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Micro-contact impedance spectroscopy (MCIS) is potentially a powerful tool for the exploration of resistive surface layers on top of a conductive bulk or substrate material. MCIS employs micro-contacts in contrast to conventional IS where macroscopic electrodes are used. To extract the conductivity of each region accurately using MCIS requires the data to be corrected for geometry. Using finite element modeling on a system where the resistivity of the surface layer is at least a factor of ten greater than the bulk/substrate, we show how current flows through the two layers using two typical micro-contact configurations. This allows us to establish if and what is the most accurate and reliable method for extracting conductivity values for both regions. For a top circular micro-contact and a full bottom counter electrode, the surface layer conductivity (σs) can be accurately extracted using a spreading resistance equation if the thickness is ~10 times the micro-contact radius; however, bulk conductivity (σb) values can not be accurately determined. If the contact radius is 10 times the thickness of the resistive surface, a geometrical factor using the micro-contact area provides accurate σs values. In this case, a spreading resistance equation also provides a good approximation for σb. For two top circular micro-contacts on thin resistive surface layers, the MCIS response from the surface layer is independent of the contact separation; however, the bulk response is dependent on the contact separation and at small separations contact interference occurs. As a consequence, there is not a single ideal experimental setup that works; to obtain accurate σs and σb values the micro-contact radius, surface layer thickness and the contact separation must all be considered together. Here we provide scenarios where accurate σs and σb values can be obtained that highlight the importance of experimental design and where appropriate equations can be employed for thin and thick resistive surface layers.  相似文献   
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We recently reported the discovery of phenylacetate decarboxylase (PhdB), representing one of only ten glycyl-radical-enzyme reaction types known, and a promising biotechnological tool for first-time biochemical synthesis of toluene from renewable resources. Here, we used experimental and computational data to evaluate the plausibility of three candidate PhdB mechanisms, involving either attack at the phenylacetate methylene carbon or carboxyl group [via H-atom abstraction from COOH or single-electron oxidation of COO (Kolbe-type decarboxylation)]. In vitro experimental data included assays with F-labeled phenylacetate, kinetic studies, and tests with site-directed PhdB mutants; computational data involved estimation of reaction energetics using density functional theory (DFT). The DFT results indicated that all three mechanisms are thermodynamically challenging (beyond the range of many known enzymes in terms of endergonicity or activation energy barrier), reflecting the formidable demands on PhdB for catalysis of this reaction. Evidence that PhdB was able to bind α,α-difluorophenylacetate but was unable to catalyze its decarboxylation supported the enzyme's abstraction of a methylene H atom. Diminished activity of H327A and Y691F mutants was consistent with proposed proton donor roles for His327 and Tyr691. Collectively, these and other data most strongly support PhdB attack at the methylene carbon.  相似文献   
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ABSTRACT

Mode conversion between higher-order modes is attained in a step-index four mode fibre using an in-line polarization controller followed by a force-induced long period fibre grating. By adjusting the field orientation of the LP11 mode to the antisymmetric fibre grating, the LP11 mode is converted to the LP21 mode with a spatially periodic force of 50 N along the fibre length of 50?mm. The mode conversion is evaluated by observing the far-field and near-field patterns of the fibre output and by comparing the transmitted optical power with and without the additional two-mode fibre. The phase-matching grating period is required of the accuracy of roughly ±5?μm and the radiation loss during the mode conversion is as low as 0.01?dB.  相似文献   
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The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However, current vdW magnets are limited by their extreme sensitivity to air, low ordering temperatures, and poor charge transport properties. Here the magnetic and electronic properties of CrSBr are reported, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis. Below its Néel temperature, TN = 132 ± 1 K, CrSBr adopts an A-type antiferromagnetic structure with each individual layer ferromagnetically ordered internally and the layers coupled antiferromagnetically along the stacking direction. Scanning tunneling spectroscopy and photoluminescence (PL) reveal that the electronic gap is ΔE = 1.5 ± 0.2 eV with a corresponding PL peak centered at 1.25 ± 0.07 eV. Using magnetotransport measurements, strong coupling between magnetic order and transport properties in CrSBr is demonstrated, leading to a large negative magnetoresistance response that is unique among vdW materials. These findings establish CrSBr as a promising material platform for increasing the applicability of vdW magnets to the field of spin-based electronics.  相似文献   
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Food fraud is an intentional act for economic gain. It poses a risk to food integrity, the economy, public health and consumers’ ethics. Seafood is one commodity which has endured extensive fraudulent activity owing to its increasing consumer demand, resource limitations, high value and complex supply chains. It is essential that these fraudulent opportunities are revealed, the risk is evaluated and countermeasures for mitigation are assigned. This can be achieved through mapping of the seafood supply chains and identifying the vulnerability analysis critical control points (VACCP), which can be exposed, infiltrated and exploited for fraudulent activity. This research systematically maps the seafood supply chain for three key commodities: finfish, shellfish and crustaceans in the United Kingdom. Each chain is comprised of multiple stakeholders across numerous countries producing a diverse range of products distributed globally. For each supply chain the prospect of fraud, with reference to species substitution, fishery substitution, illegal, unreported and unregulated substitution, species adulteration, chain of custody abuse, catch method fraud, undeclared product extension, modern day slavery and animal welfare, has been identified and evaluated. This mapping of the fraudulent opportunities within the supply chains provides a foundation to rank known and emerging risks and to develop a proactive mitigation plan which assigns control measures and responsibility where vulnerabilities exist. Further intelligence gathering and management of VACCPs of the seafood supply chains may deter currently unknown or unexposed fraudulent opportunities.  相似文献   
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