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The self‐assembly of anisotropic nanocrystals (stabilized by organic capping molecules) with pre‐selected composition, size, and shape allows for the creation of nanostructured materials with unique structures and features. For such a material, the shape and packing of the individual nanoparticles play an important role. This work presents a synthesis procedure for ω‐thiol‐terminated polystyrene (PS‐SH) functionalized gold nanooctahedra of variable size (edge length 37, 46, 58, and 72 nm). The impact of polymer chain length (Mw: 11k, 22k, 43k, and 66k g⋅mol−1) on the growth of colloidal crystals (e. g. mesocrystals) and their resulting crystal structure is investigated. Small‐angle X‐ray scattering (SAXS) and scanning transmission electron microscopy (STEM) methods provide a detailed structural examination of the self‐assembled faceted mesocrystals based on octahedral gold nanoparticles of different size and surface functionalization. Three‐dimensional angular X‐ray cross‐correlation analysis (AXCCA) enables high‐precision determination of the superlattice structure and relative orientation of nanoparticles in mesocrystals. This approach allows us to perform non‐destructive characterization of mesocrystalline materials and reveals their structure with resolution down to the nanometer scale. [ABSTRACT FROM AUTHOR]

The study of virus structures by X-ray free-electron lasers (XFELs) has attracted increased attention in recent decades. Such experiments are based on the collection of 2D diffraction patterns measured at the detector following the application of femtosecond X-ray pulses to biological samples. To prepare an experiment at the European XFEL, the diffraction data for the tick-borne encephalitis virus (TBEV) was simulated with different parameters and the optimal values were identified. Following the necessary steps of a well established data-processing pipeline, the structure of TBEV was obtained. In the structure determination presented, a priori knowledge of the simulated virus orientations was used. The efficiency of the proposed pipeline was demonstrated. [ABSTRACT FROM AUTHOR]

Single particle imaging (SPI) at X‐ray free‐electron lasers is particularly well suited to determining the 3D structure of particles at room temperature. For a successful reconstruction, diffraction patterns originating from a single hit must be isolated from a large number of acquired patterns. It is proposed that this task could be formulated as an image‐classification problem and solved using convolutional neural network (CNN) architectures. Two CNN configurations are developed: one that maximizes the F1 score and one that emphasizes high recall. The CNNs are also combined with expectation‐maximization (EM) selection as well as size filtering. It is observed that the CNN selections have lower contrast in power spectral density functions relative to the EM selection used in previous work. However, the reconstruction of the CNN‐based selections gives similar results. Introducing CNNs into SPI experiments allows the reconstruction pipeline to be streamlined, enables researchers to classify patterns on the fly, and, as a consequence, enables them to tightly control the duration of their experiments. Incorporating non‐standard artificial‐intelligence‐based solutions into an existing SPI analysis workflow may be beneficial for the future development of SPI experiments. [ABSTRACT FROM AUTHOR]

We show that the decomposition of caesium lead halide perovskite nanocrystals under continuous X-ray illumination depends on the surface ligand. For oleic acid/oleylamine, we observe a fast decay accompanied by the formation of elemental lead and halogen. Upon surface functionalization with a metal porphyrin derivative, the decay is markedly slower and involves the disproportionation of lead to Pb0 and Pb3+. In both cases, the decomposition is preceded by a contraction of the atomic lattice, which appears to initiate the decay. We find that the metal porphyrin derivative induces a strong surface dipole on the nanocrystals, which we hold responsible for the altered and slower decomposition pathway. These results are important for application of lead halide perovskite nanocrystals in X-ray scintillators. [ABSTRACT FROM AUTHOR]

We correlate spatially resolved fluorescence (-lifetime) measurements with X-ray nanodiffraction to reveal surface defects in supercrystals of self-assembled cesium lead halide perovskite nanocrystals and study their effect on the fluorescence properties. Upon comparison with density functional modeling, we show that a loss in structural coherence, an increasing atomic misalignment between adjacent nanocrystals, and growing compressive strain near the surface of the supercrystal are responsible for the observed fluorescence blueshift and decreased fluorescence lifetimes. Such surface defect-related optical properties extend the frequently assumed analogy between atoms and nanocrystals as so-called quasi-atoms. Our results emphasize the importance of minimizing strain during the self-assembly of perovskite nanocrystals into supercrystals for lighting application such as superfluorescent emitters. By utilizing spatially resolved fluorescence (-lifetime) measurements and high precision X-ray nanodiffraction, the authors correlate the influence of structural misalignment and fluorescence (-lifetime) properties of all-inorganic CsPbX3 (X– = Br–, Cl–) perovskite superlattices. [ABSTRACT FROM AUTHOR]

Second-order intensity interferometry was employed to study the spatial and temporal properties of the European X-ray Free-Electron Laser (EuXFEL). Measurements were performed at the soft x-ray Self-Amplified Spontaneous Emission (SASE3) undulator beamline at a photon energy of 1.2 keV in the Self-Amplified Spontaneous Emission (SASE) mode. Two high-power regimes of the SASE3 undulator settings, i.e., linear and quadratic undulator tapering at saturation, were studied in detail and compared with the linear gain regime. The statistical analysis showed an exceptionally high degree of spatial coherence up to 90% for the linear undulator tapering. Analysis of the measured data in spectral and spatial domains provided an average pulse duration of about 10 fs in our measurements. The obtained results will be valuable for the experiments requiring and exploiting short pulse duration and utilizing high coherence properties of the EuXFEL. [ABSTRACT FROM AUTHOR]