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Patrick Kluth

Publications and source records attributed to Patrick Kluth.

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Characterization of ion track etched conical nanopores in thermal and PECVD SiO$_{2}$ using small angle X-ray scattering

Conical nanopores in amorphous SiO$_{2}$ thin films fabricated using the ion track etching technique show promising potential for filtration, sensing and nanofluidic applications. The characterization of the pore morphology and size distribution, along with its dependence on the material properties and fabrication parameters, is crucial to designing nanopore systems for specific applications. Here, we present a comprehensive study of track-etched nanopores in thermal and plasma-enhanced chemical vapor deposited (PECVD) SiO$_{2}$ using synchrotron-based small-angle X-ray scattering (SAXS). We present a new approach for analyzing the complex highly anisotropic 2-dimensional SAXS patterns of the pores by reducing the analysis to two orthogonal 1-dimensional slices of the data. The simultaneous fit of the data enables an accurate determination of the pore geometry and size distribution. The analysis reveals substantial differences between the nanopores in thermal and PECVD SiO$_{2}$. The track-to-bulk etching rate ratio is significantly different for the two materials, producing nanopores with cone angles that differ by almost a factor of 2. Furthermore, thermal SiO$_2$ exhibits an exceptionally narrow size distribution of only ~2-4%, while PECVD SiO$_2$ shows a higher variation ranging from ~8-18%. The impact of ion energy between 89 MeV and 1.6 GeV on the size of the nanopores was also investigated for pores in PECVD SiO$_{2}$ and shows only negligible influence. These findings provide crucial insights for the controlled fabrication of conical nanopores in different materials, which is essential for optimizing membrane performance in applications that require precise pore geometry.

physics.app-ph

High Accuracy Protein Identification: Fusion of solid-state nanopore sensing and machine learning

Proteins are arguably the most important class of biomarkers for health diagnostic purposes. Label-free solid-state nanopore sensing is a versatile technique for sensing and analysing biomolecules such as proteins at single-molecule level. While molecular-level information on size, shape, and charge of proteins can be assessed by nanopores, the identification of proteins with comparable sizes remains a challenge. Here, we present methods that combine solid-state nanopore sensing with machine learning to address this challenge. We assess the translocations of four similarly sized proteins using amplifiers with bandwidths (BWs) of 100 kHz (sampling rate=200 ksps) and 10 MHz (sampling rate=40 Msps), the highest bandwidth reported for protein sensing, using nanopores fabricated in <10 nm thick silicon nitride membranes. F-values of up to 65.9% and 83.2% (without clustering of the protein signals) were achieved with 100 kHz and 10 MHz BW instruments, respectively, for identification of the four proteins. The accuracy of protein identification was significantly improved by grouping the signals into several clusters depending on the event features, resulting in F-value and specificity reaching as high as 88.7% and 96.4%, respectively, for combinations of four proteins. The combined improvement in sensor signals through the use of high bandwidth instruments, advanced clustering, machine learning, and other advanced data analysis methods allows identification of proteins with high accuracy.

physics.bio-ph

Highly Rectifying Conical Nanopores in Amorphous SiO2 Membranes for Nanofluidic Osmotic Power Generation and Electroosmotic Pumps

Nanopore membranes are a versatile platform for a wide range of applications ranging from medical sensing to filtration and clean energy generation. To attain high-flux rectifying ionic flow, it is required to produce short channels exhibiting asymmetric surface charge distributions. This work reports on a system of track etched conical nanopores in amorphous SiO$_2$ membranes, fabricated using the scalable track etch technique. Pores are fabricated by irradiation of 1 $μ$m thick SiO$_2$ windows with 2.2 GeV $^{197}$Au ions and subsequent chemical etching. Structural characterisation is performed using atomic force microscopy (AFM), scanning electron microscopy (SEM), small angle X-ray scattering (SAXS), ellipsometry, and surface profiling. Conductometric characterisation of the pore surface is performed using a membrane containing 16 pores, including an in-depth analysis of ionic transport characteristics. The pores have a tip radius of (5.7 $\pm$ 0.1) nm, a half-cone angle of (12.6 $\pm$ 0.1)$^{\circ}$, and a length of (710 $\pm$ 5) nm. The $pK_a$, $pK_b$, and $pI$ are determined to 7.6 $\pm$ 0.1, 1.5 $\pm$ 0.2, and 4.5 $\pm$ 0.1, respectively, enabling the fine-tuning of the surface charge density between +100 and -300 mC $m^{-2}$ and allowing to achieve an ionic current rectification ratio of up to 10. This highly versatile technology addresses challenges that contemporary nanopore systems face, and offers a platform to improve the performance of existing applications.

cond-mat.mes-hall

Annealing of swift heavy ion tracks in amorphous silicon dioxide

The annealing kinetics of the high energy ion damage in amorphous silicon dioxide (a-SiO2) are still not well understood, despite the material's widespread application in material science, physics, geology, and biology. This study investigates how annealing temperature, duration, and ambient environment affect the recovery of irradiation damage produced along the trajectory of swift heavy ions in a-SiO2. The track-annealing kinetics and the changing ion track morphology were investigated using synchrotron-based small-angle X-ray scattering (SAXS) and etching methods. We found that track annealing proceeds quicker near the sample surface demonstrated by a changing track etch rate as a function of depth. Measurements of ion tracks using SAXS show only small changes in the radial density distribution profile of the ion tracks. Activation energy of the annealing process at different sample depths was determined and the effect of the capping layer during the annealing process was also studied. Combination of oxygen diffusion and stress relaxation may contribute to the observed behaviour of preferential and anisotropic healing of the ion track. The results add to the fundamental understanding of ion track damage recovery and may have direct implications for materials for radioactive waste storage and solid state nanopores.

cond-mat.mtrl-sci

Ultra-Thin, High-Lifetime Silicon Nitride Membranes for Nanopore Sensing

Thin membranes are highly sought-after for nanopore-based single-molecule sensing and fabrication of such membranes becomes challenging in the \lesssim10 nm thickness regime where a plethora of useful molecule information can be acquired by nanopore sensing. In this work, we present a scalable and controllable method to fabricate silicon nitride (SixNy) membranes with effective thickness down to ~1.5 nm using standard silicon processing and chemical etching using hydrofluoric acid (HF). Nanopores were fabricated using the controlled breakdown method with estimated pore diameters down to ~1.8 nm yielding events >500,000 and >1,800,000 from dsDNA and bovine serum albumin (BSA) protein, respectively, demonstrating the high-performance and extended lifetime of the pores fabricated through our membranes. We used two different compositions of SixNy for membrane fabrication (near stoichiometric and silicon-rich SixNy) and compared them against commercial membranes. The final thicknesses of the membranes were measured using ellipsometry and were in good agreement with the values calculated from the bulk etch rates and DNA translocation characteristics. The stoichiometry and the density of the membrane layers were characterized with Rutherford backscattering spectrometry while the nanopores were characterized using pH-conductance, conductivity-conductance and power spectral density (PSD) graphs.

cond-mat.mtrl-sci

Influence of direct deposition of dielectric materials on the optical response of monolayer WS$_2$

The integration of two-dimensional transition metal dichalcogenide crystals (TMDCs) into a dielectric environment is critical for optoelectronic and photonic device applications. Here, we investigate the effects of direct deposition of different dielectric materials (Al$_2$O$_3$, SiO$_2$, SiN$_x$) onto atomically thin (monolayer) TMDC WS$_2$ on its optical response. Atomic layer deposition (ALD), electron beam evaporation (EBE), plasma enhanced chemical vapour deposition (PECVD), and magnetron sputtering methods of material deposition are investigated. The photoluminescence (PL) measurements reveal quenching of the excitonic emission after all deposition processes. The reduction in neutral exciton PL is linked to the increased level of charge doping and associated rise of the trion emission, and/or the localized (bound) exciton emission. Furthermore, Raman spectroscopy allows us to clearly correlate the observed changes of excitonic emission with the increased levels of lattice disorder and defects. Overall, the EBE process results in the lowest level of doping and defect densities and preserves the spectral weight of the exciton emission in the PL, as well as the exciton oscillator strength. Encapsulation with ALD appears to cause chemical changes, which makes it distinct from all other techniques. Sputtering is revealed as the most aggressive deposition method for WS$_2$, fully quenching its optical response. Our results demonstrate and quantify the effects of direct deposition of dielectric materials onto monolayer WS$_2$, which can provide a valuable guidance for the efforts to integrate monolayer TMDCs into functional optoelectronic devices.

cond-mat.mtrl-sci