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- ItemFusion of MALDI Spectrometric Imaging and Raman Spectroscopic Data for the Analysis of Biological Samples(Lausanne : Frontiers Media, 2018) Ryabchykov, Oleg; Popp, Jürgen; Bocklitz, Thomas W.Despite of a large number of imaging techniques for the characterization of biological samples, no universal one has been reported yet. In this work, a data fusion approach was investigated for combining Raman spectroscopic data with matrix-assisted laser desorption/ionization (MALDI) mass spectrometric data. It betters the image analysis of biological samples because Raman and MALDI information can be complementary to each other. While MALDI spectrometry yields detailed information regarding the lipid content, Raman spectroscopy provides valuable information about the overall chemical composition of the sample. The combination of Raman spectroscopic and MALDI spectrometric imaging data helps distinguishing different regions within the sample with a higher precision than would be possible by using either technique. We demonstrate that a data weighting step within the data fusion is necessary to reveal additional spectral features. The selected weighting approach was evaluated by examining the proportions of variance within the data explained by the first principal components of a principal component analysis (PCA) and visualizing the PCA results for each data type and combined data. In summary, the presented data fusion approach provides a concrete guideline on how to combine Raman spectroscopic and MALDI spectrometric imaging data for biological analysis.
- ItemSingle molecule level plasmonic catalysis – a dilution study of p-nitrothiophenol on gold dimers(Cambridge : Soc., 2015) Zhang, Zhenglong; Deckert-Gaudig, Tanja; Singh, Pushkar; Deckert, VolkerSurface plasmons on isolated gold dimers can initiate intermolecular reactions of adsorbed p-nitrothiophenol. At the single molecule level when dimerization is not possible an intramolecular reaction can be observed. Experimental evidence indicates that plasmon-induced hot electrons provide the required activation energy.
- ItemFluorosolvatochromism of furanyl- and thiophenyl-substituted acetophenones(London : RSC, 2015) Friebe, Nadine; Schreiter, Katja; Kübel, Joachim; Dietzek, Benjamin; Moszner, Norbert; Burtscher, Peter; Oehlke, Alexander; Spange, StefanA series of para-substituted acetophenones bearing a furanyl or a thiophenyl moiety show a large Stokes-shift, which is a function of various solvent properties. Photophysical properties such as emission lifetime of the compounds have been determined using time-correlated-single photon counting to secure the intrinsic fluorescence behaviour. The solvent dependent position of the UV/Vis emission band [small nu, Greek, tilde]max,em of the compounds has been measured in 26 various solvents. The influence of the solvent on [small nu, Greek, tilde]max,em is of very complex nature and mathematically analysed by multiple square linear solvation energy (LSE)-correlation analysis using Catalán's four-solvent parameter set. Solvent acidity has a strong influence on the bathochromic shift of 2,5-disubstituted furan derivatives compared to the non-5-substituted furan and thiophene derivatives, which show a contrary behaviour. Therefore, the 5-cyanofuranyl-substituted acetophenone derivative is useful as a probe for measuring environmental properties by fluorescence spectroscopy.
- ItemNonresonant Raman spectroscopy of isolated human retina samples complying with laser safety regulations for in vivo measurements(Bellingham, Wash. : SPIE, 2019) Stiebing, Clara; Schie, Iwan W.; Knorr, Florian; Schmitt, Michael; Keijzer, Nanda; Kleemann, Robert; Jahn, Izabella J.; Jahn, Martin; Kiliaan, Amanda J.; Ginner, Laurin; Lichtenegger, Antonia; Drexler, Wolfgang; Leitgeb, Rainer A.; Popp, JürgenRetinal diseases, such as age-related macular degeneration, are leading causes of vision impairment, increasing in incidence worldwide due to an aging society. If diagnosed early, most cases could be prevented. In contrast to standard ophthalmic diagnostic tools, Raman spectroscopy can provide a comprehensive overview of the biochemical composition of the retina in a label-free manner. A proof of concept study of the applicability of nonresonant Raman spectroscopy for retinal investigations is presented. Raman imaging provides valuable insights into the molecular composition of an isolated ex vivo human retina sample by probing the entire molecular fingerprint, i.e., the lipid, protein, carotenoid, and nucleic acid content. The results are compared to morphological information obtained by optical coherence tomography of the sample. The challenges of in vivo Raman studies due to laser safety limitations and predefined optical parameters given by the eye itself are explored. An in-house built setup simulating the optical pathway in the human eye was developed and used to demonstrate that even under laser safety regulations and the above-mentioned optical restrictions, Raman spectra of isolated ex vivo human retinas can be recorded. The results strongly support that in vivo studies using nonresonant Raman spectroscopy are feasible and that these studies provide comprehensive molecular information of the human retina. © The Authors. Published by SPIE.
- ItemMagnetic domain wall gratings for magnetization reversal tuning and confined dynamic mode localization([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Trützschler, Julia; Sentosun, Kadir; Mozooni, Babak; Mattheis, Roland; McCord, JeffreyHigh density magnetic domain wall gratings are imprinted in ferromagnetic-antiferromagnetic thin films by local ion irradiation by which alternating head-to-tail-to-head-to-tail and head-to-head-to-tail-to-tail spatially overlapping domain wall networks are formed. Unique magnetic domain processes result from the interaction of anchored domain walls. Non-linear magnetization response is introduced by the laterally distributed magnetic anisotropy phases. The locally varying magnetic charge distribution gives rise to localized and guided magnetization spin-wave modes directly constrained by the narrow domain wall cores. The exchange coupled multiphase material structure leads to unprecedented static and locally modified dynamic magnetic material properties.
- ItemBenchmark datasets for 3D MALDI- and DESI-imaging mass spectrometry(Oxford : Oxford University Press, 2015) Oetjen, Janina; Veselkov, Kirill; Watrous, Jeramie; McKenzie, James S.; Becker, Michael; Hauberg-Lotte, Lena; Kobarg, Jan Hendrik; Strittmatter, Nicole; Mróz, Anna K.; Hoffmann, Franziska; Trede, Dennis; Palmer, Andrew; Schiffler, Stefan; Steinhorst, Klaus; Aichler, Michaela; Goldin, Robert; Guntinas-Lichius, Orlando; von Eggeling, Ferdinand; Thiele, Herbert; Maedler, Kathrin; Walch, Axel; Maass, Peter; Dorrestein, Pieter C.; Takats, Zoltan; Alexandrov, TheodoreBackground: Three-dimensional (3D) imaging mass spectrometry (MS) is an analytical chemistry technique for the 3D molecular analysis of a tissue specimen, entire organ, or microbial colonies on an agar plate. 3D-imaging MS has unique advantages over existing 3D imaging techniques, offers novel perspectives for understanding the spatial organization of biological processes, and has growing potential to be introduced into routine use in both biology and medicine. Owing to the sheer quantity of data generated, the visualization, analysis, and interpretation of 3D imaging MS data remain a significant challenge. Bioinformatics research in this field is hampered by the lack of publicly available benchmark datasets needed to evaluate and compare algorithms. Findings: High-quality 3D imaging MS datasets from different biological systems at several labs were acquired, supplied with overview images and scripts demonstrating how to read them, and deposited into MetaboLights, an open repository for metabolomics data. 3D imaging MS data were collected from five samples using two types of 3D imaging MS. 3D matrix-assisted laser desorption/ionization imaging (MALDI) MS data were collected from murine pancreas, murine kidney, human oral squamous cell carcinoma, and interacting microbial colonies cultured in Petri dishes. 3D desorption electrospray ionization (DESI) imaging MS data were collected from a human colorectal adenocarcinoma. Conclusions: With the aim to stimulate computational research in the field of computational 3D imaging MS, selected high-quality 3D imaging MS datasets are provided that could be used by algorithm developers as benchmark datasets.
- ItemObservation of Ultrafast Solid-Density Plasma Dynamics Using Femtosecond X-Ray Pulses from a Free-Electron Laser(College Park, Md. : APS, 2018) Kluge, Thomas; Rödel, Melanie; Metzkes-Ng, Josefine; Pelka, Alexander; Laso Garcia, Alejandro; Prencipe, Irene; Rehwald, Martin; Nakatsutsumi, Motoaki; McBride, Emma E.; Schönherr, Tommy; Garten, Marco; Hartley, Nicholas J.; Zacharias, Malte; Grenzer, Jörg; Erbe, Artur; Georgiev, Yordan M.; Galtier, Eric; Nam, Inhyuk; Lee, Hae Ja; Glenzer, Siegfried; Bussmann, Michael; Gutt, Christian; Zeil, Karl; Rödel, Christian; Hübner, Uwe; Schramm, Ulrich; Cowan, Thomas E.The complex physics of the interaction between short-pulse ultrahigh-intensity lasers and solids is so far difficult to access experimentally, and the development of compact laser-based next-generation secondary radiation sources, e.g., for tumor therapy, laboratory astrophysics, and fusion, is hindered by the lack of diagnostic capabilities to probe the complex electron dynamics and competing instabilities. At present, the fundamental plasma dynamics that occur at the nanometer and femtosecond scales during the laser-solid interaction can only be elucidated by simulations. Here we show experimentally that small-angle x-ray scattering of femtosecond x-ray free-electron laser pulses facilitates new capabilities for direct in situ characterization of intense short-pulse laser-plasma interactions at solid density that allows simultaneous nanometer spatial and femtosecond temporal resolution, directly verifying numerical simulations of the electron density dynamics during the short-pulse high-intensity laser irradiation of a solid density target. For laser-driven grating targets, we measure the solid density plasma expansion and observe the generation of a transient grating structure in front of the preinscribed grating, due to plasma expansion. The density maxima are interleaved, forming a double frequency grating in x-ray free-electron laser projection for a short time, which is a hitherto unknown effect. We expect that our results will pave the way for novel time-resolved studies, guiding the development of future laser-driven particle and photon sources from solid targets.
- ItemEnergy-Dependent RBS Channelling Analysis of Epitaxial ZnO Layers Grown on ZnO by RF-Magnetron Sputtering(Basel : MDPI, 2019) Wittkämper, Florian; Bikowski, André; Ellmer, Klaus; Gärtner, Konrad; Wendler, ElkeThe transparent conducting oxides ZnO and ZnO:Al are interesting materials for a wide range of applications. Several of these applications need a large area, single crystalline, and specially doped thin layers. A common technique for the fabrication of those layers is RF (radio frequency) -magnetron sputtering. The investigation of the crystal quality of such layers requires methods of analysis that are destruction free and that are able to obtain information about the concentration and type of defects versus depth. One such option is the Rutherford backscattering spectroscopy (RBS) in channelling mode. In this work, we exploit the channelling effect and its energy dependence, which are sensitive to the type of defects. By using appropriate software and measuring RBS channelling spectra with different beam energies, we were able to determine the depth distribution of point defects and dislocation loops. The presence of dislocation loops was proven using other previously applied analysis methods. The main advantage of RBS in channelling mode is the quantification of point defects, which can be important for defining the electrical and optical properties of such layers. The technique demonstrated is applicable to other defective crystals or thin crystalline layers. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemDifferent storage conditions influence biocompatibility and physicochemical properties of iron oxide nanoparticles(Basel : Molecular Diversity Preservation International (MDPI), 2015) Zaloga, Jan; Janko, Christina; Agarwal, Rohit; Nowak, Johannes; Müller, Robert; Boccaccini, Aldo R.; Lee, Geoffrey; Odenbach, Stefan; Lyer, Stefan; Alexiou, ChristophSuperparamagnetic iron oxide nanoparticles (SPIONs) have attracted increasing attention in many biomedical fields. In magnetic drug targeting SPIONs are injected into a tumour supplying artery and accumulated inside the tumour with a magnet. The effectiveness of this therapy is thus dependent on magnetic properties, stability and biocompatibility of the particles. A good knowledge of the effect of storage conditions on those parameters is of utmost importance for the translation of the therapy concept into the clinic and for reproducibility in preclinical studies. Here, core shell SPIONs with a hybrid coating consisting of lauric acid and albumin were stored at different temperatures from 4 to 45 °C over twelve weeks and periodically tested for their physicochemical properties over time. Surprisingly, even at the highest storage temperature we did not observe denaturation of the protein or colloidal instability. However, the saturation magnetisation decreased by maximally 28.8% with clear correlation to time and storage temperature. Furthermore, the biocompatibility was clearly affected, as cellular uptake of the SPIONs into human T-lymphoma cells was crucially dependent on the storage conditions. Taken together, the results show that the particle properties undergo significant changes over time depending on the way they are stored.
- ItemEvaluating arbitrary strain configurations and doping in graphene with Raman spectroscopy(Bristol : IOP Publ., 2017-11-6) Mueller, Niclas S.; Heeg, Sebastian; Peña Alvarez, Miriam; Kusch, Patryk; Wasserroth, Sören; Clark, Nick; Schedin, Fredrik; Parthenios, John; Papagelis, Konstantinos; Galiotis, Costas; Kalbáč, Martin; Vijayaraghavan, Aravind; Huebner, Uwe; Gorbachev, Roman; Frank, Otakar; Reich, StephanieThe properties of graphene depend sensitively on strain and doping affecting its behavior in devices and allowing an advanced tailoring of this material. A knowledge of the strain configuration, i.e. the relative magnitude of the components of the strain tensor, is particularly crucial, because it governs effects like band-gap opening, pseudo-magnetic fields, and induced superconductivity. It also enters critically in the analysis of the doping level. We propose a method for evaluating unknown strain configurations and simultaneous doping in graphene using Raman spectroscopy. In our analysis we first extract the bare peak shift of the G and 2D modes by eliminating their splitting due to shear strain. The shifts from hydrostatic strain and doping are separated by a correlation analysis of the 2D and G frequencies, where we find Delta omega(2D)/Delta omega(G) = 2.21 +/- 0.05 for pure hydrostatic strain. We obtain the local hydrostatic strain, shear strain and doping without any assumption on the strain configuration prior to the analysis, as we demonstrate for two model cases: Graphene under uniaxial stress and graphene suspended on nanostructures that induce strain. Raman scattering with circular corotating polarization is ideal for analyzing frequency shifts, especially for weak strain when the peak splitting by shear strain cannot be resolved.