arXiv subjects

Christoph Somsen

Publications and source records attributed to Christoph Somsen.

5 recordsLinked to original sources

arXiv2026

Epitaxial Films as Model Platform for Understanding Compositionally Complex Electrocatalysts

Compositionally complex solid solutions provide a unique route for engineering high-performance electrocatalysts, where the polyelemental surface composition can be seamlessly tuned to optimize activity, selectivity, and stability. However, the mechanistic understanding of these electrocatalysts remains limited by the lack of a model system with a crystallographically-defined surface that is compatible with correlative, multi-scale characterization. Here, we present epitaxial films as a model platform for studying compositionally complex electrocatalysts. Using magnetron sputtering, we realize (111) epitaxial Ir-Pd-Pt-Rh-Ru films on (0001) sapphire substrate via a (111) Pt buffer layer, confirmed by X-ray diffraction and transmission electron microscopy. The growth approach is applicable across a broad composition range and produces smooth surfaces (root mean square roughness < 1 nm) with micrometer-sized grains in the nanoscale films. With these films, we demonstrate direct structure-activity mapping at the nanoscale through precise co-localization using micro-indents and performing correlative atomic force microscopy, electron backscatter diffraction, and scanning electrochemical cell microscopy. Our work establishes a model platform for fundamental scalebridging characterization and paves the way for rational design of compositionally complex electrocatalysts.

cond-mat.mtrl-sci↗

arXiv2026

Influence of Ru content on electrocatalytic activity and defect formation of Au-Pd-Pt-Ru compositionally complex solid solution thin films

Compositionally complex solid solutions (CCSSs) consist of a randomly mixed single phase with the potential to enhance electrocatalytic activity through their polyelemental surface atom arrangements. However, microstructural complexity originating from multiple principal elements influences local structure, chemistry, and lattice strain, which might also affect electrocatalytic activity. Here, we investigate the effect of Ru content on electrochemistry and defect formation in Au-Pd-Pt-Ru CCSS thin films. Such defects could provide active sites when terminating at the CCSS surface or modify surface composition through preferential segregation. A thin-film material library covering a wide composition range was fabricated by room-temperature combinatorial co-sputtering. High-throughput compositional, structural and functional characterization, including electron microscopy equipped with energy dispersive X-ray spectroscopy, X-ray diffraction, and electrochemical screening, were used to correlate composition and microstructural features with catalytic activity. Three representative compositions selected from the library - Au68Pd13Pt15Ru4, Au27Pd24Pt23Ru26, and Au9Pd21Pt18Ru52 - were examined in detail. The three samples exhibit face-centered cubic structures, with lattice contraction occurring with increasing Ru content. In addition, with increasing Ru content, a transition from a high density of nanotwins to high-density, atomic-layer stacking faults was observed. Moreover, the hydrogen evolution reaction activity improves with higher Ru content. Atom probe tomography reveals local compositional fluctuations, including element-specific enrichment and depletion at grain boundaries. The findings provide a new insight into surface atom arrangement design in the CCSS electrocatalysts with enhanced performance.

cond-mat.mtrl-sci↗

arXiv2019

Discovery of $ω$-free high-temperature Ti-Ta-X shape memory alloys from first principles calculations

The rapid degradation of the functional properties of many Ti-based alloys is due to the precipitation of the $ω$ phase. In the conventional high-temperature shape memory alloy Ti-Ta the formation of this phase compromises completely the shape memory effect and high (>100°C) transformation temperatures cannot be mantained during cycling. A solution to this problem is the addition of other elements to form Ti-Ta-X alloys, which often modifies the transformation temperatures; due to the largely unexplored space of possible compositions, very few elements are known to stabilize the shape memory effect without decreasing the transformation temperatures below 100°C. In this study we use transparent descriptors derived from first principles calculations to search for new ternary Ti-Ta-X alloys that combine stability and high temperatures. We suggest four new alloys with these properties, namely Ti-Ta-Sb, Ti-Ta-Bi, Ti-Ta-In, and Ti-Ta-Sc. Our predictions for the most promising of these alloys, Ti-Ta-Sc, are subsequently fully validated by experimental investigations, the new alloy Ti-Ta-Sc showing no traces of $ω$ phase after cycling. Our computational strategy is immediately transferable to other materials and may contribute to suppress $ω$ phase formation in a large class of alloys.

cond-mat.mtrl-sci↗

arXiv2008

High temperature ferromagnetism in Co-implanted TiO2 rutile

We report on structural, magnetic and electronic properties of Co-implanted TiO2 rutile single crystals for different implantation doses. Strong ferromagnetism at room temperature and above is observed in TiO2 rutile plates after cobalt ion implantation, with magnetic parameters depending on the cobalt implantation dose. While the structural data indicate the presence of metallic cobalt clusters, the multiplet structure of the Co L3 edge in the XAS spectra gives clear evidence for a substitutional Co 2+ state. The detailed analysis of the structural and magnetic properties indicates that there are two magnetic phases in Co-implanted TiO2 plates. One is a ferromagnetic phase due to the formation of long range ferromagnetic ordering between implanted magnetic cobalt ions in the rutile phase, and the second one is a superparamagnetic phase originates from the formation of metallic cobalt clusters in the implanted region. Using x-ray resonant magnetic scattering, the element specific magnetization of cobalt, oxygen and titanium in Co-implanted TiO2 single crystals are investigated. Magnetic dichroism was observed at the Co L edges as well as at the O K edge. The interaction mechanism, which leads to ferromagnetic ordering of substituted cobalt ions in the host matrix, is also discussed.

cond-mat.mtrl-sci↗

arXiv2008

Intrinsic room temperature ferromagnetism in Co-implanted ZnO

We report on the structural and magnetic properties of a cobalt-implanted ZnO film grown on a sapphire substrate. X-ray diffraction and transmission electron microscopy reveal the presence of a (10-10)-oriented hexagonal Co phase in the Al2O3 sapphire substrate, but not in the ZnO film. Co clusters, with a diameter of is about 5-6 nm, form a Co rich layer in the substrate close to the ZnO/Al2O3 interface. Magnetization measurements indicate that there exist two different magnetic phases in the implanted region. One originates from the Co clusters in Al2O3, the other one belongs to a homogeneous ferromagnetic phase with a ferromagnetic Curie temperature far above room temperature and can be attributed to Co substitution on Zn sites in the ZnO layer. We have observed magnetic dichroism at the Co L2,3 and O K edges at room temperature as well as the multiplet structure in x-ray absorption spectra around the Co L3 edge, supporting the intrinsic nature of the observed ferromagnetism in Co-implanted ZnO film. The magnetic moment per substituted cobalt is found about 2.81 Bohr magneton which is very close to the theoretical expected value of 3 Bohr magneton per Co atom for Co 2+ in its high spin state.

cond-mat.mtrl-sci↗