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Nanoscale thin films are widely implemented across a plethora of technological and scientific areas, and form the basis for many advancements that have driven human progress, owing to the high degree of functional tunability based on the chemical composition. Pulsed laser deposition is one of the multiple physical vapour deposition routes to fabricate thin films, employing laser energy to eject material from a target in the form of a plasma ...

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.

We report on the properties of laser-induced plasma plumes generated by ns pulsed excimer lasers as used for pulsed laser deposition to prepare thin oxide films. A focus is on the time and spatial evolution of chemical species in the plasma plume as well as the mechanisms related to the plume expansion. The overall dynamics of such a plume is governed by the species composition in particular if three or more elements are involved. We studied the temporal evolution of the plume, the composition of the chemical species in the plasma, as well as their electric charge. In particular, ionized species can have an important influence on film growth. Likewise, the different oxygen sources contributing to the overall oxygen content of an oxide film are presented and discussed. Important for the growth of oxide thin films is the compositional transfer of light element such as oxygen or Li. We will show and discuss how to monitor these light elements using plasma spectroscopy and plasma imaging and outline some consequences of our experimental results.