arXiv subjects

Hans-Georg Steinrück

Publications and source records attributed to Hans-Georg Steinrück.

8 recordsLinked to original sources

arXiv2026

Identifying intercalation electrodes for electrochemical ion recovery and desalination

Water sources serve as a requirement for human consumption, industrial, and agricultural needs and a resource for valuable ions. Appropriate treatment of water that captures ions from the aqueous solution can give rise to suitable `products', such as critical ions (such as Li$^+$) in selective ion recovery and usable water in the case of desalination (i.e., removal of non-essential ions). Among myriad ion capture techniques, we focus on electrochemical methods using intercalation electrodes, an energy-efficient approach capable of both selectively extracting specific ions or non-selectively extracting multiple ions from diverse water sources. However, practical realization of electrochemical ion capture requires the use of robust cation intercalation electrodes, with the state-of-the-art olivine-FePO$_4$ and spinel-Mn$_2$O$_4$ exhibiting several shortcomings. Thus, we develop a high-throughput computational workflow to identify potential intercalation electrodes for both ion recovery and desalination from a pool of 20,414 Li, Mg, Ca, Na, and/or K-containing structures from the Materials Project database. Based on the construction of Pourbaix diagrams relevant for electrodes operating under seawater conditions, modifying criteria used for defining metastability in seawater, computing average intercalation voltages and the extent of metastability of electrode structures, and computational graphs to encode ionic selectivity, we identify a total of 11 promising electrodes for selective ion recovery and one possible desalination electrode. The promising materials identified in this work include Fe$_2$(MoO$_4$)$_3$, Li$_3$Fe$_2$(PO$_4$)$_3$, LiFeP$_2$O$_7$ for selective Li-recovery. Our study provides thermodynamic insights, qualitative trends, and a promising list of intercalation electrodes for experimental testing that should advance the field of electrochemical ion recovery.

cond-mat.mtrl-sci↗

arXiv2026

Heterogeneous dynamics in a polymer solution revealed through measurement of ultraslow convection

Understanding solution-phase aggregation and dynamics in complex fluids is critical for material processing, yet widely used dynamic light scattering (DLS) fails for strongly attenuating systems such as conjugated polymers. We use X-ray photon correlation spectroscopy (XPCS) to probe the dynamics of a polymer, PM7, in toluene, revealing unexpected oscillations in the autocorrelation function that show vertical flow during measurement. Despite the relatively low X-ray absorption, measured flow velocities scale with X-ray beam power and suggest convective transport. Our analyses reveal both mobile and static scatterers that together produce oscillatory, heterodyne features in the measured correlation functions. Finite element simulations predict flow velocities much larger than observed, suggesting that entanglements of the aggregates slow their motion. These results provide a direct measurement of ultra-slow convection and highlight the need to explicitly account for even modest beam heating in interpreting XPCS results. Moreover, the observation of distinct scatterer populations underscores the structural complexity of conjugated polymer solutions.

cond-mat.soft↗

arXiv2026

"X-ray Coulomb Counting" to understand electrochemical systems

Electrochemical systems are important for a sustainable and defossilized energy system of the future. While accurate and precise, the corresponding electrochemical measurements, in which many reactions may occur simultaneously, often do not contain enough information to understand the underlying mechanism and processes. This information, however, is crucial towards rational materials and devices as well as process development and for inventing innovative concepts. In this perspective, we introduce explicitly the concept of "X-ray Coulomb Counting" in which X-ray methods are used to quantify on an absolute scale how much charge is transferred into which reactions during the electrochemical measurements. This allows to interpret the electrochemical measurements in detail and obtain the desired phenomenological and mechanistic understanding. We show a few recent examples from the Li-ion battery literature in which the concept of X-ray Coulomb Counting was employed to obtain foundational understanding.

cond-mat.mtrl-sci↗

arXiv2026

3D Electron Diffraction -- The Missing Slice for a Complete Nanoscale Analysis of Organic Solar Cells in TEM

Optimizing the performance of organic solar cells (OSCs) hinges on a comprehensive understanding of their nanostructures, yet traditional characterization methods often fall short, delivering incomplete structural snapshots. We introduce elastically filtered 3D Electron Diffraction (3D ED) as a ground-breaking technique bridging full reciprocal- and real-space structural analysis within a single transmission electron microscope (TEM). Using solvent-vapor annealed DRCN5T:PC71BM, 3D ED reproduces key structural parameters from GIWAXS including lattice spacings, coherence lengths, and mosaicity, while uniquely delivering true in-plane access and direct registration with high-resolution imaging, diffraction imaging and nano-spectroscopy on the same sample. A low-dose, distributed tilt strategy plus energy filtering yields high signal-to-background below damage thresholds. Extension to a second archetypal blend (P3HT:PC71BM; annealing evolution) demonstrates generality. Our findings underscore the transformative potential of 3D ED, particularly in analysing beam-sensitive organic thin films. This paves the way for new avenues in advanced correlative structural characterization of OSCs and holds potential for application to a multitude of other nanostructured materials.

cond-mat.mtrl-sci↗

arXiv2025

A systematic approach for quantitative orientation and phase fraction analysis of thin films through grazing incidence X-ray diffraction

Grazing incidence X-ray diffraction (GIXD) is widely used for the structural characterization of thin films, particularly for analyzing phase composition and the orientation distribution of crystallites. While various tools exist for qualitative evaluation, a widely applicable systematic procedure to achieve quantitative information has not yet been developed. This work presents a first step in that direction, allowing accurate quantitative information to be achieved through the evaluation of radial line profiles from GIXD data. An algorithm is introduced for computing radial line profiles based on the crystal structure of known compounds. By fitting experimental data with calculated line profiles, accurate quantitative information about orientation distribution and phase composition is obtained, along with additional parameters such as mosaicity and total crystal volume. The approach is demonstrated using three distinct thin film systems, highlighting the broad applicability of the algorithm. This method provides a systematic and general approach to obtaining quantitative information from GIXD data.

cond-mat.mtrl-sci↗

arXiv2024

Electrochemical Removal of HF from Carbonate-based $LiPF_6$-containing Li-ion Battery Electrolytes

Due to the hydrolytic instability of $LiPF_6$ in carbonate-based solvents, HF is a typical impurity in Li-ion battery electrolytes. HF significantly influences the performance of Li-ion batteries, for example by impacting the formation of the solid electrolyte interphase at the anode and by affecting transition metal dissolution at the cathode. Additionally, HF complicates studying fundamental interfacial electrochemistry of Li-ion battery electrolytes, such as direct anion reduction, because it is electrocatalytically relatively unstable, resulting in LiF passivation layers. Methods to selectively remove ppm levels of HF from $LiPF_6$-containing carbonate-based electrolytes are limited. We introduce and benchmark a simple yet efficient electrochemical in situ method to selectively remove ppm amounts of HF from $LiPF_6$-containing carbonate-based electrolytes. The basic idea is the application of a suitable potential to a high surface-area metallic electrode upon which only HF reacts (electrocatalytically) while all other electrolyte components are unaffected under the respective conditions.

cond-mat.mtrl-sci↗

arXiv2023

The nature of dynamic local order in CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$

Hybrid lead halide perovskites (LHPs) are a class of semiconductor with novel properties that are distinctively governed by structural fluctuations. Diffraction experiments sensitive to average, long-range order reveal a cubic structure in the device-relevant, high-temperature phase. Local probes find additional short-range order with lower symmetry that may govern the structure-function relationships of LHPs. However, the dimensionality, participating atoms, and dynamics of this short-range order are unresolved, impeding our understanding of technologically relevant properties including long carrier lifetimes and facile halide migration. Here, we determine the true structure of two prototypical hybrid LHPs, CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$, using a combination of single-crystal X-ray and neutron diffuse scattering, neutron inelastic spectroscopy, and molecular dynamics simulations. The remarkable collective dynamics we found are not suggested by previous studies and consist of a network of local two-dimensional, circular pancake-like regions of dynamically tilting lead halide octahedra (lower symmetry) that induce longer range intermolecular correlations within the CH$_3$NH$_3^+$ sublattice. The dynamic local structure can introduce transient ferroelectric or antiferroelectric domains that increase charge carrier lifetimes, and strongly affect the halide migration, a poorly understood degradation mechanism. Our approach of co-analyzing single-crystal X-ray and neutron diffuse scattering data with MD simulations will provide unparalleled insights into the structure of hybrid materials and materials with engineered disorder.

cond-mat.mtrl-sci↗

arXiv2021

Unraveling the Unconventional Order of a High-Mobility Indacenodithiophene-Benzothiadiazole Copolymer

A new class of donor-acceptor (D-A) copolymers found to produce high charge carrier mobilities competitive with amorphous silicon ($> 1 cm^{2}V^{-1}s^{-1}$) exhibits the puzzling microstructure of substantial local order, however lacking long-range order and crystallinity previously deemed necessary for achieving high mobility. Here, we demonstrate the application of low-dose transmission electron microscopy to image and quantify the nanoscale and mesoscale organization of an archetypal D-A copolymer across areas comparable to electronic devices (~ $9 μm^{2}$). The local structure is spatially resolved by mapping the backbone (001) spacing reflection, revealing nanocrystallites of aligned polymer chains over nearly the entire film. Analysis of the nanoscale structure of its ordered domains suggests significant short- and medium-range order and preferential grain boundary orientations. Moreover, we provide insights into the rich, interconnected mesoscale organization of this new family of D-A copolymers by analysis of the local orientational spatial autocorrelations.

cond-mat.mtrl-sci↗