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Spectrometer‐free Optical Hydrogen Sensing Based on Fano‐like Spatial Distribution of Transmission in a Metal−Insulator−Metal Plasmonic Doppler Grating
Optical nanosensors are promising for hydrogen sensing because they are small, free from spark generation, and feasible for remote optical readout. Conventional optical nanosensors require broadband excitation and spectrometers, rendering the devices bulky and complex. An alternative is spatial intensity-based optical sensing, which only requires an imaging system and a smartly designed platform to report the spatial distribution of analytical optical signals. Here, a spatial intensity-based hydrogen sensing platform is presented based on Fano-like spatial distribution of the transmission in a Pd-Al2O3-Au metal-insulator-metal plasmonic Doppler grating (MIM-PDG). The MIM-PDG manifests the Fano resonance as an asymmetric spatial transmission intensity profile. The absorption of hydrogen changes the spatial Fano-like transmission profiles, which can be analyzed with a “spatial” Fano resonance model and the extracted Fano resonance parameters can be used to establish analytical calibration lines. While gratings sensitive to hydrogen absorption are suitable for hydrogen sensing, hydrogen insensitive gratings are also found, which provide an unperturbed reference signal and may find applications in nanophotonic devices that require a stable optical response under fluctuating hydrogen atmosphere. The MIM-PDG platform is a spectrometer-free and intensity-based optical sensor that requires only an imaging system, making it promising for cellphone-based optical sensing applications. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH.
Liquid-Core Microstructured Polymer Optical Fiber as Fiber-Enhanced Raman Spectroscopy Probe for Glucose Sensing
This work reports the development and application of two liquid-core microstructured polymer optical fibers (LC-mPOF) with different microstructure sizes. They are used in a fiber-enhanced Raman spectroscopy sensing platform, with the aim of detecting glucose in aqueous solutions in the clinically relevant range for sodium-glucose cotransporter 2 inhibitor therapy. The sensing platform is tested for low-concentration glucose solutions using each LC-mPOF. Results confirm that a significant enhancement of the Raman signal is achieved in comparison to conventional Raman spectroscopy. Additional measurements are carried out to obtain the valid measurement range, the resolution, and the limit of detection, showing that the LC-mPOF with 66-µm-diameter central hollow core has the highest potential for future clinical applications. Finally, preliminary tests successfully demonstrate glucose identification in urine. © 1983-2012 IEEE.
1D p–n Junction Electronic and Optoelectronic Devices from Transition Metal Dichalcogenide Lateral Heterostructures Grown by One-Pot Chemical Vapor Deposition Synthesis
Lateral heterostructures of dissimilar monolayer transition metal dichalcogenides provide great opportunities to build 1D in-plane p–n junctions for sub-nanometer thin low-power electronic, optoelectronic, optical, and sensing devices. Electronic and optoelectronic applications of such p–n junction devices fabricated using a scalable one-pot chemical vapor deposition process yielding MoSe2-WSe2 lateral heterostructures are reported here. The growth of the monolayer lateral heterostructures is achieved by in situ controlling the partial pressures of the oxide precursors by a two-step heating protocol. The grown lateral heterostructures are characterized structurally and optically using optical microscopy, Raman spectroscopy/microscopy, and photoluminescence spectroscopy/microscopy. High-resolution transmission electron microscopy further confirms the high-quality 1D boundary between MoSe2 and WSe2 in the lateral heterostructure. p–n junction devices are fabricated from these lateral heterostructures and their applicability as rectifiers, solar cells, self-powered photovoltaic photodetectors, ambipolar transistors, and electroluminescent light emitters are demonstrated. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
Background Reduction in STED-FCS Using a Bivortex Phase Mask
Fluorescence correlation spectroscopy (FCS) is a valuable tool to study the molecular dynamics in living cells. When used together with a super-resolution stimulated emission depletion (STED) microscope, STED-FCS can measure diffusion processes on the nanoscale in living cells. In two-dimensional (2D) systems like the cellular plasma membrane, a ring-shaped depletion focus is most commonly used to increase the lateral resolution, leading to more than 25-fold decrease in the observation volume, reaching the relevant scale of supramolecular arrangements. However, STED-FCS faces severe limitations when measuring diffusion in three dimensions (3D), largely due to the spurious background contributions from undepleted areas of the excitation focus that reduce the signal quality and ultimately limit the resolution. In this paper, we investigate how different STED confinement modes can mitigate this issue. By simulations as well as experiments with fluorescent probes in solution and in cells, we demonstrate that the coherent-hybrid (CH) depletion pattern created by a bivortex phase mask reduces background most efficiently and thus provides superior signal quality under comparable reduction of the observation volume. Featuring also the highest robustness to common optical aberrations, CH-STED can be considered the method of choice for reliable STED-FCS-based investigations of 3D diffusion on the subdiffraction scale. Copyright © 2020 American Chemical Society.
Emission Manipulation by DNA Origami‐Assisted Plasmonic Nanoantennas
Plasmonic nanoantennas mediate far and near optical fields and confine the light to subwavelength dimensions. The spatial organization of nanoantenna elements is critical as it affects the interelement coupling and determines the resultant antenna mode. To couple quantum emitters to optical antennas, high precision on the order of a few nm with respect to the antenna is necessary. As an emerging nanofabrication technique, DNA origami has proven itself to be a robust nanobreadboard to obtain sub-5 nm positioning precision for a diverse range of materials. Eliminating the need for expensive state-of-the-art top-down fabrication facilities, DNA origami enables cost-efficient implementation of nanoscale architectures, including novel nanoantennas. The ability of DNA origami to deterministically position single quantum emitters into nanoscale hotspots further boosts the efficiency of light–matter interaction controlled via optical antennas. This review recapitulates the recent progress in plasmonic nanoantennas assisted by DNA origami and focuses on their various configurations. How those nanoantennas act on the emission and absorption properties of quantum emitters positioned in the hotspots is explicitly discussed. In the end, open challenges are outlined and future possibilities lying ahead are pointed out for this powerful triad of biotechnology, nanooptics, and photophysics. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
Non-invasive prospection techniques and direct push sensing as high-resolution validation tools in wetland geoarchaeology – Artificial water supply at a Carolingian canal in South Germany?
The prospection of (geo-)archaeological sites yield important knowledge about the concept and the utilisation of pre-historical and historical infrastructure. The satisfactory conduction of classical prospection methods like archaeological excavations or geoarchaeological vibra-coring might be challenging in the case of large sites or difficult underground conditions. This is particularly problematic in wetlands featuring a high groundwater table and high compaction rates of organic layers. In this study, we provide an alternative and non- to minimal-invasive exploration approach to discover hydro-engineering structures for artificial water supply in the surrounding of a Carolingian summit canal in South Germany. The Early Medieval Fossa Carolina was intended 792/793 CE to bridge the Central European watershed between Rhine-Main and Danube catchments. As the canal was constructed as a summit canal, an artificial water supply at the highest levels seemed very likely or even obligatory. In order to explore these obligatory hydro-engineering features, we use a wide range of on-site and off-site tools in a spatial hierarchical way. Our approach includes the large-scale SQUID magnetic survey and the sighting of historical maps. Furthermore, we integrate high-resolution direct push colour logs, and subsequent vibra-coring for small-scale stratigraphical verification and sedimentological analyses. The SQUID magnetic survey and related depth models discover two pronounced linear anomalies that might represent potential artificial water inlets in the North-Eastern and Northern Sections of the canal. I) In the North-Eastern Section, direct push colour logs, vibra-coring and 14C dating provide no evidence for a Carolingian hydro-engineering feature but reveal a natural lenticular structure of Early Holocene age. II) The linear magnetic anomaly in the Northern Section can be excluded with high probability as a hydro-engineering structure as well. Here, direct push colour logs, vibra-coring, 14C dating and the comparison with a historic map reveal evidence for a historic gravel road. Thus, we have nicely verified the magnetic information but have no prove for an artificial Carolingian water inlet from the Swabian Rezat River that contradicts with assumptions of former studies. © 2020 The Authors
Photodoping and Fast Charge Extraction in Ionic Carbon Nitride Photoanodes
Ionic carbon nitrides based on poly(heptazine imides) (PHI) represent a vigorously studied class of materials with possible applications in photocatalysis and energy storage. Herein, for the first time, the photogenerated charge dynamics in highly stable and binder-free PHI photoanodes using in operando transient photocurrents and spectroelectrochemical photoinduced absorption measurements is studied. It is discovered that light-induced accumulation of long-lived trapped electrons within the PHI film leads to effective photodoping of the PHI film, resulting in a significant improvement of photocurrent response due to more efficient electron transport. While photodoping is previously reported for various semiconductors, it has not been shown before for carbon nitride materials. Furthermore, it is found that the extraction kinetics of untrapped electrons are remarkably fast in these PHI photoanodes, with electron extraction times (ms) comparable to those measured for commonly employed metal oxide semiconductors. These results shed light on the excellent performance of PHI photoanodes in alcohol photoreforming, including very negative photocurrent onset, outstanding fill factor, and the possibility to operate under zero-bias conditions. More generally, the here reported photodoping effect and fast electron extraction in PHI photoanodes establish a strong rationale for the use of PHI films in various applications, such as bias-free photoelectrochemistry or photobatteries. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
Microfluidic chamber design for controlled droplet expansion and coalescence
The defined formation and expansion of droplets are essential operations for droplet-based screening assays. The volumetric expansion of droplets causes a dilution of the ingredients. Dilution is required for the generation of concentration graduation which is mandatory for many different assay protocols. Here, we describe the design of a microfluidic operation unit based on a bypassed chamber and its operation modes. The different operation modes enable the defined formation of sub-L droplets on the one hand and the expansion of low nL to sub-L droplets by controlled coalescence on the other. In this way the chamber acts as fluidic interface between two fluidic network parts dimensioned for different droplet volumes. Hence, channel confined droplets of about 30-40 nL from the first network part were expanded to cannel confined droplets of about 500 to about 2500 nL in the second network part. Four different operation modes were realized: (a) flow rate independent droplet formation in a self-controlled way caused by the bypassed chamber design, (b) single droplet expansion mode, (c) multiple droplet expansion mode, and (d) multiple droplet coalescence mode. The last mode was used for the automated coalescence of 12 droplets of about 40 nL volume to produce a highly ordered output sequence with individual droplet volumes of about 500 nL volume. The experimental investigation confirmed a high tolerance of the developed chamber against the variation of key parameters of the dispersed-phase like salt content, pH value and fluid viscosity. The presented fluidic chamber provides a solution for the problem of bridging different droplet volumes in a fluidic network. © 2020 by the authors.
Comparison of novel semi-airborne electromagnetic data with multi-scale geophysical, petrophysical and geological data from Schleiz, Germany
In the framework of the Deep Electromagnetic Sounding for Mineral EXploration (DESMEX) project, we carried out multiple geophysical surveys from regional to local scales in a former mining area in the state of Thuringia, Germany. We prove the applicability of newly developed semi-airborne electromagnetic (EM) systems for mineral exploration by cross-validating inversion results with those of established airborne and ground-based investigation techniques. In addition, supporting petrophysical and geological information to our geophysical measurements allowed the synthesis of all datasets over multiple scales. An initial regional-scale reconnaissance survey was performed with BGR's standard helicopter-borne geophysical system deployed with frequency-domain electromagnetic (HEM), magnetic and radiometric sensors. In addition to geological considerations, the HEM results served as base-line information for the selection of an optimal location for the intermediate-scale semi-airborne EM experiments. The semi-airborne surveys utilized long grounded transmitters and two independent airborne receiver instruments: induction coil magnetometers and SQUID sensors. Due to the limited investigation depth of the HEM method, local-scale electrical resistivity tomography (ERT) and long-offset transient electromagnetic (LOTEM) measurements were carried out on a reference profile, enabling the validation of inversion results at greater depths. The comparison of all inversion results provided a consistent overall resistivity distribution. It further confirmed that both semi-airborne receiver instruments achieve the bandwidth and sensitivity required for the investigation of the resistivity structure down to 1 km depth and therewith the detection of deeply seated earth resources. A 3D geological model, lithological and geophysical borehole logs as well as petrophysical investigations were integrated to interpret of the geophysical results. Distinct highly-conductive anomalies with resistivities of less than 10 Om were identified as alum shales over all scales. Apart from that, the petrophysical investigations exhibited that correlating geophysical and geological information using only one single parameter, such as the electrical resistivity, is hardly possible. Therefore, we developed a first approach based on clustering methods and self-organizing maps (SOMs) that allowed us to assign geological units at the surface to a given combination of geophysical and petrophysical parameters, obtained on different scales. © 2020 The Authors
Merging Top-Down and Bottom-Up Approaches to Fabricate Artificial Photonic Nanomaterials with a Deterministic Electric and Magnetic Response
Artificial photonic nanomaterials made from densely packed scatterers are frequently realized either by top-down or bottom-up techniques. While top-down techniques offer unprecedented control over achievable geometries for the scatterers, by trend they suffer from being limited to planar and periodic structures. In contrast, materials fabricated with bottom-up techniques do not suffer from such disadvantages but, unfortunately, they offer only little control on achievable geometries for the scatterers. To overcome these limitations, a nanofabrication strategy is introduced that merges both approaches. A large number of scatterers are fabricated with a tailored optical response by fast character projection electron-beam lithography and are embedded into a membrane. By peeling-off this membrane from the substrate, scrambling, and densifying it, a bulk material comprising densely packed and randomly arranged scatterers is obtained. The fabrication of an isotropic material from these scatterers with a strong electric and magnetic response is demonstrated. The approach of this study unlocks novel opportunities to fabricate nanomaterials with a complex optical response in the bulk but also on top of arbitrarily shaped surfaces. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim