An improved analysis for single-particle imaging (SPI) experiments, using the limited data, is presented here. Results are based on a study of bacteriophage PR772 performed at the Atomic, Molecular and Optical Science instrument at the Linac Coherent Light Source as part of the SPI initiative. Existing methods were modified to cope with the shortcomings of the experimental data: inaccessibility of information from half of the detector and a small fraction of single hits. The general SPI analysis workflow was upgraded with the expectation-maximization based classification of diffraction patterns and mode decomposition on the final virus-structure determination step. The presented processing pipeline allowed us to determine the 3D structure of bacteriophage PR772 without symmetry constraints with a spatial resolution of 6.9 nm. The obtained resolution was limited by the scattering intensity during the experiment and the relatively small number of single hits.
The assembly of colloidal semiconductive nanocrystals into highly ordered superlattices predicts novel structure‐related properties by design. However, those structure–property relationships, such as charge transport depending on the structure or even directions of the superlattice, have remained unrevealed so far. Here, electric transport measurements and X‐ray nanodiffraction are performed on self‐assembled lead sulfide nanocrystal superlattices to investigate direction‐dependent charge carrier transport in microscopic domains of these materials. By angular X‐ray cross‐correlation analysis, the structure and orientation of individual superlattices is determined, which are directly correlated with the electronic properties of the same microdomains. By that, strong evidence for the effect of superlattice crystallinity on the electric conductivity is found. Further, anisotropic charge transport in highly ordered monocrystalline domains is revealed, which is attributed to the dominant effect of shortest interparticle distance. This implies that transport anisotropy should be a general feature of weakly coupled nanocrystal superlattices.
Nanoparticle assemblies
with long-range packing order and preferred
crystallographic orientation of building blocks, i.e., mesocrystals, are of high interest not only because of their unique physical
properties but also due to their complex structure and morphogenesis.
In this study, faceted mesocrystals have been assembled from the dispersion
of truncated cubic-shaped iron oxide nanoparticles stabilized by oleic
acid (OA) molecules using the nonsolvent “gas phase diffusion
technique” into an organic solvent. The effects of synthesis
conditions as well as of the nanoparticle size and shape on the structure
and morphogenesis of mesocrystals were examined. The interactions
of OA-capped iron oxide nanoparticles with solvent molecules were
probed by analytical ultracentrifugation and double difference pair
distribution function analysis. It was shown that the structure of
the organic shell significantly depends on the nature and polarity
of solvent molecules. For the nonpolar solvents, the interaction of
the aliphatic chains of OA molecules with the solvent molecules is
favorable and the chains extend into the solvent. The solvation shell
around the nanoparticles is more extended in nonpolar and more compact
in polar solvents. There is a clear trend for more spherical particles
to be assembled into the fcc superlattice, whereas
less truncated cubes form rhombohedral and tetragonal structures.
The observed changes in packing symmetry are reminiscent of structural
polymorphism known for “classical” (atomic and molecular)
crystals.
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.
Depending on the volume fraction and interparticle interactions, colloidal suspensions can form different phases, ranging from fluids, crystals, and glasses to gels. For soft microgels that are made from thermoresponsive...
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