The dynamic responses of a rhodium catalyst and a graphene sheet are investigated upon random excitation with 80 kV electrons. An extraordinary electron microscope stability and resolution allow studying temporary atom displacements from their equilibrium lattice sites into metastable sites across projected distances as short as 60 pm. In the rhodium catalyst, directed and reversible atom displacements emerge from excitations into metastable interstitial sites and surface states Our experiments suggest operating electron microscopes with beam currents as small as zeptoAmperes / nm 2 in a "weak-excitation" approach to improve on sample integrity and allow for time-resolved studies of conformational object changes that probe for functional behavior of catalytic surfaces or molecules.
The controlled incorporation of excess As into GaAs grown by molecular beam epitaxy at low growth temperatures (LT-GaAs) is explored. The substrate temperature and the As/Ga flux ratio were systematically varied to investigate the influence of growth parameters on the formation of native defects and structural properties. Near infrared absorption, magnetic circular dichroism of absorption, and slow positron annihilation were applied to determine point defect concentrations of As antisites (AsGa) and Ga vacancies (VGa). Structural properties of as-grown and annealed LT-GaAs layers were investigated by x-ray diffraction and transmission electron microscopy. In a well defined parameter range the lattice expansion of the LT-GaAs layers correlates with the amount of AsGa. The VGa acceptor concentration can quantitatively account for the ionization of the AsGa donors.
Transmission electron microscopy (TEM) has become an indispensable technique for studying heterogeneous catalysts. In particular, advancements of aberration-corrected electron optics and data acquisition schemes have made TEM capable of delivering images of catalysts with sub-Ångström resolution and single-atom sensitivity. Parallel developments of differentially pumped electron microscopes and of gas cells enable in situ observations of catalysts during the exposure to reactive gas environments at pressures of up to atmospheric levels and temperatures of up to several hundred centigrade. Here, we outline how to take advantage of the emerging state-of-the-art instrumentation and methodologies to study surface structures and dynamics to improve the understanding of structure-sensitive catalytic functionality. The concept of using low electron dose-rates in TEM in conjunction with in-line holography and aberration-correction at low voltage (80 kV) is introduced to allow maintaining atomic resolution and sensitivity during in situ observations of catalysts. Benefits are illustrated by exit wave reconstructions of TEM images of a nanocrystalline Co3O4 catalyst material acquired in situ during their exposure to either a reducing or oxidizing gas environment.
A combination of atomic resolution phase contrast electron microscopy and pulsed electron beams reveals pristine properties of MgCl 2 at 1.7 Å resolution that were previously masked by air and beam damage. Both the inter-and intra-layer bonding in pristine MgCl 2 are weak, which leads to uncommonly large local orientation variations that characterize this Ziegler-Natta catalyst support. By delivering electrons with 1-10 ps pulses and ≈160 ps delay times, phonons induced by the electron irradiation in the material are allowed to dissipate before the subsequent delivery of the next electron packet, thus mitigating phonon accumulations. As a result, the total electron dose can be extended by a factor of 80-100 to study genuine material properties at atomic resolution without causing object alterations, which is more effective than reducing the sample temperature. In conditions of minimal damage, beam currents approach femtoamperes with dose rates around 1 eÅ −2 s −1 . Generally, the utilization of pulsed electron beams is introduced herein to access genuine material properties while minimizing beam damage.
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