The implementation of imaging techniques with low-energy electrons at synchrotron laboratories allowed for significant advancement in the field of spectromicroscopy. The spectroscopic photoemission and low energy electron microscope, SPELEEM, is a notable example. We summarize the multitechnique capabilities of the SPELEEM instrument, reporting on the instrumental aspects and the latest developments on the technical side. We briefly review applications, which are grouped into two main scientific fields. The first one covers different aspects of graphene physics. In particular, we highlight the recent work on graphene/Ir(100). Here, SPELEEM was employed to monitor the changes in the electronic structure that occur for different film morphologies and during the intercalation of Au. The Au monolayer, which creeps under graphene from the film edges, efficiently decouples the graphene from the substrate lowering the Dirac energy from 0.42 eV to 0.1 eV. The second field combines magnetism studies at the mesoscopic length scale with self-organized systems featuring ordered nanostructures. This example highlights the possibility to monitor growth processes in real time and combine chemical characterization with X-ray magnetic circular dichroism–photoemission electron microscopy (XMCD–PEEM) magnetic imaging by using the variable photon polarization and energy available at the synchrotron source.
Redox‐based memristive devices are one of the most attractive candidates for future nonvolatile memory applications and neuromorphic circuits, and their performance is determined by redox processes and the corresponding oxygen‐ion dynamics. In this regard, brownmillerite SrFeO2.5 has been recently introduced as a novel material platform due to its exceptional oxygen‐ion transport properties for resistive‐switching memory devices. However, the underlying redox processes that give rise to resistive switching remain poorly understood. By using X‐ray absorption spectromicroscopy, it is demonstrated that the reversible redox‐based topotactic phase transition between the insulating brownmillerite phase, SrFeO2.5, and the conductive perovskite phase, SrFeO3, gives rise to the resistive‐switching properties of SrFeOx memristive devices. Furthermore, it is found that the electric‐field‐induced phase transition spreads over a large area in (001) oriented SrFeO2.5 devices, where oxygen vacancy channels are ordered along the in‐plane direction of the device. In contrast, (111)‐grown SrFeO2.5 devices with out‐of‐plane oriented oxygen vacancy channels, reaching from the bottom to the top electrode, show a localized phase transition. These findings provide detailed insight into the resistive‐switching mechanism in SrFeOx‐based memristive devices within the framework of metal–insulator topotactic phase transitions.
The molecule–substrate interaction plays a key role in charge injection organic-based devices. Charge transfer at molecule–metal interfaces strongly affects the overall physical and magnetic properties of the system, and ultimately the device performance. Here, we report theoretical and experimental evidence of a pronounced charge transfer involving nickel tetraphenyl porphyrin molecules adsorbed on Cu(100). The exceptional charge transfer leads to filling of the higher unoccupied orbitals up to LUMO+3. As a consequence of this strong interaction with the substrate, the porphyrin’s macrocycle sits very close to the surface, forcing the phenyl ligands to bend upwards. Due to this adsorption configuration, scanning tunneling microscopy cannot reliably probe the states related to the macrocycle. We demonstrate that photoemission tomography can instead access the Ni-TPP macrocycle electronic states and determine the reordering and filling of the LUMOs upon adsorption, thereby confirming the remarkable charge transfer predicted by density functional theory calculations.