48 research outputs found
Real Space Imaging of Nanoparticle Assembly at Liquid-Liquid Interfaces with Nanoscale Resolution.
Bottom up self-assembly of functional materials at liquid-liquid interfaces has recently emerged as method to design and produce novel two-dimensional (2D) nanostructured membranes and devices with tailored properties. Liquid-liquid interfaces can be seen as a "factory floor" for nanoparticle (NP) self-assembly, because NPs are driven there by a reduction of interfacial energy. Such 2D assembly can be characterized by reciprocal space techniques, namely X-ray and neutron scattering or reflectivity. These techniques have drawbacks, however, as the structural information is averaged over the finite size of the radiation beam and nonperiodic isolated assemblies in 3D or defects may not be easily detected. Real-space in situ imaging methods are more appropriate in this context, but they often suffer from limited resolution and underperform or fail when applied to challenging liquid-liquid interfaces. Here, we study the surfactant-induced assembly of SiO2 nanoparticle monolayers at a water-oil interface using in situ atomic force microscopy (AFM) achieving nanoscale resolved imaging capabilities. Hitherto, AFM imaging has been restricted to solid-liquid interfaces because applications to liquid interfaces have been hindered by their softness and intrinsic dynamics, requiring accurate sample preparation methods and nonconventional AFM operational schemes. Comparing both AFM and grazing incidence X-ray small angle scattering data, we unambiguously demonstrate correlation between real and reciprocal space structure determination showing that the average interfacial NP density is found to vary with surfactant concentration. Additionally, the interaction between the tip and the interface can be exploited to locally determine the acting interfacial interactions. This work opens up the way to studying complex nanostructure formation and phase behavior in a range of liquid-liquid and complex liquid interfaces
Expérience de lévitation électromagnétique sous rayonnement synchrotron
La lévitation électromagnétique est utilisée
lors de l’élaboration, à haut degré de pureté, et de la mesure de propriétés
thermophysiques d’alliages métalliques. La validation des modèles numériques existants
est entravée par l'absence de données expérimentales relatives aux vitesses d'écoulement
à l'intérieur de l’alliage fondu. À l'aide d'une technique d'imagerie rayons X
(ESRF-faisceau ID15A), nous voulons mesurer les vitesses dans une goutte de métal en
lévitation
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Atomic-Scale Surface Demixing in a Eutectic Liquid BiSn Alloy
Resonant x-ray reflectivity of the surface of the liquid phase of the Bi43Sn57 eutectic alloy reveals atomic-scale demixing extending over three near-surface atomic layers. Because of the absence of an underlying atomic lattice which typically defines adsorption in crystalline alloys, studies of adsorption in liquid alloys provide unique insight on interatomic interactions at the surface. The observed composition modulation could be accounted for quantitatively by the Defay-Prigogine and Strohl-King multilayer extensions of the single-layer Gibbs model, revealing a near-surface domination of the attractive Bi-Sn interaction over the entropy.Engineering and Applied Science
Solvent Mediated Assembly of Nanoparticles Confined in Mesoporous Alumina
The controlled self-assembly of thiol stabilized gold nanocrystals in a
mediating solvent and confined within mesoporous alumina was probed in situ
with small angle x-ray scattering. The evolution of the self-assembly process
was controlled reversibly via regulated changes in the amount of solvent
condensed from an undersaturated vapor. Analysis indicated that the
nanoparticles self-assembled into cylindrical monolayers within the porous
template. Nanoparticle nearest-neighbor separation within the monolayer
increased and the ordering decreased with the controlled addition of solvent.
The process was reversible with the removal of solvent. Isotropic clusters of
nanoparticles were also observed to form temporarily during desorption of the
liquid solvent and disappeared upon complete removal of liquid. Measurements of
the absorption and desorption of the solvent showed strong hysteresis upon
thermal cycling. In addition, the capillary filling transition for the solvent
in the nanoparticle-doped pores was shifted to larger chemical potential,
relative to the liquid/vapor coexistence, by a factor of 4 as compared to the
expected value for the same system without nanoparticles.Comment: 9 pages, 9 figures, appeared in Phys. Rev.
Nanoscale Structure of the Oil-Water Interface
X-ray reflectivity (XR) and atomistic molecular dynamics (MD) simulations,
carried out to determine the structure of the oil-water interface, provide new
insight into the simplest liquid-liquid interface. For several oils (hexane,
dodecane, and hexadecane) the XR shows very good agreement with a monotonic
interface-normal electron density profile (EDP) broadened only by capillary
waves. Similar agreement is also found for an EDP including a sub-Ă… thick
electron depletion layer separating the oil and the water. The XR and MD
derived depletions are much smaller than reported for the interface between
solid-supported hydrophobic monolayers and water
Molecular scale structure and dynamics at an ionic liquid/electrode interface
The structural arrangement and dynamics of ions near the IL/electrode interface during charging and discharging was studied by a combination of time resolved X-ray reflectivity and impedance spectroscopy.</p
Atomic-scale surface demixing in a eutectic liquid BiSn alloy
Resonant x-ray reflectivity of the surface of the liquid phase of the
BiSn eutectic alloy reveals atomic-scale demixing extending over
three near-surface atomic layers. Due to the absence of underlying atomic
lattice which typically defines adsorption in crystalline alloys, studies of
adsorption in liquid alloys provide unique insight on interatomic interactions
at the surface. The observed composition modulation could be accounted for
quantitatively by the Defay-Prigogine and Strohl-King multilayer extensions of
the single-layer Gibbs model, revealing a near-surface domination of the
attractive Bi-Sn interaction over the entropy.Comment: 4 pages (two-column), 3 figures, 1 table; Added a figure, updated
references, discussion; accepted at Phys. Rev. Let