Data Science

Using operando time-resolved X-ray absorption spectroscopy, we investigated the origin of volcano-shaped ethanol oxidative dehydrogenation activity trend of VOx/CeO2 catalysts as a function of VOx surface coverage. Vanadium and cerium synergistically change their oxidation states during the catalytic cycle. The catalytic activity correlates with the concentration of reversible Ce4+/3+species.

The ability to study in situ the formation and consumption of Pd hydrides (PdH) in liquid environments is a significant challenge hampering a deeper understanding of catalyzed liquid-phase hydrogenation reactions. Here, using quick scanning X-ray absorption spectroscopy (QEXAFS), we present a detailed kinetic study of Pd hydride formation and reactivity on Pd/Al₂O₃ in 2-propanol solvent. 

Oxynitrides are promising materials for visible light-driven water splitting. However, limited information regarding their electron-momentum resolved electronic structure exists. Here, with the advantage of the enhanced probing depth and chemical state specificity of soft-X-ray ARPES, we determine the electronic structure of the photocatalyst oxynitride LaTiO₂N and monitor its evolution as a consequence of the oxygen evolution reaction. After the photoelectrochemical reactions, we observe a partial loss of Ti- and La-N 2p states, distortions surrounding the local environment of titanium atoms and, unexpectedly, an indication of an electron accumulation layer at or near the surface, which may be connected with either a large density of metallic surface states or downward band bending. The distortions and defects associated with the titanium 3d states lead to the trapping of electrons and charge recombination, which is a major limitation for the oxynitride LaTiO₂N. The presence of an accumulation layer and its evolution suggests complex mechanisms of the photoelectrochemical reaction, especially in cases where co-catalysts or passivation layers are used.

“Soft” x-rays are notoriously hard to detect. Particularly, in the context of high-performance synchrotron and free electron laser (FEL) experiments, suitable detector options for low-energy x-rays are highly sought after. Currently available options only provide limited area, readout speed, and dynamic range. Now, a team of scientists from the Laboratory for X-Ray Nanoscience and Technologies (LXN) at PSI are challenging these limitations. They combined a detector made at PSI with newly developed silicon sensors to push the resolution toward the soft x-ray limit. A first version of this detector system is now in operation at the SwissFEL endstation Maloja. And it points to further possibilities to refine the detector technology to eventually catch the elusive soft x-rays.

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal.

Operando/in situ spectro-electrochemical studies often require high loadings and thick catalyst layers (CLs) leading to large ion- and mass-transport limitations. In this study we investigate PdH-formation in two Pd-catalysts with similar surface areas but drastically different morphologies. Our results unveil that the CL-thickness largely determines the PdH formation trends calling for the minimization of the CL-thickness in such experiments.

For contributions to the development of detectors for XFELs and specifically for their verification, characterization, and calibration

We report on the commissioning results of the cold neutron multiplexing secondary spectrometer CAMEA (Continuous Angle Multi-Energy Analysis) at the Swiss Spallation Neutron Source at the Paul Scherrer Institut, Switzerland. CAMEA is optimized for ...

Zeolites are a class of shapely, colourful minerals with very special properties, making them omnipresent in our surroundings. They accelerate chemical reactions, absorb hazardous contaminants and water to a high degree, for example. Their only limitation is that they usually lose their peculiar crystalline structure at high temperatures. Now researchers at the University of Bern have found an unexpected exception.

3d transition metals often exhibit a quenched orbital moment when in a solid state system. Therefore, the proposition of a large unquenched orbital moment for V in VI₃ caused some surprise and discussion in the scientific community. Experimental and theoretical works diverge on the fact of whether the orbital moment is quenched or not. In our work we have been able to give an answer this open issue, proposing also a model for the ground state of VI₃.