Bragg coherent diffraction imaging is a powerful strain imaging tool, often limited by beam-induced sample instability for small particles and high power densities. Here, we devise and validate an adapted diffraction volume assembly algorithm, capable of recovering three-dimensional datasets from particles undergoing uncontrolled and unknown rotations. We apply the method to gold nanoparticles which rotate under the influence of a focused coherent x-ray beam, retrieving their three-dimensional shapes and strain fields. The results show that the sample instability problem can be overcome, enabling the use of fourth generation synchrotron sources for Bragg coherent diffraction imaging to their full potential.
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.
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 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 transparent conductive oxides and other polycrystalline materials at the nanoscale.
The optical analysis of multilayer structures formed from the topmost layer of InGaAs/GaAs quantum rings (QRs) grown on a vertically stacked and laterally aligned InGaAs/GaAs quantum dot (QD) superlattice has been performed to elucidate the nature of the contribution from each layer. These hybrid structures representing a coupled QR chain layer and the layers of self-assembled QD chains display strong optical anisotropy. Unusually strong oscillations are observed in the circularly polarized photoluminescence (PL) intensities under magnetic field for emissions in the spectral range of the QD structure and these oscillations occur simultaneously with weaker oscillations related to the Aharonov-Bohm interference that modulates the emissions from the QR top layer of the structure. The behavior seen in the magneto-PL spectrum is interpreted in terms of joint effects associated to strain, spatial, and magnetic field confinements on the valence band states forming the magnetoexciton ground state of this multilayered structure. The result can be ascribed to a magnetically induced dark exciton contribution where the heavy-hole (type II) state becomes localized outside, whereas light-hole (type I) as well as electron states remain inside the spatial confinement area of the QD.