Wilfried Sigle

The NdNiO₃ (NNO) system has attracted a considerable amount of attention owing to the discovery of superconductivity in Nd_0.8Sr_0.2NiO₂. In rare-earth nickelates, Ruddlesden–Popper (RP) faults play a significant role in functional properties, motivating our exploration of its microstructural characteristics and the electronic structure. Here, we employed aberration-corrected scanning transmission electron microscopy and spectroscopy to study a NdNiO₃ film grown by layer-by-layer molecular beam epitaxy (MBE). We found RP faults with multiple configurations in high-angle annular dark-field images. Elemental intermixing occurs at the SrTiO₃–NdNiO₃ interface and in the RP fault regions. Quantitative analysis of the variation in lattice constants indicates that large strains exist around the substrate–film interface. We demonstrate that the Ni valence change around RP faults is related to a strain and structure variation. This work provides insights into the microstructure and electronic-structure modifications around RP faults in nickelates.

Atomic design of a 2D‐material such as graphene can be substantially influenced by etching, deliberately induced in a transmission electron microscope. It is achieved primarily by overcoming the threshold energy for defect formation by controlling the kinetic energy and current density of the fast electrons. Recent studies have demonstrated that the presence of certain species of atoms can catalyze atomic bond dissociation processes under the electron beam by reducing their threshold energy. Most of the reported catalytic atom species are single atoms, which have strong interaction with single‐layer graphene (SLG). Yet, no such behavior has been reported for molecular species. This work shows by experimentally comparing the interaction of alkali and halide species separately and conjointly with SLG, that in the presence of electron irradiation, etching of SLG is drastically enhanced by the simultaneous presence of alkali and iodine atoms. Density functional theory and first principles molecular dynamics calculations reveal that due to charge‐transfer phenomena the CC bonds weaken close to the alkali‐iodide species, which increases the carbon displacement cross‐section. This study ascribes pronounced etching activity observed in SLG to the catalytic behavior of the alkali‐iodide species in the presence of electron irradiation.

In this work, the fabrication of zinc oxide (ZnO) nanowire networks is presented. By combining ion-track technology, electrochemical deposition, and atomic layer deposition, hierarchical and self-supporting three-dimensional (3D) networks of pure ZnO- and TiO₂-coated ZnO nanowires were synthesized. Analysis by means of high-resolution transmission electron microscopy revealed a highly crystalline structure of the electrodeposited ZnO wires and the anatase phase of the TiO₂ coating. In photoelectrochemical measurements, the ZnO and ZnO/TiO₂ nanowire networks, used as anodes, generated higher photocurrents compared to those produced by their film counterparts. The ZnO/TiO₂ nanowire network exhibited the highest photocurrents. However, the protection by the TiO₂ coatings against chemical corrosion still needs improvement. The one-dimensionality of the nanowires and the large electrolyte-accessible area make these 3D networks promising photoelectrodes, due to the improved transport properties of photogenerated charge carriers and faster redox reactions at the surface. Moreover, they can find further applications in e.g., sensing, catalytical, and piezoelectric devices.

Non-isolated nanoparticles show a plasmonic response that is governed by the localized surface plasmon resonance (LSPR) collective modes created by the nanoparticle aggregates. The individual and collective LSPR modes of silver nanoparticle aggregated by covalent binding by means of bifunctional molecular linkers are described in this study. Individual contributions to the collective modes are investigated at nanometer scale by means of energy-filtering transmission electron microscopy and compared to ultraviolet–visible spectroscopy. It is found that the aspect ratio and the shape of the clusters are the two main contributors to the low-energy collective modes.