Christoph Schwanke

Implications of TCO Topography on Intermediate Reflector Design for a-Si/μc-Si Tandem Solar Cells—Experiments and Rigorous Optical Simulations

The influence of the transparent conducting oxide (TCO) topography was studied on the performance of a silicon oxide intermediate reflector layer (IRL) in a-Si/μc-Si tandem cells, both experimentally and by 3-D optical simulations. Therefore, cells with varying IRL thickness were deposited on three different types of TCOs. Clear differences were observed regarding the performance of the IRL as well as its ideal thickness, both experimentally and in the simulations. Optical modeling suggests that a small autocorrelation length is essential for a good performance. Design rules for both the TCO topography and the IRL thickness can be derived from this interplay.

Probing ion-specific effects on aqueous acetate solutions: Ion pairing versus water structure modifications

The effect of monovalent cations (Li+, K+, NH4+, Na+) on the water structure in aqueous chloride and acetate solutions was characterized by oxygen K-edge X-ray absorption spectroscopy (XAS), X-ray emission spectroscopy, and resonant inelastic X-ray scattering (RIXS) of a liquid microjet. We show ion- and counterion dependent effects on the emission spectra of the oxygen K-edge, which we attribute to modifications of the hydrogen bond network of water. For acetates, ion pairing with carboxylates was also probed selectively by XAS and RIXS. We correlate our experimental results to speciation data and to the salting-out properties of the cations.

Electrochemical flowcell for in-situ investigations by soft x-ray absorption and emission spectroscopy

A new liquid flow-cell designed for electronic structure investigations at the liquid-solid interface by soft X-ray absorption and emission spectroscopy is presented. A thin membrane serves simultaneously as a substrate for the working electrode and solid state samples as well as for separating the liquid from the surrounding vacuum conditions. In combination with counter and reference electrodes this approach allows in-situ studies of electrochemical deposition processes and catalytic reactions at the liquid-solid interface in combination with potentiostatic measurements. As model system in-situ monitoring of the deposition process of Co metal from a 10 mM CoCl2 aqueous solution by X-ray absorption and emission spectroscopy is presented.

Correlating Oxygen Evolution Catalysts Activity and Electronic Structure by a High-Throughput Investigation of Ni1-y-zFeyCrzOx

High-throughput characterization by soft X-ray absorption spectroscopy (XAS) and electrochemical characterization is used to establish a correlation between electronic structure and catalytic activity of oxygen evolution reaction (OER) catalysts. As a model system a quasi-ternary materials library of Ni1-y-zFeyCrzOx was synthesized by combinatorial reactive magnetron sputtering, characterized by XAS, and an automated scanning droplet cell. The presence of Cr was found to increase the OER activity in the investigated compositional range. The electronic structure of NiII and CrIII remains unchanged over the investigated composition spread. At the Fe L-edge a linear combination of two spectra was observed. These spectra were assigned to FeIII in Oh symmetry and FeIII in Td symmetry. The ratio of FeIII Oh to FeIII Td increases with the amount of Cr and a correlation between the presence of the FeIII Oh and a high OER activity is found.

A soft XAS transmission cell for operando studies.

A new cell for operando soft X-ray absorption spectroscopy in transmission mode is presented. Developed for investigations on solar water-splitting catalysts, the cell allows the study of solid films in direct contact with electrolyte solution while applying voltage and visible light. The design is optimized for fast sample exchange and the simultaneous measurement of fluorescence and transmission signal. The capability of the cell is presented on a manganese oxide (MnOx) film, where electronic structure changes are monitored during forward and backward potential changes. Detailed information about the varying contributions of several Mn oxidation states during this process was revealed.

Influence of the Outer Ligands on Metal-to-Ligand Charge Transfer in Solvated Manganese Porphyrins.

Two manganese porphyrin complexes, manganese tetraphenylporphyrin chloride (MnTPP-Cl) and manganese octaethylporphyrin chloride (MnOEP-Cl), exhibit distinctive spectral features of metal-to-ligand charge-transfer (MLCT) when dissolved in dichloromethane, characterized by resonant inelastic X-ray scattering at the Mn L-edge and N K-edge. The metal-ligand orbital mixing that mediates the MLCT is analyzed with the help of density functional theory/restricted open-shell configuration interaction singles calculations. On the basis of experimental and theoretical analyses, the distinctive MLCT is argued to originate from alteration of the porphyrin outer ligands: phenyl groups in MnTPP-Cl and ethyl groups in MnOEP-Cl.

3D optical modeling of thin-film a-Si/μc-Si tandem solar cells with random textured interfaces using FEM

We present a FEM based simulator for 3D rigorous optical modeling of a-Si/μc-Si tandem thin-film solar cells with randomly textured layer interfaces. Our focus lies on a detailed analysis of the numerical error.

Multiscale Photo-Based In-Situ and Operando Spectroscopies in Time and Energy Landscapes

Following catalytic reactions, in-situ and operando are now the focus of a number of dedicated experiments at light sources which have been developed to track the electronic and molecular structural dynamics of catalysts. The challenges for this goal are two-fold: first, the development of spectroscopic tools in the energy domain and time domain is required. The photocatalytic processes have early dynamics of tens of femtoseconds, while further reaction takes seconds, minutes, and even hours. Second, a combination of tools to probe processes not only in solids, but also in solutions and at interfaces, is now needed. In this special issue, we present recent developments at the synchrotron facility BESSY II using photon energy from the infrared and extreme ultraviolet up to the soft X-ray regime for in-situ and operando applications addressing these two major challenges. As this work is a result of contributions from several groups, each section will present the groups activities and related team members involved.