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1.
Nat Commun ; 12(1): 6517, 2021 Nov 11.
Artículo en Inglés | MEDLINE | ID: mdl-34764290

RESUMEN

Catalytic hydrogen oxidation on a polycrystalline rhodium foil used as a surface structure library is studied by scanning photoelectron microscopy (SPEM) in the 10-6 mbar pressure range, yielding spatially resolved X-ray photoemission spectroscopy (XPS) measurements. Here we report an observation of a previously unknown coexistence of four different states on adjacent differently oriented domains of the same Rh sample at the exactly same conditions. A catalytically active steady state, a catalytically inactive steady state and multifrequential oscillating states are simultaneously observed. Our results thus demonstrate the general possibility of multi-states in a catalytic reaction. This highly unusual behaviour is explained on the basis of peculiarities of the formation and depletion of subsurface oxygen on differently structured Rh surfaces. The experimental findings are supported by mean-field micro-kinetic modelling. The present observations raise the interdisciplinary question of how self-organising dynamic processes in a heterogeneous system are influenced by the permeability of the borders confining the adjacent regions.

2.
Ultramicroscopy ; 179: 15-23, 2017 08.
Artículo en Inglés | MEDLINE | ID: mdl-28364683

RESUMEN

We discuss the feasibility of detecting spin polarized electronic transitions with a vortex filter. This approach does not rely on the principal condition of the standard electron energy-loss magnetic chiral dichroism (EMCD) technique, the precise alignment of the crystal in order to use it as a beam splitter, and thus would pave the way for the application of EMCD to new classes of materials and problems, like amorphous magnetic alloys and interface magnetism. The dichroic signal strength at the L2, 3-edge of ferromagnetic Cobalt (Co) is estimated on theoretical grounds using a single atom scattering approach. To justify this approach, multi-slice simulations were carried out in order to confirm that orbital angular momentum (OAM) is conserved in amorphous materials over an extended range of sample thickness and also in very thin crystalline specimen, which is necessary for the detection of EMCD. Also artefact sources like spot size, mask tilt and astigmatism are discussed. In addition, the achievable SNR under typical experimental conditions is assessed.

3.
Sci Rep ; 6: 34003, 2016 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-27666531

RESUMEN

This work introduces an additive direct-write nanofabrication technique for producing extremely conductive gold nanostructures from a commercial metalorganic precursor. Gold content of 91 atomic % (at. %) was achieved by using water as an oxidative enhancer during direct-write deposition. A model was developed based on the deposition rate and the chemical composition, and it explains the surface processes that lead to the increases in gold purity and deposition yield. Co-injection of an oxidative enhancer enabled Focused Electron Beam Induced Deposition (FEBID)-a maskless, resistless deposition method for three dimensional (3D) nanostructures-to directly yield pure gold in a single process step, without post-deposition purification. Gold nanowires displayed resistivity down to 8.8 µΩ cm. This is the highest conductivity achieved so far from FEBID and it opens the possibility of applications in nanoelectronics, such as direct-write contacts to nanomaterials. The increased gold deposition yield and the ultralow carbon level will facilitate future applications such as the fabrication of 3D nanostructures in nanoplasmonics and biomolecule immobilization.

4.
Nat Commun ; 5: 4586, 2014 Aug 08.
Artículo en Inglés | MEDLINE | ID: mdl-25105563

RESUMEN

Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometre-sized electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions.

5.
Ultramicroscopy ; 115: 21-5, 2012 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-22459114

RESUMEN

The holographic mask technique is used to create freely moving electrons with quantized angular momentum. With electron optical elements they can be focused to vortices with diameters below the nanometer range. The understanding of these vortex beams is important for many applications. Here, we produce electron vortex beams and compare them to a theory of electrons with topological charge. The experimental results show excellent agreement with simulations. As an immediate application, fundamental experimental parameters like spherical aberration and partial coherence are determined.

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