X-ray Reciprocal Space Mapping Research Articles

Pinpointing lattice-matched conditions for wurtzite ScxAl1−xN/GaN heterostructures with x-ray reciprocal space analysis

Using comprehensive x-ray reciprocal space mapping, we establish the precise lattice-matching composition for wurtzite ScxAl1−xN layers on (0001) GaN to be x = 0.14 ± 0.01. 100 nm thick ScxAl1−xN films (x = 0.09–0.19) were grown in small composition increments on c-plane GaN templates by plasma-assisted molecular beam epitaxy. The alloy composition was estimated from the fit of the (0002) x-ray peak positions, assuming the c-lattice parameter of ScAlN films coherently strained on GaN increases linearly with Sc-content determined independently by Rutherford backscattering spectrometry [Dzuba et al., J. Appl. Phys. 132, 175701 (2022)]. Reciprocal space maps obtained from high-resolution x-ray diffraction measurements of the (101¯5) reflection reveal that ScxAl1−xN films with x = 0.14 ± 0.01 are coherently strained with the GaN substrate, while the other compositions show evidence of relaxation. The in-plane lattice-matching with GaN is further confirmed for a 300 nm thick Sc0.14Al0.86N layer. The full-width-at-half-maximum of the (0002) reflection rocking curve for this Sc0.14Al0.86N film is 106 arc sec and corresponds to the lowest value reported in the literature for wurtzite ScAlN films.

Crystallographic and band structure analysis of β-(AlxGa1−x)2O3/β-(InyGa1−y)2O3 thin film grown on β-Ga2O3 substrate via mist CVD

We successfully achieved the growth of a stacked layer composed of β-(AlxGa1−x)2O3/β-(InyGa1−y)2O3 on a (010) β-Ga2O3 substrate using mist chemical vapor deposition (CVD). X-ray diffraction and reciprocal space mapping analyses were conducted, elucidating that the multilayer structure of the β-(AlxGa1−x)2O3/β-(InyGa1−y)2O3 thin film exhibited excellent crystallinity and coherent growth. Scanning transmission electron microscopy further revealed a continuous atomic arrangement at the heterointerface of β-(AlxGa1−x)2O3/β-(InyGa1−y)2O3. Furthermore, the bandgap values of β-(AlxGa1−x)2O3 and β-(InyGa1−y)2O3 thin films were determined to be 5.21 and 4.62 eV, respectively, through electron energy-loss spectroscopy. Notably, a slight broadening was observed in the bandgap transition at the interface of β-(AlxGa1−x)2O3/β-(InyGa1−y)2O3. Energy dispersive x-ray spectroscopy analysis indicated that this phenomenon could be attributed to the diffusion of In into the β-(AlxGa1−x)2O3 thin film layer. These results support mist CVD as a promising growth technique for developing β-Ga2O3-based heterojunction devices.

Dynamical and kinematical X-ray diffraction in a bent crystal

Numerical modeling of kinematical and dynamical X-ray diffraction in a bent crystal was performed on the basis of two approaches to integrating the Takagi–Taupin equations, and using two-dimensional recurrence relations. Within the framework of kinematical diffraction, a new equation is obtained that describes the distribution of diffracted intensity inside a bent crystal. The time taken for numerical calculations based on this equation is significantly reduced in comparison with the use of algorithms of the dynamical diffraction theory. The simulation shows for the first time that, for strongly bent crystals, the maximum value of the diffraction intensity is formed inside the deformed structure and not on its surface. In the case of strong bending of the crystal structure, the deviation of the X-ray beam from the Bragg angle does not change the diffraction pattern but shifts it along the lateral direction. The results of calculations of diffraction in a strongly bent crystal based on the equations of dynamical and kinematical diffraction coincide, while the computations for weakly bent crystals differ. The possibility of estimating the primary extinction length of a bent crystal as a function of the bending radius is shown. In the case of kinematical diffraction in bent crystalline microsystems, a new method has been developed to calculate X-ray reciprocal-space mapping.

X-ray reciprocal space mapping analysis of ferromagnetic GdN films grown by pulsed laser epitaxy

Epitaxial thin films of ferromagnetic rare-earth nitride, GdN, were synthesized using pulsed laser deposition (PLD) on (001) MgO, pseudo-cubic (001) YAlO3, and (001) TiN buffered (001) MgO substrates. X-ray high-resolution reciprocal space mappings confirmed the epitaxial relationship between GdN and the substrates. The use of a TiN buffer layer changed the growth direction of the GdN films from (001) to (111). The ferromagnetic behavior of the films was characterized, and it was found that the magnetic easy axis could be tuned according to the crystal growth direction. These results suggest that PLD is a viable method for synthesizing epitaxial GdN films with tunable magnetic properties. The ability to control the crystal growth direction and magnetic easy axis of GdN films could be useful for developing spintronic devices.

Orbital ordering and ultrafast carrier dynamics anisotropies in orientation-engineered orthorhombic YMnO3 films

The rich physical properties unveiled in a plethora of transition and rare-earth metal oxides have been attributed to the intricate interplays between the orbital, charge, and spin degrees of freedom. Among them, rare-earth manganites (RMnO3) have been attracting tremendous attention owing to the ionic size-induced lattice distortion dictated by the Goldschmidt tolerance factor and the substantial Jahn–Teller distortion unique to Mn3+ ions, which evidently have resulted in a variety of emergent characteristics in electronic, magnetic, and orbital ordering. In this work, we deliberately engineered the orientation of a series of orthorhombic YMnO3 (o-YMO) films grown on SrTiO3(100) [STO(100)] and SrTiO3(110) [STO(110)] substrates by means of pulsed laser deposition. The x-ray diffraction (XRD) and reciprocal space mapping revealed that o-YMO/STO(100) is c-axis-oriented and o-YMO/STO(110) is a-axis-oriented, respectively. The XRD ϕ-scans further indicate that both films have excellent in-plane crystallinity, allowing the exploration of anisotropies along the respective crystallographic orientations. Indeed, the x-ray absorption linear dichroism spectroscopy taken along the respective crystallographic orientations evidently exhibited substantial anisotropy. Theoretical fitting with configuration interaction cluster calculations suggests that the d3z2−r2 orbitals are parallel to YMO[001]/(100), leading to stronger electron scattering along the c-axis. Independent polarization-dependent Δ R/R spectra obtained using the femtosecond pump–probe method exhibited substantial anisotropic behaviors in carrier relaxation dynamics when probing along different crystallographic orientations, presumably due to orbital ordering anisotropies.

Perpendicular magnetic anisotropy in Bi-substituted yttrium iron garnet films

Magnetic garnet thin films exhibiting perpendicular magnetic anisotropy (PMA) and ultra-low damping have recently been explored for applications in magnonics and spintronics. Here, we present a systematic study of PMA and magnetic damping in bismuth-substituted yttrium iron garnet (Bi-YIG) films grown on sGGG (111) substrates by pulsed laser deposition. Films with thicknesses ranging from 5 to 160 nm are investigated. Structural characterization using x-ray diffraction and reciprocal space mapping demonstrates the pseudomorphic growth of the films. The films exhibit perpendicular magnetic anisotropy up to 160 nm thickness, with the zero-magnetic field state changing from fully saturated for low thicknesses to a dense magnetic stripe pattern for thicker films. The films show a ferromagnetic resonance (FMR) linewidth of 100–200 MHz with a Gilbert damping constant of the order of 4×10−3. The broad FMR linewidth is caused by inhomogeneities of magnetic properties on micrometer length scales.

Analysis of strain in ion implanted 4H-SiC by fringes observed in synchrotron X-ray topography

A novel high energy implantation system has been successfully developed to fabricate 4H-SiC superjunction devices for medium and high voltage via implantation of dopant atoms with multi-energies ranging from 13 to 66 MeV. The significantly higher levels of energy used compared to conventional implantation processes, necessitates detailed characterization of the lattice damage caused by implantation. To achieve this by employing the novel high energy system, 4H-SiC wafer with 12 μm epilayers were blanket implanted by 13.8–65.7 MeV Al atoms. The lattice damages induced by the implantation were primarily characterized by Synchrotron X-ray Plane Wave Topography (SXPWT) and Reciprocal Space Mapping (RSM). Topographs reveal fringe contrast akin to multiple asymmetric diffraction peaks with an angular separation of only 2″ (arcseconds) observed on rocking curves, indicating inhomogeneous strain distribution across the implanted layer. The strain profile of the implanted layer was extracted from the fringe contrast by applying Rocking-curve Analysis by Dynamical Simulation (RADS). The maximum strain value is similar to that measured on the RSM.

Porous pseudo-substrates for InGaN quantum well growth: Morphology, structure, and strain relaxation

Strain-related piezoelectric polarization is detrimental to the radiative recombination efficiency for InGaN-based long wavelength micro-LEDs. In this paper, partial strain relaxation of InGaN multiple quantum wells (MQWs) on the wafer scale has been demonstrated by adopting a partially relaxed InGaN superlattice (SL) as the pseudo-substrate. Such a pseudo-substrate was obtained through an electro-chemical etching method, in which a sub-surface InGaN/InGaN superlattice was etched via threading dislocations acting as etching channels. The degree of strain relaxation in MQWs was studied by x-ray reciprocal space mapping, which shows an increase of the in-plane lattice constant with the increase of etching voltage used in fabricating the pseudo-substrate. The reduced strain in the InGaN SL pseudo-substrate was demonstrated to be transferable to InGaN MQWs grown on top of it, and the engineering of the degree of strain relaxation via porosification was achieved. The highest relaxation degree of 44.7% was achieved in the sample with the porous InGaN SL template etched under the highest etching voltage. Morphological and structural properties of partially relaxed InGaN MQWs samples were investigated with the combination of atomic force and transmission electron microscopy. The increased porosity of the InGaN SL template and the newly formed small V-pits during QW growth are suggested as possible origins for the increased strain relaxation of InGaN MQWs.

Mechanically Robust Interface at Metal/Muscovite Quasi van der Waals Epitaxy.

Quasi van der Waals epitaxy is an approach to constructing the combination of 2D and 3D materials. Here, we quantify and discuss the 2D/3D interface structure and the corresponding features in metal/muscovite systems. High-resolution scanning transmission electron microscopy reveals the atomic arrangement at the interface. The theoretical results explain the formation mechanism and predict the mechanical robustness of these metal/muscovite quasi van der Waals epitaxies. The evidence of superior interface quality is delivered according to the outstanding performance of the designed systems in both retention (>105 s) and cycling tests (>105 cycles) through electromechanical measurements. With high-temperature X-ray reciprocal space mapping, the unique anisotropy of thermal expansion is discovered and predicted to sustain the thermal stress with a sizable thermal actuation. A maximum bending curvature of 264 m-1 at 243 °C can be obtained in the silver/muscovite heteroepitaxy. The electrothermal and photothermal methods show a fast response to thermal stress and demonstrate the interface robustness.

SiGeSn buffer layer for the growth of GeSn films

Inclusion of Si atoms to the growth surface during the molecular beam epitaxy of Ge and Sn to form a SiGeSn alloy was identified as a reactive surface species and as a means to compensate strain, which allowed for the subsequent growth of GeSn alloys with high Sn content. The development of a SiGeSn virtual substrate having a 15% Sn concentration and lattice parameter larger than 5.72 Å is demonstrated, using atomic force microscopy, x-ray reciprocal space mapping, and transmission electron microscopy, as a method for the direct growth of thick (>500 nm) fully relaxed GeSn alloys with greater than 10% Sn. This buffer layer enables the monolithic integration of GeSn with silicon for optoelectronic applications, as the SiGeSn virtual substrate allows for selective chemical etching of GeSn, which is important for device fabrication.

Improved polarization retention in epitaxial BiFeO3 thin films induced by strain relaxation

This study investigated the impact of lattice mismatch strain (LMS) on the polarization retention of epitaxial ferroelectric BiFeO3 (BFO) thin films. The application of varying degrees of LMS on the BFO films was achieved by tuning the film thickness, which was verified through X-ray diffraction and reciprocal space mapping. As the strain was gradually eliminated, the film demonstrated a more saturated hysteresis loop with a reduced negative coercive electric field. Additionally, a significant increase in polarization retention was observed with increasing film thickness, strongly indicating the crucial role of LMS in driving the formation of preferred polarization, which is intimately connected with the built-in field induced by oxygen vacancies-relevant space charge alignment. Moreover, the anisotropic LMS state of the BFO films was utilized to horizontally reverse local polarization in a sub-micrometer scale, revealing that strain accelerates the back-switching of polarization to eliminate the artificially created ferroelastic domain walls. To counteract the strain effect, charge injection of electrons was proposed to enhance the retention of switched polarization by fully suppressing the built-in field and pinning the artificially created domain walls. The findings provide valuable insights into the impact of strain on polarization retention for the development of ferroelectric memories.

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).

Combining x-ray real and reciprocal space mapping techniques to explore the epitaxial growth of semiconductors

In the present work, the importance of determining the strain states of semiconductor compounds with high accuracy is demonstrated. For the matter in question, new software titled LAPAs, the acronym for LAttice PArameters is presented. The lattice parameters as well as the chemical composition of Al1−x In x N and Ge1−x Sn x compounds grown on top of GaN- and Ge- buffered c-Al2O3 and (001) oriented Si substrates, respectively, are calculated via the real space Bond’s method. The uncertainties in the lattice parameters and composition are derived, compared and discussed with the ones found via x-ray diffraction reciprocal space mapping. Broad peaks lead to increased centroid uncertainty and are found to constitute up to 99% of the total uncertainty in the lattice parameters. Refraction correction is included in the calculations and found to have an impact of 0.001 Å in the lattice parameters of both hexagonal and cubic crystallographic systems and below 0.01% in the quantification of the InN and Sn contents. Although the relaxation degrees of the nitride and tin compounds agree perfectly between the real and reciprocal-spaces methods, the uncertainty in the latter is found to be ten times higher. The impact of the findings may be substantial for the development of applications and devices as the intervals found for the lattice match the condition of Al1−x In x N grown on GaN templates vary between ∼1.8% (0.1675–0.1859) and 0.04% (0.1708–0.1712) if derived via the real- and reciprocal spaces methods.

Room-temperature ferroelectric-like behavior in anatase TiO2 epitaxial films prepared by chemical solution deposition

Ferroelectrics of simple oxides have been of great interest due to they are easy to integrate with silicon semiconductors. The FE hysteresis loop was measured for the first time in pure anatase-phase titanium dioxide is reported, demonstrating that the ferroelectric-like behavior in a-TiO2 epitaxial thin films (7.5 nm to 228.8 nm) prepared by chemical solution deposition method on (001) SrTiO3 based substrates. Synchrotron based X-ray diffraction and reciprocal space mapping analysis prove that we have prepared high-quality epitaxial films. According to the results of the FE hysteresis loop, Pr can reach approximately 0.42 μC/cm2 in a-TiO2 film with a thickness of 14.5 nm. Furthermore, the PFM shows that the ferroelectric-like behavior is exhibited in a-TiO2 film of 7.5 nm and that the PFM polarization switch can be maintained for more than 100 min. All of these seem to indicate the presence of ferroelectric behavior in a-TiO2 films. We recognize that the origin of ferroelectric-like behavior is due to the distortion induced by strain and vacancy. However, since the polarization value is not very large and the PFM decays, the electrochemical effect has a non-negligible influence on the intrinsic ferroelectric performance.

Toward ultraclean correlated metal CaVO3

We report the synthesis and electronic properties of the correlated metal CaVO3, grown by hybrid molecular beam epitaxy. Films were grown on (100) LaAlO3 substrates at a temperature of 900 °C by supplying a flux of elemental Ca through a thermal effusion cell and metalorganic precursor, vanadium oxitriisopropoxide, as a source of vanadium. The presence of a self-regulated growth regime was revealed by the appearance of a specific surface reconstruction detected by reflection high-energy electron diffraction. Films grown within the growth window were characterized by atomically flat surfaces. X-ray reciprocal space maps revealed that the films were coherently strained to the substrate and inherited its twinned microstructure. Despite the presence of twin walls, CaVO3 thin films, grown within the stoichiometric growth window, revealed very low electrical resistivities at low temperatures, with residual resistivity ratios exceeding 90, while films grown at either Ca- or V-excess show deteriorated transport properties, attributed to the presence of extrinsic defects arising from the non-stoichiometry present in these films.

Emergent chirality in a polar meron to skyrmion phase transition

Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of −1) to a two-dimensional, tetratic lattice of merons (with topological charge of −1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). We show how scanning electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and phase-field simulations.

Large negative electrocaloric response induced by nanoscale phase transition in (Bi, Na)TiO3-based thin films

Electrocaloric effect (ECE) offers an efficient and environmentally friendly route for solid-state cooling. Either positive or negative ECE could exhibit a large adiabatic temperature change (ΔT). Compared to the positive electrocaloric response, the investigation of negative ECE is lagging behind, largely due to the fact that its origin is still elusive. In this work, the negative ECE behavior of conventional ferroelectric thin films, namely 0.94(Bi0.5Na0.5)TiO3-0.06BaTiO3 (BNBT), was studied. A remarkable ΔT of −26.1 K was acquired near 160 °C under a moderate electric field of 875 kV/cm, attributing to the ferroelectric phase transition in the polar nanoregions from rhombohedral (R3c) to tetragonal (P4bm), as confirmed by temperature-dependent dielectric permittivity, Raman spectra, and x-ray reciprocal space mapping. The BNBT thin film presents a high electrocaloric coefficient (ΔT/ΔE) of 0.0298 K cm kV−1, transcending that of the most reported negative electrocaloric response of thin films.

Coherent growth of β-(Al x Ga1−x )2O3 alloy thin films on (010) β-Ga2O3 substrates using mist CVD

Herein, we demonstrate β-(Al x Ga1−x )2O3 thin films that were coherently grown on a (010) β-Ga2O3 substrate using mist chemical vapor deposition (CVD). X-ray diffraction and reciprocal space mapping results revealed that the β-(Al x Ga1−x )2O3 thin films were of high-crystalline quality and were grown coherently to attain an Al content of 18.3% as measured by Rutherford backscattering spectroscopy. Importantly, based on their surface morphologies, the coherently grown β-(Al x Ga1−x )2O3 thin films have atomically flat surfaces. These results indicate that mist CVD is a promising technique for β-(Al x Ga1−x )2O3/β-Ga2O3 heterojunction devices.

Influence of growth temperature and miscut angle of m-plane sapphire substrate on the semi-polar (11–22) AlN film grown by HVPE

The high-quality semi-polar (11-22) AlN thin films were grown on m-plane sapphire substrates by hydride vapor phase epitaxy (HVPE). The surface morphology and crystalline quality of the AlN film were greatly influenced by the growth temperature and the substrate miscut angle. As the temperature increased, the grain size on the surface increased and the grain density decreased. In addition, the higher growth temperature also resulted in smaller values of the full width at half maximum (FWHM) of X-ray rocking curves (XRC) when temperature was more than 1,460 °C. At high temperature of 1,530 °C, the introduction of 1° -off miscut angle to the substrate resulted in smooth surface, low density of stacking faults and low FWHM of XRC. The misfit dislocation density was calculated from the tilt angle of epilayer measured by X-ray reciprocal space mappings along [−1−123] AlN. The misfit dislocation density of the sample grown on 1° -off substrates was 6.7 × 105 cm−2. The improvement of crystal quality is believed to be due to the enhancement of adatom mobility at higher temperatures and also the appropriate miscut variation.

Strain relaxation in epitaxial SrTi0.5Fe0.5 O[formula omitted] thin films on LaAlO3: An X-ray reciprocal space mapping study

SrTi0.5Fe0.5O3−δ (STF) has emerged as a promising cathode material for solid oxide fuel cells due to its excellent high ionic and electronic conductivity. We investigated the strain-state in epitaxial STF thin films on LaAlO3 (001) using synchrotron x-ray reciprocal space mapping measurement. The STF layer consists of two groups of compressively strained domains mixed horizontally in the film plane with a strain difference of about 1.4 %. The stress-free relaxed unit cell of more compressively strained domains, where a large degree of Sr segregation is expected, is relatively larger indicating that Sr segregation causes unit cell expansion. The lattice strain becomes gradually relaxed as the film thickness increases and the in-plane domain size decreases. We conjecture that the segregated Sr from compressively strained domains diffuse to the surface to form a layer of SrOx islands.