Geometry and confinement effects at the nanoscale can result in substantial modifications to a material's properties with significant consequences in terms of chemical reactivity, biocompatibility and toxicity. Although benefiting applications across a diverse array of environmental and technological settings, the long-term effects of these changes, for example in the reaction of metallic nanoparticles under atmospheric conditions, are not well understood. Here, we use the unprecedented resolution attainable with aberration-corrected scanning transmission electron microscopy to study the oxidation of cuboid Fe nanoparticles. Performing strain analysis at the atomic level, we reveal that strain gradients induced in the confined oxide shell by the nanoparticle geometry enhance the transport of diffusing species, ultimately driving oxide domain formation and the shape evolution of the particle. We conjecture that such a strain-gradient-enhanced mass transport mechanism may prove essential for understanding the reaction of nanoparticles with gases in general, and for providing deeper insight into ionic conductivity in strained nanostructures.
Solar wind Magnetosphere Ionosphere Link Explorer, is a joint science mission between the European Space Agency and the Chinese Academy of Sciences. The spacecraft will be uniquely equipped to study the interaction between the Earth's magnetosphere-ionosphere system and the solar wind on a global scale. SMILE's instruments will explore this science through imaging of the solar wind charge exchange soft X-ray emission from the dayside magnetosheath, simultaneous imaging of the UV northern aurora and in-situ monitoring of the solar wind and magnetosheath plasma and magnetic field conditions.The Soft X-ray Imager (SXI) is the instrument being designed to observe X-ray photons emitted by the solar wind charge exchange process at photon energies between 200 eV and 2000 eV. X-rays will be collected using a focal plane array of two custom-designed CCDs, each consisting of 18 µm square pixels in a 4510 by 4510 array.SMILE will be placed in a highly elliptical polar orbit, passing in and out of the Earth's radiation belts every 48 hours. Radiation damage accumulated in the CCDs during the mission's nominal 3-year lifetime will degrade their performance (such as through decreases in charge transfer efficiency), negatively impacting the instrument's ability to detect low energy X-rays incident on the regions of the CCD image area furthest from the detector outputs. The design of the SMILE-SXI CCDs is presented here, including features and operating methods for mitigating the effects of radiation damage and expected end of life CCD performance. Measurements with a PLATO device 1Corresponding author.
The extremely surface sensitive technique of metastable de-excitation spectroscopy (MDS) has been utilized to probe the bonding and reactivity of crotyl alcohol over Pd(111) and provide insight into the selective oxidation pathway to crotonaldehyde. Auger de-excitation (AD) of metastable He (23S) atoms reveals distinct features associated with the molecular orbitals of the adsorbed alcohol, corresponding to emission from the hydrocarbon skeleton, the O n nonbonding, and CC π states. The O n and CC π states of the alcohol are reversed when compared to those of the aldehyde. Density functional theory (DFT) calculations of the alcohol show that an adsorption mode with both CC and O bonds aligned somewhat parallel to the surface is energetically favored at a substrate temperature below 200 K. Density of states calculations for such configurations are in excellent agreement with experimental MDS measurements. MDS revealed oxidative dehydrogenation of crotyl alcohol to crotonaldehyde between 200 and 250 K, resulting in small peak shifts to higher binding energy. Intramolecular changes lead to the opposite assignment of the first two MOs in the alcohol versus the aldehyde, in accordance with DFT and UPS studies of the free molecules. Subsequent crotonaldehyde decarbonylation and associated propylidyne formation above 260 K could also be identified by MDS and complementary theoretical calculations as the origin of deactivation and selectivity loss. Combining MDS and DFT in this way represents a novel approach to elucidating surface catalyzed reaction pathways associated with a “real-world” practical chemical transformation, namely the selective oxidation of alcohols to aldehydes.
Ho silicide nanostructures were formed by the deposition of submonolayer coverages of Ho onto a clean Si͑001͒ 2 ϫ 1 surface at various substrate temperatures. Depending on the deposition temperature and coverage, the substrate surrounding the nanostructures reconstructs into either a 2 ϫ 4 or 2ϫ 7 structure or a combination of the two. We use metastable de-excitation spectroscopy ͑He 2 3 S͒ to complement scanning tunneling microscopy ͑STM͒ to study these reconstructions revealing the electronic similarities between the 2 ϫ 4 and 2 ϫ 7 phases. The presence in the spectra of features due to hybridized Si 3s3p-Ho 6s5d bonds at the surface suggest that prominent maxima in the corresponding STM images are due to Ho atoms and that these reconstructions form as a precursor to nanowire formation.
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