphire substrate (SCES). High resolution X-ray reciprocal space mapping measurements revealed that the GaN layers on the SCES were under significant anisotropic in-plane strain of −0.0140% and −0.1351% along the directions perpendicular and parallel to the stripe pattern, respectively. The anisotropic in-plane strain in the GaN layers was attributed to the anisotropic strain relaxation due to the anisotropic arrangement of cavity-incorporated membranes. Linearly polarized PL behavior such as the observed angle-dependent shift in PL peak position and intensity comparable with the calculated value based on k·p perturbation theory. It was found that the polarized PL behavior was attributed to the modification of valence band structures induced by anisotropic in-plane strain in the GaN layers on the SCES.

In-Plane Anisotropic Photoconduction in Nonpolar Epitaxial a-Plane GaN.

Nonpolar a-plane GaN epitaxial films were grown on an r-plane sapphire using the plasma-assisted molecular beam epitaxy system, with various nitrogen plasma power conditions. The crystallinity of the films was characterized by high-resolution X-ray diffraction and reciprocal space mapping. Using the X-ray "rocking curve-phi scan", [0002], [1-100], and [1-102] azimuth angles were identified, and interdigitated electrodes along these directions were fabricated to evaluate the direction-dependent UV photoresponses. UV responsivity ( R) and internal gain ( G) were found to be dependent on the azimuth angle and in the order of [0002] > [1-102] > [1-100], which has been attributed to the enhanced crystallinity and lowest defect density along [0002] azimuth. The temporal response was very stable irrespective of growth conditions and azimuth angles. Importantly, response time, responsivity, and internal gain were 210 ms, 1.88 A W-1, and 648.9%, respectively, even at a bias as low as 1 V. The results were validated using the Silvaco Atlas device simulator, and experimental observations were consistent with simulated results. Overall, the photoresponse is dependent on azimuth angles and requires further optimization, especially for materials with in-plane crystal anisotropy.

Entirely relaxed lattice-mismatched GaSb/GaAs/Si(001) heterostructure grown via metalorganic chemical vapor deposition

A GaSb epilayer is grown on a GaAs/Si(001) epitaxial substrate via metalorganic chemical vapor deposition. High-resolution transmission electron microscopy micrographs and high-resolution X-ray reciprocal space mapping indicate an entirely relaxed interfacial misfit (IMF) array GaSb epilayer. The valence-band offset and conduction-band offset of the Al2O3/GaSb/GaAs/Si structure are estimated to be 2.39 and 3.65 eV, respectively. The fabricated Al2O3/p-GaSb/GaAs/Si MOS capacitors exhibited good capacitance–voltage characteristics with a small accumulation frequency dispersion of approximately 1.05% per decade. These results imply that the GaSb epilayer grown on the GaAs/Si platform in the IMF mode can be used for future complementary metal–oxide semiconductor applications.

In-line monitoring of strain distribution using high resolution X-ray Reciprocal space mapping into 20 nm SiGe pMOS

Together with the downscaling comes the introduction of new materials, such as strained SiGe, in order to boost the transistor performances. For an effective deployment it requires the implementation of methods capable to monitor the strain directly in the process lines. High Resolution X-Ray Diffraction has played a critical role in industry for thin films metrology purpose and have the potential to extend its capability to the strain characterization in the transistors. The latest industrial instruments provide fast and automatic measurement capabilities. This enables the use of Reciprocal Space Mapping (RSM), a key feature for strain characterization, as a monitoring method. To do so, automatic data extraction of RSMs is of course mandatory, so preliminary work performed on RSM treatment will be introduced in this paper. So far these studies have been carried out on nanostructures representative of transistor technologies and reveal innovative and conclusive results.

Anisotropic optical polarization dependence on internal strain in AlGaN epilayer grown on AlxGa1−xN templates

Anisotropic optical polarization of AlGaN has been one of the major challenges responsible for the poor efficiency of AlGaN-based ultraviolet light emitting diodes (UV LEDs). In this work, we experimentally investigated the effect of internal strain on the optical polarization of AlGaN epilayers which were pseudomorphically grown on AlxGa1−xN templates with Al composition changing from 0.1 to 0.42. High-resolution x-ray diffraction and reciprocal space mapping were conducted to determine the crystal quality and strain status. Polarization-dependent photoluminescence (PL) measurement was performed to study the degree of polarization (DOP) of light emission from lateral facet of the AlGaN epilayer. The result showed that the DOP increased from −0.69 to −0.24 with the in-plane strain changing from tensile status (1.19%) to compressive status (−0.70%) and it exhibited a strong dependence of the DOP on the strain. These results demonstrated that the compressive in-plane strain could facilitate TE mode emission from AlGaN, which providing a potential way to enhance the surface light emission of AlGaN-based UV LEDs via strain management of the active region.

InxGa1−xN/GaN Multiple Quantum Well Solar Cells with Conversion Efficiency of 3.77%**Supported by the National Basic Research Program of China (No 2012CB619303), and the National High-Technology Research and Development Program of China (No 2011AA050514).

We report on fabrication and photovoltaic characteristics of InxGa1−xN/GaN multiple quantum well solar cells with different indium compositions and barrier thicknesses. The as-grown samples are characterized by high-resolution x-ray diffraction and reciprocal space mapping. The results show that the sample with a thick barrier thickness (10.0nm) and high indium composition (0.23) has better crystalline quality. In addition, the dark current density-voltage (J–V) measurement of this device shows a significant decrease of leakage current, which leads to high open-circuit voltage Voc. Through the J–V characteristics under an Air Mass 1.5 Global (AM 1.5 G) illumination, this device exhibits a Voc of 1.89 V, a short-circuit current density Jsc of 3.92 mA/cm2 and a fill factor of 50.96%. As a result, the conversion efficiency (η) is enhanced to be 3.77% in comparison with other devices.

Critical thickness for strain relaxation of Ge1−xSnx (x ≤ 0.17) grown by molecular beam epitaxy on Ge(001)

We investigated the critical thickness (hc) for plastic relaxation of Ge1−xSnx grown by molecular beam epitaxy. Ge1−xSnx films with various Sn mole fraction x (x ≤ 0.17) and different thicknesses were grown on Ge(001). The strain relaxation of Ge1−xSnx films and the hc were investigated by high-resolution x-ray diffraction and reciprocal space mapping. It demonstrates that the measured hc values of Ge1−xSnx layers are as much as an order of magnitude larger than that predicted by the Matthews and Blakeslee (M-B) model. The People and Bean (P-B) model was also used to predict the hc values in Ge1−xSnx/Ge system. The measured hc values for various Sn content follow the trend, but slightly larger than that predicted by the P-B model.

Lattice-Matched InGaAs-InAlAs Core-Shell Nanowires with Improved Luminescence and Photoresponse Properties.

Core–shell nanowires (NW) have become very prominent systems for band engineered NW heterostructures that effectively suppress detrimental surface states and improve performance of related devices. This concept is particularly attractive for material systems with high intrinsic surface state densities, such as the low-bandgap In-containing group-III arsenides, however selection of inappropriate, lattice-mismatched shell materials have frequently caused undesired strain accumulation, defect formation, and modifications of the electronic band structure. Here, we demonstrate the realization of closely lattice-matched radial InGaAs–InAlAs core–shell NWs tunable over large compositional ranges [x(Ga)∼y(Al) = 0.2–0.65] via completely catalyst-free selective-area molecular beam epitaxy. On the basis of high-resolution X-ray reciprocal space maps the strain in the NW core is found to be insignificant (ε < 0.1%), which is further reflected by the absence of strain-induced spectral shifts in luminescence spectra and nearly unmodified band structure. Remarkably, the lattice-matched InAlAs shell strongly enhances the optical efficiency by up to 2 orders of magnitude, where the efficiency enhancement scales directly with increasing band offset as both Ga- and Al-contents increase. Ultimately, we fabricated vertical InGaAs−InAlAs NW/Si photovoltaic cells and show that the enhanced internal quantum efficiency is directly translated to an energy conversion efficiency that is ∼3–4 times larger as compared to an unpassivated cell. These results highlight the promising performance of lattice-matched III–V core–shell NW heterostructures with significant impact on future development of related nanophotonic and electronic devices.