In situ observation of synthesized nanoparticles in ultra-dilute aerosols via X-ray scattering

In-air epitaxy of nanostructures (Aerotaxy) has recently emerged as a viable route for fast, large-scale production. In this study, we use small-angle X-ray scattering to perform direct in-flight characterizations of the first step of this process, i.e., the engineered formation of Au and Pt aerosol nanoparticles by spark generation in a flow of N₂ gas. This represents a particular challenge for characterization because the particle density can be extremely low in controlled production. The particles produced are examined during production at operational pressures close to atmospheric conditions and exhibit a lognormal size distribution ranging from 5–100 nm. The Au and Pt particle production and detection are compared. We observe and characterize the nanoparticles at different stages of synthesis and extract the corresponding dominant physical properties, including the average particle diameter and sphericity, as influenced by particle sintering and the presence of aggregates. We observe highly sorted and sintered spherical Au nanoparticles at ultra-dilute concentrations (< 5 × 10⁵ particles/cm³) corresponding to a volume fraction below 3 × 10^–10, which is orders of magnitude below that of previously measured aerosols. We independently confirm an average particle radius of 25 nm via Guinier and Kratky plot analysis. Our study indicates that with high-intensity synchrotron beams and careful consideration of background removal, size and shape information can be obtained for extremely low particle concentrations with industrially relevant narrow size distributions.

     

Small-angle X-ray scattering from phase-separating amorphous metallic alloys undergoing nanocrystallization

We performed a combined small- and wide-angle X-ray scattering (SAXS/WAXS) study of nanocrystallization during annealing of binary Al₉₂Sm₈ and Al₉₁Gd₉ melt-spun glassy alloys. In course of the transformation an interference maximum develops in the SAXS region while WAXS spectra show formation of fcc-Al nanocrystals in the glassy phase. In order to determine the origin of the SAXS maximum the theoretical SAXS intensity and distance distribution function were calculated considering two structural models. The first model represented a single nanocrystal with a solute layer on its surface and the second one a phase-separated alloy with spatially correlated compositional fluctuations. The results of the calculations are compared with the experimental data. It is demonstrated that only the model representing correlated fluctuations reasonably reproduces the experimental results. We conclude that nano-scale glassy phase separation occurs in the investigated alloys and the nanocrystals form inside the Al-rich amorphous regions.     

Observation of empty liquids and equilibrium gels in a colloidal clay

The relevance of anisotropic interactions in colloidal systems has recently emerged in the context of the rational design of new soft materials. Patchy colloids of different shapes, patterns and functionalities are considered the new building blocks of a bottom-up approach toward the realization of self-assembled bulk materials with predefined properties. The ability to tune the interaction anisotropy will make it possible to recreate molecular structures at the nano- and micro-scales (a case with tremendous technological applications), as well as to generate new unconventional phases, both ordered and disordered. Recent theoretical studies suggest that the phase diagram of patchy colloids can be significantly altered by limiting the particle coordination number (that is, valence). New concepts such as empty liquids—liquid states with vanishing density—and equilibrium gels—arrested networks of bonded particles, which do not require an underlying phase separation to form—have been formulated. Yet no experimental evidence of these predictions has been provided. Here we report the first observation of empty liquids and equilibrium gels in a complex colloidal clay, and support the experimental findings with numerical simulations.     

Erratum to: In situ observation of synthesized nanoparticles in ultra-dilute aerosols via X-ray scattering

Nano Research - The article In situ observation of synthesized nanoparticles in ultradilute aerosols via X-ray scattering, written by Sarah R. McKibbin, Sofie Yngman, Olivier Balmes, Bengt O....