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The interest in metal halide perovskites has grown as impressive results have been shown in solar cells, light emitting devices, and scintillators, but this class of materials have a complex crystal structure that is only partially understood. In particular, the dynamics of the nanoscale ferroelastic domains in metal halide perovskites remains difficult to study. An ideal in situ imaging method for ferroelastic domains requires a challenging combination of high spatial resolution and long penetration depth. Here, we demonstrate in situ temperature-dependent imaging of ferroelastic domains in a single nanowire of metal halide perovskite, CsPbBr3. Scanning X-ray diffraction with a 60 nm beam was used to retrieve local structural properties for temperatures up to 140 °C. We observed a single Bragg peak at room temperature, but at 80 °C, four new Bragg peaks appeared, originating in different real-space domains. The domains were arranged in periodic stripes in the center and with a hatched pattern close to the edges. Reciprocal space mapping at 80 °C was used to quantify the local strain and lattice tilts, revealing the ferroelastic nature of the domains. The domains display a partial stability to further temperature changes. Our results show the dynamics of nanoscale ferroelastic domain formation within a single-crystal perovskite nanostructure, which is important both for the fundamental understanding of these materials and for the development of perovskite-based devices.

Semiconductor nanowires in wrapped, gate-all-around transistor geometry are highly favorable for future electronics. The advanced nanodevice processing results in strain due to the deposited dielectric and metal layers surrounding the nanowires, significantly affecting their performance. Therefore, non-destructive nanoscale characterization of complete devices is of utmost importance due to the small feature sizes and three-dimensional buried structure. Direct strain mapping inside heterostructured GaSb-InAs nanowire tunnel field-effect transistor embedded in dielectric HfO2, W metal gate layers, and an organic spacer is performed using fast scanning X-ray nanodiffraction. The effect of 10 nm W gate on a single embedded nanowire with segment diameters down to 40 nm is retrieved. The tensile strain values reach 0.26% in the p-type GaSb segment of the transistor. Supported by the finite element method simulation, we establish a connection between the Ar pressure used during the W layer deposition and the nanowire strain state. Thus, we can benchmark our models for further improvements in device engineering. Our study indicates, how the significant increase in X-ray brightness at 4th generation synchrotron, makes high-throughput measurements on realistic nanoelectronic devices viable.

Strain and interactions at grain boundaries during solid-phase crystallization are known to play a significant role in the functional properties of polycrystalline materials. However, elucidating three-dimensional nanoscale grain morphology, kinetics, and strain under realistic conditions is challenging. Here, we image a single-grain growth during the amorphous-to-polycrystalline transition in technologically relevant transparent conductive oxide (TCO) film of In2O3:Zr with in-situ Bragg coherent X-ray diffraction imaging and transmission electron microscopy. We find that the Johnson-Mehl-Avrami-Kolmogorov theory, which describes the average kinetics of polycrystalline films growth, can be applied to the single grains as well. The quantitative analysis stems directly from imaging results. We elucidate the interface-controlled nature of the single-grain growth in thin films and reveal the surface strains which may be a driving force for anisotropic crystallization rates. Our results bring in-situ imaging with coherent X-rays towards understanding and controlling the crystallization processes of TCOs and other polycrystalline materials at the nanoscale.

Ferroelectric and ferroelastic domains have been predicted to enhance metal halide perovskite (MHP) solar cell performance. While the formation of such domains can be modified by temperature, pressure, or strain, established methods lack spatial control at the level of single domains. Here, we induce the formation of ferroelastic domains in CsPbBr3 nanowires at room temperature using an atomic force microscope (AFM) tip and visualize the domains using nanofocused x-ray diffraction with a 60 nm beam. Regions scanned with a low AFM tip force show orthorhombic 004 reflections along the nanowire axis, while regions exposed to higher forces exhibit 220 reflections. The applied stress locally changes the crystal structure, leading to lattice tilts that define ferroelastic domains, which spread spatially and terminate at {112}-type domain walls. The ability to induce individual ferroelastic domains within MHPs using AFM gives new possibilities for device design and fundamental experimental studies.

Tuning of crystal structures and shapes of submicrometer-sized noble metals have revealed fascinating catalytic, optical, electrical, and magnetic properties that enable developments of environmentally friendly and durable nanotechnological applications. Several attempts have been made to stabilize Au, knowing its extraordinary stability in its conventional face-centered cubic (fcc) lattice, into different lattices, particularly to develop Au-based catalysis for industry. Here, we report the results from scanning X-ray diffraction microscopy (SXDM) measurements on an ambient-stable penta-twinned bipyramidal Au microcrystallite (about 1.36 μm in length and 230 nm in diameter) stabilized in noncubic lattice, exhibiting catalytic properties. With more than 82% of the crystal volume, the majority crystallite structure is identified as body-centered orthorhombic (bco), while the remainder is the standard fcc. A careful analysis of the diffraction maps reveals that the tips are made up of fcc, while the body contains mainly bco with very high strain. The reported structural imaging technique of representative single crystallite will be useful to investigate the growth mechanism of similar multiphase nano- and micrometer-sized crystals.

Journal of synchrotron radiation 27(5), 1121 - 1130 (2020). doi:10.1107/S1600577520007900, Modern subtractive and additive manufacturing techniques present new avenues for X-ray optics with complex shapes and patterns. Refractive phase plates acting as glasses for X-ray optics have been fabricated, and spherical aberration in refractive X-ray lenses made from beryllium has been successfully corrected. A diamond phase plate made by femtosecond laser ablation was found to improve the Strehl ratio of a lens stack with a numerical aperture (NA) of 0.88 × 10−3 at 8.2 keV from 0.1 to 0.7. A polymer phase plate made by additive printing achieved an increase in the Strehl ratio of a lens stack at 35 keV with NA of 0.18 × 10−3 from 0.15 to 0.89, demonstrating diffraction-limited nanofocusing at high X-ray energies., Published by Wiley-Blackwell, [S.l.]

Journal of synchrotron radiation 27(3), 625 - 632 (2020). doi:10.1107/S1600577520002192, The unique diagnostic possibilities of X-ray diffraction, small X-ray scattering and phase-contrast imaging techniques applied with high-intensity coherent X-ray synchrotron and X-ray free-electron laser radiation can only be fully realized if a sufficient dynamic range and/or spatial resolution of the detector is available. In this work, it is demonstrated that the use of lithium fluoride (LiF) as a photoluminescence (PL) imaging detector allows measuring of an X-ray diffraction image with a dynamic range of ∼107 within the sub-micrometre spatial resolution. At the PETRA III facility, the diffraction pattern created behind a circular aperture with a diameter of 5 µm irradiated by a beam with a photon energy of 500 eV was recorded on a LiF crystal. In the diffraction pattern, the accumulated dose was varied from 1.7 × 10$^5$ J cm$^{−3}$ in the central maximum to 2 × 10$^{−2}$ J cm$^{−3}$ in the 16th maximum of diffraction fringes. The period of the last fringe was measured with 0.8 µm width. The PL response of the LiF crystal being used as a detector on the irradiation dose of 500 eV photons was evaluated. For the particular model of laser-scanning confocal microscope Carl Zeiss LSM700, used for the readout of the PL signal, the calibration dependencies on the intensity of photopumping (excitation) radiation (λ = 488 nm) and the gain have been obtained., Published by Wiley-Blackwell, [S.l.]

Correction for ‘Strain mapping inside an individual processed vertical nanowire transistor using scanning X-ray nanodiffraction’ by Dmitry Dzhigaev et al., Nanoscale, 2020, 12, 14487–14493, DOI: 10.1039/D0NR02260H.

Applied Sciences 11(20), 9419 (2021). doi:10.3390/app11209419 special issue: "X-ray Technologies and Applications for Materials Structure & Properties Characterization", Semiconductor nanowires (NWs) have a broad range of applications for nano- andoptoelectronics. The strain field of gallium nitride (GaN) NWs could be signicantlychanged when contacts are applied to them to form a final device. Investigation ofinfluence of the metallic contacts on the structure of the NWs is of high importance fortheir applications in real devices. We have studied a series of different type of contactsand influence of the applied voltage bias on the contacted GaN NWs with the lengthof about 3 to 4 micrometers and with two different diameters of 200 nm and 350 nm.It was demonstrated that the NWs with the diameter of 200 nm are bend already bythe interaction with the substrate. For all GaN NWs, significant structural changeswere revealed after the contacts deposition. The results of our research may contributeto the future optoelectronic applications of the GaN nanowires., Published by MDPI, Basel

InAs

Nanotechnology 30(50), 505703 (2019). doi:10.1088/1361-6528/ab40f1, InAs x P1−x nanowires are promising building blocks for future optoelectronic devices and nanoelectronics. Their structure may vary from nanowire to nanowire, which may influence their average optoelectronic properties. Therefore, it is highly important for their applications to know the average properties of an ensemble of the nanowires. Structural properties of the InAs x P1−x -InP core–shell nanowires were investigated using the coplanar x-ray diffraction performed at a synchrotron facility. Studies of series of symmetric and asymmetric x-ray Bragg reflections allowed us to determine the 26% ± 3% of As chemical composition in the InAs x P1−x core, core–shell relaxation, and the average tilt of the nanowires with respect to the substrate normal. Based on the x-ray diffraction, scanning, and transmission electron microscopy measurements, a model of the core–shell relaxation was proposed. Partial relaxation of the core was attributed to misfit dislocations formed at the core–shell interface and their linear density was estimated to be 3.3 ± 0.3 × 104 cm−1., Published by IOP Publ., Bristol

Metal halide perovskites attract significant interest due to their remarkable performance in optoelectronic devices. However, the gap in understanding the relationship between their nanoscale structure and properties limits their application towards novel devices. In this work, twinned ferroelastic domains in single 500 nm CsPbBr3 particles are studied with 3D Bragg coherent x-ray diffraction imaging. A preferential double-domain structure is revealed in four identical particles, with one domain oriented along the [110] and the other along the [002] direction. The particles exhibit similar scattering volume ratios of 0.12 ± 0.026 between twin phases, suggesting the possibility of a deterministic formation process. The domains exhibit a difference in lattice tilt of 0.59 degrees, in excellent agreement with calculations of the lattice mismatch at the (112) twin boundary. These results provide important insights both for the fundamental understanding of ferroelastic nanoscale materials and for the performance improvement of perovskite-based devices. Moreover, this work paves the way towards real-time imaging of the domain dynamics in ferroic systems.

Nano letters 18(9), 5446 - 5452 (2018). doi:10.1021/acs.nanolett.8b01802, GaN nanowires (NWs) are promising building blocks for future optoelectronic devices and nanoelectronics. They exhibit stronger piezoelectric properties than bulk GaN. This phenomena may be crucial for applications of NWs and makes their study highly important. We report on an investigation of the structure evolution of a single GaN NW under an applied voltage bias along polar [0001] crystallographic direction until its mechanical break. The structural changes were investigated using coherent X-ray Bragg diffraction. The three-dimensional (3D) intensity distributions of the NWs without metal contacts, with contacts, and under applied voltage bias in opposite polar directions were analyzed. Coherent X-ray Bragg diffraction revealed the presence of significant bending of the NWs already after metal contacts deposition, which was increased at applied voltage bias. Employing analytical simulations based on elasticity theory and a finite element method (FEM) approach, we developed a 3D model of the NW bending under applied voltage. From this model and our experimental data, we determined the piezoelectric constant of the GaN NW to be about 7.7 pm/V in [0001] crystallographic direction. The ultimate tensile strength of the GaN NW was obtained to be about 1.22 GPa. Our work demonstrates the power of in operando X-ray structural studies of single NWs for their effective design and implementation with desired functional properties., Published by ACS Publ., Washington, DC

Physical review / E 98(5), 052703 (2018). doi:10.1103/PhysRevE.98.052703, Experimental and theoretical studies of a smectic-A–hexatic-B transition in freely suspended films of thickness 2 –10 $μm$ of the n-pentyl-4′−n-pentanoyloxy-biphenyl-4-carboxylate (54COOBC) compound are presented. X-ray investigations revealed a discontinuous first-order transition into the hexatic phase. The temperature region of two-phase coexistence near the phase transition point diminishes with decreasing film thickness. The width of this temperature region as a function of the film thickness was derived on the basis of a Landau mean-field theory in the vicinity of a tricritical point (TCP). Close to TCP the surface hexatic-B order penetrates anomalously deep into the film interior., Published by APS, Woodbury, NY

We present results of the studies of dynamics in colloidal crystals performed by pump-probe experiments using an X-ray free-electron laser (XFEL). Colloidal crystals were pumped with an infrared laser at a wavelength of 800 nm with varying power and probed by XFEL pulses at an energy of 8 keV with a time delay up to 1000 ps. The positions of the Bragg peaks, and their radial and azimuthal widths were analyzed as a function of the time delay. The spectral analysis of the data did not reveal significant enhancement of frequencies expected in this experiment. This allowed us to conclude that the amplitude of vibrational modes excited in colloidal crystals was less than the systematic error caused by the noise level.

The future of solid-state lighting can be potentially driven by applications of InGaN/GaN core-shell nanowires. These heterostructures provide the possibility for fine-tuning of functional properties by controlling a strain state between mismatched layers. We present a nondestructive study of a single 400 nm-thick InGaN/GaN core-shell nanowire using two-dimensional (2D) X-ray Bragg ptychography (XBP) with a nanofocused X-ray beam. The XBP reconstruction enabled the determination of a detailed three-dimensional (3D) distribution of the strain in the particular nanowire using a model based on finite element method. We observed the strain induced by the lattice mismatch between the GaN core and InGaN shell to be in the range from -0.1% to 0.15% for an In concentration of 30%. The maximum value of the strain component normal to the facets was concentrated at the transition region between the main part of the nanowire and the GaN tip. In addition, a variation in misfit strain relaxation between the axial growth and in-plane directions was revealed.

Physical review / A 95(2), 023843(2017). doi:10.1103/PhysRevA.95.023843, We present a comprehensive experimental analysis of statistical properties of the self-amplified spontaneous emission free-electron laser (FEL) FLASH by means of Hanbury Brown and Twiss interferometry. The experiments were performed at FEL wavelengths of 5.5, 13.4, and 20.8 nm. We determined the second-order intensity correlation function for all wavelengths and different operation conditions of FLASH. In all experiments a high degree of spatial coherence (above 50%) was obtained. Our analysis performed in spatial and spectral domains provided us with the independent measurements of an average pulse duration of the FEL that were below 60 fs. To explain the complicated behavior of the second-order intensity correlation function we developed an advanced theoretical model that includes the presence of multiple beams and external positional jitter of the FEL pulses. By this analysis we determined that in one of the experiments external positional jitter was about 25% of the beam size. We envision that methods developed in our study will be used widely for analysis and diagnostics of FEL radiation., Published by APS, Woodbury, NY

Ptychographic imaging with soft X-rays, especially in the water window energy range, suffers from limited detector dynamic range that directly influences the maximum spatial resolution achievable. High-dynamic-range data can be obtained by multiple exposures. By this approach we have increased the dynamic range of a ptychographic data set by a factor of 76 and obtained diffraction signal till the corners of the detector. The real space half period resolution was improved from 50 nm for the single exposure data to 18 nm for the high-dynamic-range data., Comment: 4 pages, 3 figures, Proceedings of XRM-2016 Conference, Oxford, UK

The core-shell nanowires have the promise to become the future building blocks of light emitting diodes, solar cells and quantum computers. The high surface to volume ratio allows efficient elastic strain relaxation, making it possible to combine a wider range of materials into the heterostructures as compared to the traditional, planar geometry. As a result, the strain fields appear in both the core and the shell of the nanowires, which can affect the device properties. The hard x-ray nanoprobe is a tool that enables a nondestructive mapping of the strain and tilt distributions where other techniques cannot be applied. By measuring the positions of the Bragg peaks for each point on the sample we can evaluate the values of local tilt and strain. In this paper we demonstrate the detailed strain mapping of the strained InGaN/GaN core-shell nanowire. We observe an asymmetric strain distribution in the GaN core caused by an uneven shell relaxation. Additionally, we analyzed the local micro-tilt distribution, which shows the edge effects at the top and bottom of the nanowire. The measurements were compared to the finite element modelling and show a good agreement.

X-ray Bragg ptychography (XBP) is an experimental technique for high-resolution strain mapping in a single nano- and mesoscopic crystalline structures. In this work we discuss the conditions that allow direct interpretation of the ptychographic reconstructions in terms of the strain distribution obtained from the two dimensional (2D) XBP. Simulations of the 2D XBP experiments under realistic experimental conditions are performed with a model of InGaN/GaN core-shell nanowire with low (1%) and high (30%) Indium concentrations in the shell.

Water window ptychographic coherent diffractive imaging was demonstrated at the P04 beamline of PETRA III synchrotron radiation source. The beam coherence was characterized with the non-redundant array method., A ptychographical coherent diffractive imaging experiment in the water window with focused soft X-rays at 500 eV is reported. An X-ray beam with high degree of coherence was selected for ptychography at the P04 beamline of PETRA III synchrotron radiation source. The beam coherence was measured with the newly developed non-redundant array method, and a coherence length of 4.1 µm and global degree of coherence of 35% at 100 µm exit slit opening in the vertical direction were determined. A pinhole, 2.6 µm in size, selected the coherent part of the beam that was used to obtain ptychographic reconstruction results of a lithographically manufactured test sample and a fossil diatom. The achieved resolution was 53 nm for the test sample and was only limited by the size of the detector. The diatom was imaged at a resolution better than 90 nm.

Journal of physics / Conference Series 499, 012020 (2014). doi:10.1088/1742-6596/499/1/012020, We present the ptychographical reconstruction of the x-ray beam formed by nanofocusing lenses (NFLs) containing a number of phase singularities (vortices) in the vicinity of the focal plane. As a test object Siemens star pattern was used with the finest features of 50 nm for ptychographical measurements. The extended ptychographical iterative engine (ePIE) algorithm was applied to retrieve both complex illumination and object functions from the set of diffraction patterns. The reconstruction revealed the focus size of 91.4±1.1 nm in horizontal and 70±0.3 nm in vertical direction at full width at half maximum (FWHM). The complex probe function was propagated along the optical axis of the beam revealing the evolution of the phase singularities., Published by IOP Publ., Bristol

We present a method to characterize the spatial coherence of soft X-ray radiation from a single diffraction pattern. The technique is based on scattering from non-redundant arrays (NRA) of slits and records the degree of spatial coherence at several relative separations from one to 15 microns, simultaneously. Using NRAs we measured the transverse coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III synchrotron storage ring as a function of different beam parameters. To verify the results obtained with the NRAs additional Young's double pinhole experiments were conducted and show good agreement., Comment: 15 pages, 6 figures, 2 tables, 42 references

Physical review / E 88(4), 044501 (2013). doi:10.1103/PhysRevE.88.044501, We present an x-ray study of liquid crystal membranes in the vicinity of the hexatic-smectic phase transitionby means of angular x-ray cross-correlation analysis. By applying two-point angular-intensity cross-correlation functions to the measured series of diffraction patterns the parameters of bond-orientational (BO) order in hexatic phase were directly determined. The temperature dependence of the positional correlation lengths was analyzed as well. The obtained correlation lengths show larger values for the higher-order Fourier components of BO order. These findings indicate a strong coupling between BO and positional order., Published by APS, College Park, Md.

Strained InGaN/GaN core-shell nanowires (NWs) are promising candidates for solid state lighting applications due to their superior properties compared to planar films. NW based devices consist of multiple functional layers, which sum up to many hundred nanometers in thickness, that can uniquely be accessed in a non-destructive fashion by hard X-rays. Here, we present a detailed nanoscale strain mapping performed on a single, 400 nm thick and 2 μm long core-shell InGaN/GaN nanowire with an x-ray beam focused down to 100 nm. We observe an inhomogeneous strain distribution caused by the asymmetric strain relaxation in the shell. One side of the InGaN shell was fully strained, whereas the other side and the top part were relaxed. Additionally, tilt and strain gradients were determined at the interface with the substrate.