arXiv subjects

Lothar Houben

Publications and source records attributed to Lothar Houben.

14 recordsLinked to original sources

arXiv2026

Discovery of New Zintl Films and Nanowires Grown by Topotaxy Conversion of III-V Semiconductors

Zintl phases draw broad interest for their diverse structural, magnetic, thermoelectric, topological and optical properties. Recently, Zintl Eu$_3$In$_2$As$_4$ and Eu$_5$In$_2$As$_6$ nanowires with axion magneto-topology have been synthesized by molecular beam epitaxy via topotactic conversion of InAs wurtzite and zincblende nanowires. Here we extend this methodology, demonstrating that topotaxial mutual-exchange growth applies not only to a broader set of III-V semiconductors beyond InAs but also to three-dimensional substrates whose surfaces are converted into Zintl thin films, as well as to nanowires. We report the growth of two new compounds: Eu$_5$Ga$_2$As$_6$ thin films converted from GaAs substrates, and Eu$_5$Al$_2$As$_6$ thin films from AlAs films. We also convert GaAs nanowires of both wurtzite and zincblende structures into Eu$_5$Ga$_2$As$_6$ nanowires. Though the stoichiometry is the same as in the previously reported Eu$_5$In$_2$As$_6$ case, microscopy and diffraction reveal a single-phase Pnma symmetry group rather than Pbam, highlighting symmetry-guided topotactic pathways to new Zintl frameworks. The compounds host an intricate magnetic phase diagram with three magnetic transitions, including two distinct antiferromagnetic orders and a canted antiferromagnetic phase that evolves into another antiferromagnetic phase under applied field through a spin-flop transition. Ab initio calculations predict that both Zintls are semiconductors with gaps of 0.79 eV in Eu$_5$Ga$_2$As$_6$ and 0.90 eV in Eu$_5$Al$_2$As$_6$. The lower symmetry and increased structural complexity suggest suppressed lattice thermal conductivity, pointing to thermoelectric potential alongside prospects in spintronics and detector technologies. These results give an epitaxy-compatible route for discovering and integrating magnetic Zintl thin films and nanowires directly from relevant III-V semiconductors.

cond-mat.mtrl-sci↗

arXiv2026

DINO4DSTEM: A self-supervised framework for structural discovery in 4D-STEM

Nanodiffraction using 4D-STEM has become a key technique for quantitative nanoscale structural mapping in materials research, yet interpreting its high-dimensional datasets in structurally complex materials remains a major bottleneck. Existing analysis workflows typically rely on structural models, manual annotation, predefined classes, or sample-specific heuristics, limiting their ability to characterize heterogeneous complex materials. Here, we introduce DINO4DSTEM, a self-supervised machine learning framework that automatically discovers structurally meaningful states directly from raw diffraction data. Without structural models, manual labels, a predefined number of classes, or system-specific parameter tuning, the framework learns representations that organize diffraction patterns by their intrinsic structural similarities, transforming large collections of low-dose measurements into quantitative nanoscale structure maps. Across diverse datasets, DINO4DSTEM consistently identifies the dominant structural degrees of freedom, providing segmentation without human supervision. We applied the framework to the crystallization of indomethacin, a beam-sensitive, multidomain pharmaceutical system, revealing that crystallinity emerges from a partially ordered precursor and spans a continuous spectrum of structural order. The discovered nanoscale structural states are mapped to reveal the evolution of order across the specimen quantitatively. By replacing task-specific analysis with general self-supervised representation learning, DINO4DSTEM provides a broadly applicable framework for quantitative nanoscale structural mapping in complex materials, enabling the discovery of emergent structural organization in heterogeneous, beam-sensitive systems.

cond-mat.mtrl-sci↗

arXiv2026

Chiral Epitaxy: Enantioselective Growth of Chiral Nanowires on Low-Symmetry Two-Dimensional Materials

Chiral crystals exhibit useful handedness-dependent properties, including spin selectivity and circularly polarized light sensitivity, yet controlling which enantiomer forms during synthesis remains a central challenge. Existing approaches utilize molecules in solution to template crystal growth, which restricts processing conditions and introduces organic contaminants incompatible with device fabrication. Enantioselective growth of a chiral crystal on a chiral surface via vapor-phase synthesis (chiral epitaxy) has not yet been demonstrated. Here, we show chiral epitaxy of aligned tellurium nanowires on a low-symmetry two-dimensional material, ReSe2. In situ electron microscopies suggest a mechanism where handedness is determined at nucleation by the interface energy difference between Te enantiomers and the chiral substrate surface. Chiral epitaxy provides a solvent-free, vapor-solid route to homochiral crystals compatible with semiconductor and quantum manufacturing processes.

cond-mat.mtrl-sci↗

arXiv2025

Topotactic Growth of Zintl Phase Eu$_5$In$_2$As$_6$ Nanowires with Antiferromagnetic Behavior

We demonstrate a topotactic transformation of zincblende InAs(Sb) nanowires into the Zintl phase Eu$_5$In$_2$As$_6$ through a vapor-solid mutual exchange process involving Eu and In in molecular beam epitaxy. This conversion preserves the polyhedral coordination lattice of the parent InAs(Sb) structure while inducing orthorhombic symmetry in the product phase, Eu$_5$In$_2$As$_6$, in which quasi-one-dimensional [InAs$_3$]$^6$$^-$ chains with tetrahedral sites align along the <110> direction of the zincblende structure. Local and global magnetic characterization identified two distinct antiferromagnetic phase transitions at approximately 7 K and 16 K in Eu$_5$In$_2$As$_6$ nanowires, potentially classified as altermagnetic phases. The versatility of the topotactic conversion of III-V semiconductor nanowires provides a platform for designing functional Zintl materials with tunable magnetic properties, making them promising candidates for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Topotaxial Mutual-Exchange Growth of Magnetic Zintl Eu$_3$In$_2$As$_4$ Nanowires with Axion Insulator Classification

Nanomaterials bring to expression unique electronic properties that promote advanced functionality and technologies. Albeit, nanoscale growth presents paramount challenges for synthesis limiting the diversity in structures and compositions. Here, we demonstrate solid-state topotactic exchange that converts Wurtzite InAs nanowires into Zintl phase Eu$_3$In$_2$As$_4$ nanowires. In situ evaporation of Eu and As over InAs nanowire cores in molecular beam epitaxy results in mutual exchange of Eu from the shell and In from the core. A continuous Eu$_3$In$_2$As$_4$ shell thereby grows that gradually consumes the InAs core and converts it into a single phase Eu$_3$In$_2$As$_4$ nanowire. Topotaxy, which facilitates the mutual exchange, is supported by the substructure of the As matrix which is similar across the Wurtzite InAs and Zintl Eu$_3$In$_2$As$_4$. We provide initial evidence of an antiferromagnetic transition at T$_N$ $\sim$ 6.5 K in the Zintl phase Eu$_3$In$_2$As$_4$ nanowires. Ab initio calculation confirms the antiferromagnetic state and classifies Eu$_3$In$_2$As$_4$ as a $C_2 T$ axion insulator hosting both chiral hinge modes and unpinned Dirac surface states. The topotactic mutual-exchange growth of Zintl Eu$_3$In$_2$As$_4$ nanowires thus enables the exploration of intricate magneto-topological states of nanomaterials. Moreover, it may open the path for topotactic mutual-exchange synthesis of nanowires made of other exotic compounds.

cond-mat.mtrl-sci↗

arXiv2020

Growth-Etch Metal-Organic Chemical Vapor Deposition Approach of WS2 Atomic-Layers

Metal organic chemical vapor deposition (MOCVD) is one of the main methodologies used for thin film fabrication in the semiconductor industry today and is considered one of the most promising routes to achieve large-scale and high-quality 2D transition metal dichalcogenides (TMDCs). However, if not taken special measures, MOCVD suffers from some serious drawbacks, such as small domain size and carbon contamination, resulting in poor optical and crystal quality, which may inhibit its implementation for the large-scale fabrication of atomic-thin semiconductors. Here we present a Growth-Etch MOCVD (GE-MOCVD) methodology, in which a small amount of water vapor is introduced during the growth, while the precursors are delivered in pulses. The evolution of the growth as a function of the amount of water vapor, the number and type of cycles and the gas composition is described. We show a significant domain size increase is achieved relative to our conventional process. The improved crystal quality of WS2 (and WSe2) domains was demonstrated by means of Raman spectroscopy, photoluminescence (PL) spectroscopy and HRTEM studies. Moreover, time-resolved PL studies show very long exciton lifetimes, comparable to those observed in mechanically exfoliated flakes. Thus, the GE-MOCVD approach presented here may facilitate their integration into a wide range of applications.

physics.app-ph↗

arXiv2020

Vacuum Rabi splitting of a dark plasmonic cavity mode revealed by fast electrons

Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenced by Rabi-split spectra. Coupling strengths of up to 85 meV place the bowtie-emitter devices at the onset of the strong coupling regime. Remarkably, the coupling occurs at the bowtie gap periphery, even while the electron beam probes their center. Our findings pave the way for using EEL spectroscopy to study exciton-plasmon interactions involving non-emissive photonic modes.

cond-mat.mes-hall↗

arXiv2017

Nanoscale X-ray investigation of magnetic metallofullerene peapods

Endohedral lanthanide ions packed inside carbon nanotubes (CNTs) in a one-dimensional assembly have been studied with a combination of high resolution transmission electron microscopy (HRTEM), scanning transmission X-ray microscopy (STXM), and X-ray magnetic circular dichroism (XMCD). By correlating HRTEM and STXM images we show that structures down to 30 nm are resolved with chemical contrast and record X-ray absorption spectra from endohedral lanthanide ions embedded in individual nanoscale CNT bundles. XMCD measurements of an Er$_3$N@C$_{80}$ bulk sample and a macroscopic assembly of filled CNTs indicates that the magnetic properties of the endohedral Er3+ ions are unchanged when encapsulated in CNTs. This study demonstrates the feasibility of local magnetic X-ray characterization of low concentrations of lanthanide ions embedded in molecular nanostructures.

cond-mat.mtrl-sci↗

arXiv2017

Probing the local nature of excitons and plasmons in few-layer MoS2

Excitons and plasmons are the two most fundamental types of collective electronic excitations occurring in solids. Traditionally, they have been studied separately using bulk techniques that probe their average energetic structure over large spatial regions. However, as the dimensions of materials and devices continue to shrink, it becomes crucial to understand how these excitations depend on local variations in the crystal- and chemical structure on the atomic scale. Here we use monochromated low-loss scanning-transmission-electron-microscopy electron-energy-loss (LL-STEM-EEL) spectroscopy, providing the best simultaneous energy and spatial resolution achieved to-date to unravel the full set of electronic excitations in few-layer MoS2 nanosheets over a wide energy range. Using first-principles many-body calculations we confirm the excitonic nature of the peaks at ~2eV and ~3eV in the experimental EEL spectrum and the plasmonic nature of higher energy-loss peaks. We also rationalise the non-trivial dependence of the EEL spectrum on beam and sample geometry such as the number of atomic layers and distance to steps and edges. Moreover, we show that the excitonic features are dominated by the long wavelength (q=0) components of the probing field, while the plasmonic features are sensitive to a much broader range of q-vectors, indicating a qualitative difference in the spatial character of the two types of collective excitations. Our work provides a template protocol for mapping the local nature of electronic excitations that open new possibilities for studying photo-absorption and energy transfer processes on a nanometer scale.

cond-mat.mtrl-sci↗

arXiv2017

Dynamic ligand control of crystalline phase and habit in cesium lead halide nanoparticles

Active control over the shape, composition and crystalline habit of nanocrystals is a long sought-after goal. Various methods have been shown to enable post-synthesis modification of nanoparticles, including the use of the Kirkendall effect, galvanic replacement and cation or anion exchange, all taking advantage of enhanced solid-state diffusion on the nanoscale. In all these processes, however, alteration of the nanoparticles requires introduction of new precursor materials. Here we show that for cesium lead halide perovskite nanoparticles, a reversible structural and compositional change can be induced at room temperature solely by modification of the ligand composition in solution. Reversible transformation of cubic CsPbX3 nanocrystals to rhombohedral Cs4PbX6 nanocrystals is achieved by controlling the ratio of oleylamine to oleic acid capping molecules. This scheme does not only enable fabrication of high purity monodisperse Cs4PbX6 nanoparticles with controlled sizes. Rather, dependent on the Cs4PbX6 nanoparticles final size afforded by reaction time, the back reaction yields CsPbX3 nanoplatelets with controlled thickness. These results shed some light on the unique properties of this family of materials, provide hints to the origin of their superb photovoltaic performance and point at possible routes for their controlled fabrication and stabilization.

cond-mat.mtrl-sci↗

arXiv2013

Line Defects in Molybdenum Disulfide Layers

Layered molecular materials and especially MoS2 are already accepted as promising candidates for nanoelectronics. In contrast to the bulk material, the observed electron mobility in single-layer MoS2 is unexpectedly low. Here we reveal the occurrence of intrinsic defects in MoS2 layers, known as inversion domains, where the layer changes its direction through a line defect. The line defects are observed experimentally by atomic resolution TEM. The structures were modeled and the stability and electronic properties of the defects were calculated using quantum-mechanical calculations based on the Density-Functional Tight-Binding method. The results of these calculations indicate the occurrence of new states within the band gap of the semiconducting MoS2. The most stable non-stoichiometric defect structures are observed experimentally, one of which contains metallic Mo-Mo bonds and another one bridging S atoms.

cond-mat.mtrl-sci↗

arXiv2013

Geometric reconstruction methods for electron tomography

Electron tomography is becoming an increasingly important tool in materials science for studying the three-dimensional morphologies and chemical compositions of nanostructures. The image quality obtained by many current algorithms is seriously affected by the problems of missing wedge artefacts and nonlinear projection intensities due to diffraction effects. The former refers to the fact that data cannot be acquired over the full $180^\circ$ tilt range; the latter implies that for some orientations, crystalline structures can show strong contrast changes. To overcome these problems we introduce and discuss several algorithms from the mathematical fields of geometric and discrete tomography. The algorithms incorporate geometric prior knowledge (mainly convexity and homogeneity), which also in principle considerably reduces the number of tilt angles required. Results are discussed for the reconstruction of an InAs nanowire.

math-ph↗

arXiv2011

New route for stabilization of 1T-WS2 and MoS2 phases

The phenomenon of a partial 2H\rightarrow1T phase transition within multiwalled WS2 nanotubes under substitutional Rhenium doping is discovered by means of high-resolution transmission electron microscopy. Using density-functional calculations for the related MoS2 compound we consider a possible origin of this phase transition, which was known formerly only for WS2 and MoS2 intercalated by alkali metals. An interplay between the stability of layered or nanotubular forms of 2H and 1T allotropes is found to be intimately related with their electronic structures and electro-donating ability of an impurity.

cond-mat.mtrl-sci↗

arXiv2011

Comprehensive characterization of an individual carbon nanotube transport device

We present a comprehensive characterization of an individual multiwalled carbon nanotube transport device combining electron microscopy and Raman spectroscopy with electrical measurements. Each method gives complementary information that mutually help to interpret each other. A sample design that allows for combining these investigation methods on individual carbon nanotube devices is introduced. This offers a direct correlation of transport features and shifts of Raman modes with structural properties as e.g. the contact interface and the morphology of the nanotube.

cond-mat.mes-hall↗