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- ItemSpectrometer‐free Optical Hydrogen Sensing Based on Fano‐like Spatial Distribution of Transmission in a Metal−Insulator−Metal Plasmonic Doppler Grating(Weinheim : Wiley-VCH, 2021) Chen, Yi‐Ju; Lin, Fan‐Cheng; Singh, Ankit Kumar; Ouyang, Lei; Huang, Jer‐ShingOptical 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.
- ItemSurface-Enhanced Raman Spectroscopy to Characterize Different Fractions of Extracellular Vesicles from Control and Prostate Cancer Patients(Basel : MDPI, 2021) Osei, Eric Boateng; Paniushkina, Liliia; Wilhelm, Konrad; Popp, Jürgen; Nazarenko, Irina; Krafft, ChristophExtracellular vesicles (EVs) are membrane-enclosed structures ranging in size from about 60 to 800 nm that are released by the cells into the extracellular space; they have attracted interest as easily available biomarkers for cancer diagnostics. In this study, EVs from plasma of control and prostate cancer patients were fractionated by differential centrifugation at 5000× g, 12,000× g and 120,000× g. The remaining supernatants were purified by ultrafiltration to produce EV-depleted free-circulating (fc) fractions. Spontaneous Raman and surface-enhanced Raman spectroscopy (SERS) at 785 nm excitation using silver nanoparticles (AgNPs) were employed as label-free techniques to collect fingerprint spectra and identify the fractions that best discriminate between control and cancer patients. SERS spectra from 10 µL droplets showed an enhanced Raman signature of EV-enriched fractions that were much more intense for cancer patients than controls. The Raman spectra of dehydrated pellets of EV-enriched fractions without AgNPs were dominated by spectral contributions of proteins and showed variations in S-S stretch, tryptophan and protein secondary structure bands between control and cancer fractions. We conclude that the AgNPs-mediated SERS effect strongly enhances Raman bands in EV-enriched fractions, and the fractions, EV12 and EV120 provide the best separation of cancer and control patients by Raman and SERS spectra.
- ItemFiber-based SORS-SERDS system and chemometrics for the diagnostics and therapy monitoring of psoriasis inflammatory disease in vivo(Washington, DC : Optica, 2021-1-28) Schleusener, Johannes; Guo, Shuxia; Darvin, Maxim E.; Thiede, Gisela; Chernavskaia, Olga; Knorr, Florian; Lademann, Jürgen; Popp, Jürgen; Bocklitz, Thomas W.Psoriasis is considered a widespread dermatological disease that can strongly affect the quality of life. Currently, the treatment is continued until the skin surface appears clinically healed. However, lesions appearing normal may contain modifications in deeper layers. To terminate the treatment too early can highly increase the risk of relapses. Therefore, techniques are needed for a better knowledge of the treatment process, especially to detect the lesion modifications in deeper layers. In this study, we developed a fiber-based SORS-SERDS system in combination with machine learning algorithms to non-invasively determine the treatment efficiency of psoriasis. The system was designed to acquire Raman spectra from three different depths into the skin, which provide rich information about the skin modifications in deeper layers. This way, it is expected to prevent the occurrence of relapses in case of a too short treatment. The method was verified with a study of 24 patients upon their two visits: the data is acquired at the beginning of a standard treatment (visit 1) and four months afterwards (visit 2). A mean sensitivity of ≥85% was achieved to distinguish psoriasis from normal skin at visit 1. At visit 2, where the patients were healed according to the clinical appearance, the mean sensitivity was ≈65%.
- ItemAutofluorescence guided welding of heart tissue by laser pulse bursts at 1550 nm(Washington, DC : Optica, 2020) Litvinova, Karina; Chernysheva, Maria; Stegemann, Berthold; Leyva, FranciscoWound healing and other surgical technologies traditionally solved by suturing and stapling have recently been enhanced by the application of laser tissue welding. The usage of high energy laser radiation to anastomose tissues eliminates a foreign body reaction, reduces scar formation, and allows for the creation of watertight closure. In the current work, we show that an ultrafast pulsed fibre laser beam with 183 µJ·cm−2 energy fluence at 1550 nm provides successful welding of dissected chicken heart walls with the tensile strength of 1.03±0.12 kg·cm−2 equal to that of native tissue. The welding process was monitored employing fluorescence spectroscopy that detects the biochemical composition of tissues. We believe that fluorescence spectroscopy guided laser tissue welding is a promising approach for decreasing wound healing times and the avoiding risks of postoperative complications.
- ItemActivity and electron donor preference of two denitrifying bacterial strains identified by Raman gas spectroscopy(Berlin [u.a.] : Springer, 2022) Blohm, Annika; Kumar, Swatantar; Knebl, Andreas; Herrmann, Martina; Küsel, Kirsten; Popp, Jürgen; Frosch, TorstenHuman activities have greatly increased the input of reactive nitrogen species into the environment and disturbed the balance of the global N cycle. This imbalance may be offset by bacterial denitrification, an important process in maintaining the ecological balance of nitrogen. However, our understanding of the activity of mixotrophic denitrifying bacteria is not complete, as most research has focused on heterotrophic denitrification. The aim of this study was to investigate substrate preferences for two mixotrophic denitrifying bacterial strains, Acidovorax delafieldii and Hydrogenophaga taeniospiralis, under heterotrophic, autotrophic or mixotrophic conditions. This complex analysis was achieved by simultaneous identification and quantification of H2, O2, CO2, 14N2, 15N2 and 15N2O in course of the denitrification process with help of cavity-enhanced Raman spectroscopic (CERS) multi-gas analysis. To disentangle electron donor preferences for both bacterial strains, microcosm-based incubation experiments under varying substrate conditions were conducted. We found that Acidovorax delafieldii preferentially performed heterotrophic denitrification in the mixotrophic sub-experiments, while Hydrogenophaga taeniospiralis preferred autotrophic denitrification in the mixotrophic incubation. These observations were supported by stoichiometric calculations. The results demonstrate the prowess of advanced Raman multi-gas analysis to study substrate use and electron donor preferences in denitrification, based on the comprehensive quantification of complex microbial gas exchange processes. © 2021, The Author(s).
- ItemIsolation of bacteria from artificial bronchoalveolar lavage fluid using density gradient centrifugation and their accessibility by Raman spectroscopy(Berlin [u.a.] : Springer, 2021) Wichmann, Christina; Rösch, Petra; Popp, JürgenRaman spectroscopy is an analytical method to identify medical samples of bacteria. Because Raman spectroscopy detects the biochemical properties of a cell, there are many factors that can influence and modify the Raman spectra of bacteria. One possible influence is a proper method for isolation of the bacteria. Medical samples in particular never occur in purified form, so a Raman-compatible isolation method is needed which does not affect the bacteria and thus the resulting spectra. In this study, we present a Raman-compatible method for isolation of bacteria from bronchoalveolar lavage (BAL) fluid using density gradient centrifugation. In addition to measuring the bacteria from a patient sample, the yield and the spectral influence of the isolation on the bacteria were investigated. Bacteria isolated from BAL fluid show additional peaks in comparison to pure culture bacteria, which can be attributed to components in the BAL sample. The isolation gradient itself has no effect on the spectra, and with a yield of 63% and 78%, the method is suitable for isolation of low concentrations of bacteria from a complex matrix. Graphical abstract.
- ItemEmission Manipulation by DNA Origami‐Assisted Plasmonic Nanoantennas(Weinheim : Wiley-VCH, 2021) Yeşilyurt, Ayşe Tuğça Mina; Huang, Jer‐ShingPlasmonic 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
- ItemIt Takes Three to Tango - the length of the oligothiophene determines the nature of the long-lived excited state and the resulting photocytotoxicity of a Ru(II) photodrug(Weinheim : Wiley-VCH, 2021) Chettri, Avinash; Roque, John A.; Schneider, Kilian R.A.; Cole, Houston D.; Cameron, Colin G.; McFarland, Sherri A.; Dietzek, BenjaminTLD1433 is the first Ru(II) complex to be tested as a photodynamic therapy agent in a clinical trial. In this contribution we study TLD1433 in the context of structurally-related Ru(II)-imidozo[4,5-f][1,10]phenanthroline (ip) complexes appended with thiophene rings to decipher the unique photophysical properties which are associated with increasing oligothiophene chain length. Substitution of the ip ligand with ter- or quaterthiophene changes the nature of the long-lived triplet state from metal-to-ligand charge-transfer to 3ππ* character. The addition of the third thiophene thus presents a critical juncture which not only determines the photophysics of the complex but most importantly its capacity for 1O2 generation and hence the potential of the complex to be used as a photocytotoxic agent.
- ItemSediment budgeting of short‐term backfilling processes: The erosional collapse of a Carolingian canal construction(New York, NY [u.a.] : Wiley, 2020) Schmidt, Johannes; Werther, Lukas; Rabiger‐Völlmer, Johannes; Herzig, Franz; Schneider, Birgit; Werban, Ulrike; Dietrich, Peter; Berg, Stefanie; Linzen, Sven; Ettel, Peter; Zielhofer, ChristophSediment budgeting concepts serve as quantification tools to decipher the erosion and accumulation processes within a catchment and help to understand these relocation processes through time. While sediment budgets are widely used in geomorphological catchment-based studies, such quantification approaches are rarely applied in geoarchaeological studies. The case of Charlemagne's summit canal (also known as Fossa Carolina) and its erosional collapse provides an example for which we can use this geomorphological concept and understand the abandonment of the Carolingian construction site. The Fossa Carolina is one of the largest hydro-engineering projects in Medieval Europe. It is situated in Southern Franconia (48.9876°N, 10.9267°E; Bavaria, southern Germany) between the Altmühl and Swabian Rezat rivers. It should have bridged the Central European watershed and connected the Rhine–Main and Danube river systems. According to our dendrochronological analyses and historical sources, the excavation and construction of the Carolingian canal took place in AD 792 and 793. Contemporary written sources describe an intense backfill of excavated sediment in autumn AD 793. This short-term erosion event has been proposed as the principal reason for the collapse and abandonment of the hydro-engineering project. We use subsurface data (drillings, archaeological excavations, and direct-push sensing) and geospatial data (a LiDAR digital terrain model (DTM), a pre-modern DTM, and a 3D model of the Fossa Carolina] for the identification and sediment budgeting of the backfills. Dendrochronological findings and radiocarbon ages of macro remains within the backfills give clear evidence for the erosional collapse of the canal project during or directly after the construction period. Moreover, our quantification approach allows the detection of the major sedimentary collapse zone. The exceedance of the manpower tipping point may have caused the abandonment of the entire construction site. The spatial distribution of the dendrochronological results indicates a north–south direction of the early medieval construction progress.
- ItemUnderstanding Nonlinear Pulse Propagation in Liquid Strand-Based Photonic Bandgap Fibers(Basel : MDPI, 2021) Qi, Xue; Schaarschmidt, Kay; Li, Guangrui; Junaid, Saher; Scheibinger, Ramona; Lühder, Tilman; Schmidt, Markus A.Ultrafast supercontinuum generation crucially depends on the dispersive properties of the underlying waveguide. This strong dependency allows for tailoring nonlinear frequency conversion and is particularly relevant in the context of waveguides that include geometry-induced resonances. Here, we experimentally uncovered the impact of the relative spectral distance between the pump and the bandgap edge on the supercontinuum generation and in particular on the dispersive wave formation on the example of a liquid strand-based photonic bandgap fiber. In contrast to its air-hole-based counterpart, a bandgap fiber shows a dispersion landscape that varies greatly with wavelength. Particularly due to the strong dispersion variation close to the bandgap edges, nanometer adjustments of the pump wavelength result in a dramatic change of the dispersive wave generation (wavelength and threshold). Phase-matching considerations confirm these observations, additionally revealing the relevance of third order dispersion for interband energy transfer. The present study provides additional insights into the nonlinear frequency conversion of resonance-enhanced waveguide systems which will be relevant for both understanding nonlinear processes as well as for tailoring the spectral output of nonlinear fiber sources.