arXiv subjects

Andreas Fery

Publications and source records attributed to Andreas Fery.

9 recordsLinked to original sources

arXiv2025

Nanoscale Charge Transport in Au@PANI Assemblies: Bulk-like Films and Linear Assemblies

Hybrid nanostructures from metal nanoparticles equipped with conducting polymer shells are of great interest for use as functional materials in sensing and optoelectronics, as well as for ink-deposited conductors. Here, we investigate the charge transport mechanism of nanostructures composed of gold nanoparticles coated with a polyaniline shell (Au@PANI). In particular, we focus on how geometry influences the charge transport behavior. Highly ordered linear assemblies of Au@PANI nanoparticles were fabricated using template-assisted assembly, while bulk-like films were obtained via drop-casting. Temperature-dependent transport measurements were analyzed using established conductance models. Linear assemblies exhibit more localized transport, characterized by variable-range hopping (VRH) and thermally assisted tunneling (TAT), whereas bulk-like films show more delocalized transport, dominated by Arrhenius-type and thermionic conduction. These findings highlight the critical role of geometry, also due to its effect on electrical field strength in determining charge transport mechanisms in nanoparticle-based hybrid systems.

physics.app-ph↗

arXiv2025

How Microplastics cross the Buoyancy Barrier: A multi-scale Study

Microplastics (MPs), though less dense than water, are frequently recovered from sediments in aqueous environments, indicating they can cross the buoyancy barrier. We quantify eco-corona mediated MP-sediment attraction and MP transport from the nanoscale to the macroscale, linking all scales to a coherent mechanism explaining how MP overcome buoyancy and settle in sediments through interaction with suspended sediment. Colloidal probe atomic force microscopy (CP-AFM) detected attractive forces (0.15 - 17 mN/m) enabling heteroaggregation. Microscale tests confirmed aggregation and on larger scales sediment retention more than doubled with an eco-corona. Simulations showed that environmental shear force ($4 \cdot 10^{-4} mN/m$) cannot disrupt aggregates. In sedimentation columns, biofilm-covered MPs settled twice as often as plain MPs in bentonite suspensions. MP retention increased by 32 %. These results demonstrate that eco-corona/biofilm-mediated heteroaggregation is a robust pathway for MP sinking, accumulation, and retention in sediment beds. By identifying physical interaction thresholds and aggregation stability, we provide mechanistic insight into MP fate, highlight probable accumulation hotspots, and offer an evidence base for improved risk assessment and environmental modelling.

cond-mat.soft↗

arXiv2025

Molecular Cross-linking of MXenes: Tunable Interfaces and Chemiresistive Sensing

MXenes, a family of 2D transition metal compounds, have emerged as promising materials due to their unique electronic properties and tunable surface chemistry. However, the translation of these nanoscale properties into macroscopic devices is constrained by suitable cross-linking strategies that enable both processability and controlled inter-flake charge transport. Herein, we demonstrate the tunability of interfaces and the inter-layer spacing between Ti$_3$C$_2$T$_x$ MXene flakes through molecular cross-linking with homologous diamines. Oleylamine was first used to stabilize MXenes in chloroform, followed by diamine-mediated cross-linking to tune precisely the interlayer spacing. Grazing incidence X-ray scattering (GIXRD/GIWAXS) confirmed the correlation between ligand chain length and inter-layer spacing, which was further supported by Density Functional Theory (DFT) calculations. Furthermore, we investigated the charge transport properties of thin films consisting of these diamine-crosslinked Ti$_3$C$_2$T$_x$ MXenes and observed a strong dependence of the conductivity on the interlayer spacing. The dominating charge transport mechanism is variable range hopping (VRH) in accordance with the structure analysis of the films. Finally, we probed chemiresistive vapor sensing in MXene composites, observing pronounced water sensitivity and selectivity, highlighting their potential for use in humidity sensors. Insights into molecular cross-linking and its impact on charge transport open avenues for next-generation MXene-based electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Plasmonic Particle Integration into Near-Infrared Photodetectors and Photoactivated Gas Sensors: Towards Sustainable Next-Generation Ubiquitous Sensing

Current challenges in environmental science, medicine, food chemistry as well as the emerging use of artificial intelligence for solving problems in these fields require distributed, local sensing. Such ubiquitous sensing requires components with (1) high sensitivity, (2) power efficiency, (3) miniaturizability and (4) the ability to directly interface with electronic circuitry, i.e., electronic readout of sensing signals. Over the recent years, several nanoparticle-based approaches have found their way into this field and have demonstrated high performance. However, challenges remain, such as the toxicity of many of today's narrow bandgap semiconductors for NIR detection and the high energy consumption as well as low selectivity of state-of-the-art commercialized gas sensors. With their unique light-matter interaction and ink-based fabrication schemes, plasmonic nanostructures provide potential technological solutions to these challenges, leading also to better environmental performance. In this perspective we discuss recent approaches of using plasmonic nanoparticles for the fabrication of NIR photodetectors and light-activated, energy-efficient gas sensing devices. In addition, we point out new strategies implying computational approaches for miniaturizable spectrometers, exploiting the wide spectral tunability of plasmonic nanocomposites, and for selective gas sensors, utilizing dynamic light activation. The benefits of colloidal approaches for device fabrication are discussed with regard to technological advantages and environmental aspects, which have been barely considered so far.

physics.app-ph↗

arXiv2024

Structural Reinforcement in Mechanically Interlocked Two-Dimensional Polymers by Suppressing Interlayer Sliding

Preserving the superior mechanical properties of monolayer two-dimensional (2D) materials when transitioning to bilayer and layer-stacked structures poses a great challenge, primarily arising from the weak van der Waals (vdW) forces that facilitate interlayer sliding and decoupling. Here, we discover that mechanically interlocked 2D polymers (2DPs) offer a means for structural reinforcement from monolayer to bilayer. Incorporating macrocyclic molecules with one and two cavities into 2DPs backbones enables the precision synthesis of mechanically interlocked monolayer (MI-M2DP) and bilayer (MI-B2DP). Intriguingly, we have observed an exceptionally high effective Young's modulus of 222.4 GPa for MI-B2DP, surpassing those of MI-M2DP (130.1 GPa), vdW-stacked MI-M2DPs (2 MI-M2DP, 8.1 GPa) and other reported multilayer 2DPs. Modeling studies demonstrate the extraordinary effectiveness of mechanically interlocked structures in minimizing interlayer sliding (~0.1 {\AA}) and energy penalty (320 kcal/mol) in MI-B2DP compared to 2 MI-M2DP (~1.2 {\AA}, 550 kcal/mol), thereby suppressing mechanical relaxation and resulting in prominent structural reinforcement.

physics.chem-ph↗

arXiv2021

Repulsive interactions of eco-corona covered microplastic particles quantitatively follow modelling of polymer brushes

Environmental fate and toxicity of microplastic particles is dominated by their surface properties. In the environment an adsorbed layer of biomolecules and natural organic matter forms the so-called eco-corona. A quantitative description of how this eco-corona changes the particles' colloidal interactions is still missing. Here, we demonstrate with colloidal probe-atomic force microscopy that the formation of the eco-corona on microplastic particles introduces a soft film on the surface which changes the mechanical behaviour. We measure single particle-particle interactions and find a pronounced increase of long-range repulsive interactions upon eco-corona formation. These force-distance characteristics follow well the polymer brush model by Alexander and de Gennes. We further compare the obtained fitting parameters to known systems like polyelectrolyte multilayers and propose these as a model system for the eco-corona. The foundation of the eco-corona interacting like a polymer brush with its surrounding may help understand microplastic transport and aggregation in the environment.

cond-mat.soft↗

arXiv2019

Silver particles with rhombicuboctahedral shape and effectively isotropic interactions with light

Truly spherical silver nanoparticles are of great importance for fundamental studies including plasmonic applications, but the direct synthesis in aqueous media is not feasible. Using the commonly employed copper-based etching processes, isotropicplasmonic response can be achieved by etching well-defined silver nanocubes. Whilst spherical like shape is typically prevailing in such processes, we established that there is a preferential growth towards silver rhombicuboctahedra (AgRCOs), which is thethermodynamically most stable product of this synthesis. The rhombicuboctahedral morphology is further evidenced by comprehensive characterization with small-angle X-ray scattering in combination with TEM tomographyand high resolution TEM. Wealso elucidate the complete reaction mechanism based on UV-Vis kinetic studies, and the postulated mechanism can also be extended to all copper-based etching processes.

physics.app-ph↗

arXiv2019

Direct Observation of Plasmon Band Formation and Delocalization in Quasi-Infinite Nanoparticle Chains

Chains of metallic nanoparticles sustain strongly confined surface plasmons with relatively low dielectric losses. To exploit these properties in applications,such as waveguides, the fabrication of long chains of low disorder and a thorough understanding of the plasmon-mode properties, such as dispersion relations, are indispensable. Here, we use a wrinkled template for directed self-assembly to assemble chains of gold nanoparticles. With this up-scalable method, chain lengths from two particles (140 nm) to 20 particles (1500 nm) and beyond can be fabricated. Electron energy-loss spectroscopy supported by boundary element simulations, finite-difference time-domain, and a simplified dipole coupling model reveal the evolution of a band of plasmonic waveguide modes from degenerated single-particle modes in detail. In striking difference from plasmonic rod-like structures, the plasmon band is confined in excitation energy, which allows light manipulations below the diffraction limit. The non-degenerated surface plasmon modes show suppressed radiative losses for efficient energy propagation over a distance of 1500 nm.

cond-mat.mes-hall↗

arXiv2018

Efficient energy propagation through self-assembled gold nanoparticle chain waveguides

The strong interaction of light with metallic nanoparticles enables field confinement well below the diffraction limit. Plasmonic waveguides consisting of metal nanoparticle chains could be used for the propagation of energy or information on the nanoscale, but high losses have thus far impeded practical applications. Here we demonstrate that efficient waveguiding is possible through gold nanoparticle chains despite the high dissipative losses of gold. A DNA origami directed self-assembly of monocrystalline, spherical nanoparticles allows the interparticle spacing to be decreased to 2 nm or below, which gives rise to lower-energy plasmon resonance modes. Our simulations imply that these lower energy modes allow efficient waveguiding but collapse if interparticle gap sizes are increased. Individual waveguides are characterized with nanometer-resolution by electron energy loss spectroscopy, and directed propagation of energy towards a fluorescent nanodiamond and nanoscale energy conversion is shown by cathodoluminescence imaging spectroscopy on a single-device level. With this approach, micrometer-long propagation lengths might be achieved, enabling applications in information technology, sensing and quantum optics.

physics.optics↗