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Lukas Mielke

Publications and source records attributed to Lukas Mielke.

3 recordsLinked to original sources

Dynamic Sensing via Photomodulated Gas Desorption in Plasmonic Nanoparticle Chemiresistors

Quasi-static sensing, i.e., measurement of a sensor signal change induced by analyte presence with respect to a baseline signal observed in a reference gas beforehand, is the state of the art for qualitative and quantitative analyte identification in chemiresistive sensing. However, this approach is prone to baseline drift and, especially for inexpensive miniaturized point-of-care sensors, repeated calibration with reference gas is not feasible. To access reliable baseline information, active switching between analyte and reference gas would be required, causing a limitation for miniaturized implementation. Dynamic excitation of sensors offers an alternative: Via external stimuli the sensor is reversibly driven out of equilibrium in a controlled way, and the resulting transient sensor response, which is dependent on analytes present, is recorded and interpreted. Correlation of excitation and response signals can reduce effects of baseline drift and furthermore, dynamic features in sensor responses may contain valuable information. Especially light activation is a powerful and potentially miniaturizable approach to agitate sorption processes and therefore induce dynamics. In this work we report photothermal heating of hybrid, chemiresistive gold nanoparticle composites via LED excitation matching the plasmon resonance, to dynamically shift the analyte sorption equilibrium and induce dynamic sensor responses in a highly controlled way. We demonstrate that these sensor responses enable the detection of volatile organic compounds (VOC) via interpretation of differential signal components and that this approach improves the chemiresistors' baseline stability.

physics.app-ph

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

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