2019, Pahlow, Susanne, Lehniger, Lydia, Hentschel, Stefanie, Seise, Barbara, Braun, Sascha D., Ehricht, Ralf, Berg, Albrecht, Popp, Jürgen, Weber, Karina

With this study, an innovative and convenient enrichment and detection strategy for eight clinically relevant pneumonia pathogens, namely, Acinetobacter baumannii, Escherichia coli, Haemophilus influenzae, Klebsiella pneumoniae, Moraxella catarrhalis, Pseudomonas aeruginosa, Staphylococcus aureus, and Streptococcus pneumoniae is introduced. Bacteria were isolated from sputum samples with amine-modified particles exploiting pH-dependent electrostatic interactions between bacteria and the functionalized particle surface. Following this, an asymmetric polymerase chain reaction as well as subsequent stringent array-based hybridization with specific complementary capture probes were performed. Finally, results were visualized by an enzyme-induced silver nanoparticle deposition, providing stable endpoint signals and consequently an easy detection possibility. The assay was optimized using spiked samples of artificial sputum with different strains of the abovementioned bacterial species. Furthermore, actual patient sputum samples with S. pneumoniae were successfully analyzed. The presented approach offers great potential for the urgent need of a fast, specific, and reliable isolation and identification platform for important pneumonia pathogens, covering the complete process chain from sample preparation up to array-based detection within only 4 h.With this study, an innovative and convenient enrichment and detection strategy for eight clinically relevant pneumonia pathogens, namely, Acinetobacter baumannii, Escherichia coli, Haemophilus influenzae, Klebsiella pneumoniae, Moraxella catarrhalis, Pseudomonas aeruginosa, Staphylococcus aureus, and Streptococcus pneumoniae is introduced. Bacteria were isolated from sputum samples with amine-modified particles exploiting pH-dependent electrostatic interactions between bacteria and the functionalized particle surface. Following this, an asymmetric polymerase chain reaction as well as subsequent stringent array-based hybridization with specific complementary capture probes were performed. Finally, results were visualized by an enzyme-induced silver nanoparticle deposition, providing stable endpoint signals and consequently an easy detection possibility. The assay was optimized using spiked samples of artificial sputum with different strains of the abovementioned bacterial species. Furthermore, actual patient sputum samples with S. pneumoniae were successfully analyzed. The presented approach offers great potential for the urgent need of a fast, specific, and reliable isolation and identification platform for important pneumonia pathogens, covering the complete process chain from sample preparation up to array-based detection within only 4 h.

2018, Herrmann, Janning F., Höppener, Christiane

Plasmonic nanoantennas have found broad applications in the fields of photovoltaics, electroluminescence, non-linear optics and for plasmon enhanced spectroscopy and microscopy. Of particular interest are fundamental limitations beyond the dipolar approximation limit. We introduce asymmetric gold nanoparticle antennas (AuNPs) with improved optical near-field properties based on the formation of sub-nanometer size gaps, which are suitable for studying matter with high-resolution and single molecule sensitivity. These dumbbell antennas are characterized in regard to their far-field and near-field properties and are compared to similar dimer and trimer antennas with larger gap sizes. The tailoring of the gap size down to sub-nanometer length scales is based on the integration of rigid macrocyclic cucurbituril molecules. Stable dimer antennas are formed with an improved ratio of the electromagnetic field enhancement and confinement. This ratio, taken as a measure of the performance of an antenna, can even exceed that exhibited by trimer AuNP antennas composed of comparable building blocks with larger gap sizes. Fluctuations in the far-field and near-field properties are observed, which are likely caused by distinct deviations of the gap geometry arising from the faceted structure of the applied colloidal AuNPs.

2018, Raie, Diana S., Mhatre, Eisha, El-Desouki, Doaa S., Labena, Ahmed, El-Ghannam, Gamal, Farahat, Laila, Youssef, Tareq, Fritzsche, Wolfgang, Kovács, Ákos

The present work was targeted to design a surface against cell seeding and adhering of bacteria, Bacillus subtilis. A multi-walled carbon nanotube/titanium dioxide nano-power was produced via simple mixing of carbon nanotube and titanium dioxide nanoparticles during the sol-gel process followed by heat treatment. Successfully, quercetin was immobilized on the nanocomposite via physical adsorption to form a quercetin/multi-walled carbon nanotube/titanium dioxide nanocomposite. The adhesion of bacteria on the coated-slides was verified after 24 h using confocal laser-scanning microscopy. Results indicated that the quercetin/multi-walled carbon nanotube/titanium dioxide nanocomposite had more negativity and higher recovery by glass surfaces than its counterpart. Moreover, coating surfaces with the quercetin-modified nanocomposite lowered both hydrophilicity and surface-attached bacteria compared to surfaces coated with the multi-walled carbon nanotubes/titanium dioxide nanocomposite.

2019, Zedler, Linda, Krieck, Sven, Kupfer, Stephan, Dietzek, Benjamin

Electron transfer reactions play a key role for artificial solar energy conversion, however, the underlying reaction mechanisms and the interplay with the molecular structure are still poorly understood due to the complexity of the reaction pathways and ultrafast timescales. In order to investigate such light-induced reaction pathways, a new spectroscopic tool has been applied, which combines UV-vis and resonance Raman spectroscopy at multiple excitation wavelengths with electrochemistry in a thin-layer electrochemical cell to study [RuII(tbtpy)2]2+ (tbtpy = tri-tert-butyl-2,2′:6′,2′′-terpyridine) as a model compound for the photo-activated electron donor in structurally related molecular and supramolecular assemblies. The new spectroscopic method substantiates previous suggestions regarding the reduction mechanism of this complex by localizing photo-electrons and identifying structural changes of metastable intermediates along the reaction cascade. This has been realized by monitoring selective enhancement of Raman-active vibrations associated with structural changes upon electronic absorption when tuning the excitation wavelength into new UV-vis absorption bands of intermediate structures. Additional interpretation of shifts in Raman band positions upon reduction with the help of quantum chemical calculations provides a consistent picture of the sequential reduction of the individual terpyridine ligands, i.e., the first reduction results in the monocation [(tbtpy)Ru(tbtpy•)]+, while the second reduction generates [(tbtpy•)Ru(tbtpy•)]0 of triplet multiplicity. Therefore, the combination of this versatile spectro-electrochemical tool allows us to deepen the fundamental understanding of light-induced charge transfer processes in more relevant and complex systems.

2019, Tseng M.L., Lin Z.-H., Kuo H.Y., Huang T.-T., Huang Y.-T., Chung T.L., Chu C.H., Huang J.-S., Tsai D.P.

Metasurfaces comprising 3D chiral structures have shown great potential in chiroptical applications such as chiral optical components and sensing. So far, the main challenges lie in the nanofabrication and the limited operational bandwidth. Homogeneous and localized broadband near-field optical chirality enhancement has not been achieved. Here, an effective nanofabrication method to create a 3D chiral metasurface with far- and near-field broadband chiroptical properties is demonstrated. A focused ion beam is used to cut and stretch nanowires into 3D Archimedean spirals from stacked films. The 3D Archimedean spiral is a self-similar chiral fractal structure sensitive to the chirality of light. The spiral exhibits far- and near-field broadband chiroptical responses from 2 to 8 µm. With circularly polarized light (CPL), the spiral shows superior far-field transmission dissymmetry and handedness-dependent near-field localization. With linearly polarized excitation, homogeneous and highly enhanced broadband near-field optical chirality is generated at a stably localized position inside the spiral. The effective yet straightforward fabrication strategy allows easy fabrication of 3D chiral structures with superior broadband far-field chiroptical response as well as strongly enhanced and stably localized broadband near-field optical chirality. The reported method and chiral metasurface may find applications in broadband chiral optics and chiral sensing. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

2018, Lühder, Tilman, Wieduwilt, Torsten, Schneidewind, Henrik, Schmidt, Markus A.

Here we introduce the concept of electrically tuning surface plasmon polaritons using current-driven heat dissipation, allowing controlling plasmonic properties via a straightforward-to-access quantity. The key idea is based on an electrical current flowing through the plasmonic layer, changing plasmon dispersion and phase-matching condition via a temperature-imposed modification of the refractive index of one of the dielectric media involved. This scheme was experimentally demonstrated on the example of an electrically connected plasmonic fiber taper that has sensitivities >50000 nm/RIU. By applying a current, dissipative heat generated inside metal film heats the surrounding liquid, reducing its refractive index correspondingly and thus modifying the phase-matching condition to the fundamental taper mode. We observed spectral shifts of the plasmonic resonance up to 300 nm towards shorter wavelength by an electrical power of ≤ 80 mW, clearly showing that our concept is important for applications that demand precise real-time and external control on plasmonic dispersion and resonance wavelengths.

2018, Patze, Sophie, Hübner, Uwe, Weber, Karina, Cialla-May, Dana, Popp, Jürgen

Surface-enhanced Raman spectroscopy (SERS) is known as a molecular-specific and highly sensitive method. In order to enable the routine application of SERS, powerful SERS substrates are of great importance. Within this manuscript, a TopUp SERS substrate is introduced which is fabricated by a top-down process based on microstructuring as well as a bottom-up generation of silver nanostructures. The Raman signal of the support material acts as an internal standard in order to improve the quantification capabilities. The analyte molecule coverage of sulfamethoxazole on the surface of the nanostructures is characterized by the SERS signal evolution fitted by a Langmuir–Freundlich isotherm.

2021, Chen, Yi‐Ju, Lin, Fan‐Cheng, Singh, Ankit Kumar, Ouyang, Lei, Huang, Jer‐Shing

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.

2021, Yeşilyurt, Ayşe Tuğça Mina, Huang, Jer‐Shing

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

2020, Kielpinski, Mark, Walther, Oliver, Cao, Jialan, Henkel, Thomas, Köhler, J. Michael, Groß, G. Alexander

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.