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- ItemDistinction of nucleobases - A tip-enhanced Raman approach(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2011) Treffer, R.; Lin, X.; Bailo, E.; Deckert-Gaudig, T.; Deckert, V.The development of novel DNA sequencing methods is one of the ongoing challenges in various fields of research seeking to address the demand for sequence information. However, many of these techniques rely on some kind of labeling or amplification steps. Here we investigate the intrinsic properties of tip-enhanced Raman scattering (TERS) towards the development of a novel, label-free, direct sequencing method. It is known that TERS allows the acquisition of spectral information with high lateral resolution and single-molecule sensitivity. In the presented experiments, single stranded adenine and uracil homopolymers were immobilized on different kinds of substrates (mica and gold nanoplates) and TERS experiments were conducted, which demonstrated the reproducibility of the technique. To elucidate the signal contributions from the specific nucleobases, TERS spectra were collected on single stranded calf thymus DNA with arbitrary sequence. The results show that, while the Raman signals with respect to the four nucleobases differ remarkably, specific markers can be determined for each respective base. The combination of sensitivity and reproducibility shows that the crucial demands for a sequencing procedure are met.
- ItemTowards multiple readout application of plasmonic arrays(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2011) Cialla, D.; Weber, K.; Böhme, R.; Hübner, U.; Schneidewind, H.; Zeisberger, M.; Mattheis, R.; Möller, R.; Popp, J.In order to combine the advantages of fluorescence and surface-enhanced Raman spectroscopy (SERS) on the same chip platform, a nanostructured gold surface with a unique design, allowing both the sensitive detection of fluorescence light together with the specific Raman fingerprint of the fluorescent molecules, was established. This task requires the fabrication of plasmonic arrays that permit the binding of molecules of interest at different distances from the metallic surface. The most efficient SERS enhancement is achieved for molecules directly adsorbed on the metallic surface due to the strong field enhancement, but where, however, the fluorescence is quenched most efficiently. Furthermore, the fluorescence can be enhanced efficiently by careful adjustment of the optical behavior of the plasmonic arrays. In this article, the simultaneous application of SERS and fluorescence, through the use of various gold nanostructured arrays, is demonstrated by the realization of a DNA detection scheme. The results shown open the way to more flexible use of plasmonic arrays in bioanalytics.
- ItemTechnical Note: One year of Raman-lidar measurements in Gual Pahari EUCAARI site close to New Delhi in India – Seasonal characteristics of the aerosol vertical structure(München : European Geopyhsical Union, 2012) Komppula, M.; Mielonen, T.; Arola, A.; Korhonen, K.; Lihavainen, H.; Hyvärinen, A.-P.; Baars, H.; Engelmann, R.; Althausen, D.; Ansmann, A.; Müller, D.; Panwar, T.S.; Hooda, R.K.; Sharma, V.P.; Kerminen, V.-M.; Lehtinen, K.E.J.; Viisanen, Y.One year of multi-wavelength (3 backscatter + 2 extinction + 1 depolarization) Raman lidar measurements at Gual Pahari, close to New Delhi, were analysed. The data was split into four seasons: spring (March–May), summer (June–August), autumn (September–November) and winter (December–February). The vertical profiles of backscatter, extinction, and lidar ratio and their variability during each season are presented. The measurements revealed that, on average, the aerosol layer was at its highest in spring (5.5 km). In summer, the vertically averaged (between 1–3 km) backscatter and extinction coefficients had the highest averages (3.3 Mm−1 sr−1 and 142 Mm−1 at 532 nm, respectively). Aerosol concentrations were slightly higher in summer compared to other seasons, and particles were larger in size. The autumn showed the highest lidar ratio and high extinction-related Ångström exponents (AEext), indicating the presence of smaller probably absorbing particles. The winter had the lowest backscatter and extinction coefficients, but AEext was the highest, suggesting still a large amount of small particles.
- ItemCeilometer lidar comparison: Backscatter coefficient retrieval and signal-to-noise ratio determination(München : European Geopyhsical Union, 2010) Heese, B.; Flentje, H.; Althausen, D.; Ansmann, A.; Frey, S.The potential of a new generation of ceilometer instruments for aerosol monitoring has been studied in the Ceilometer Lidar Comparison (CLIC) study. The used ceilometer was developed by Jenoptik, Germany, and is designed to find both thin cirrus clouds at tropopause level and aerosol layers at close ranges during day and night-time. The comparison study was performed to determine up to which altitude the ceilometers are capable to deliver particle backscatter coefficient profiles. For this, the derived ceilometer profiles are compared to simultaneously measured lidar profiles at the same wavelength. The lidar used for the comparison was the multi-wavelengths Raman lidar PollyXT. To demonstrate the capabilities and limits of ceilometers for the derivation of particle backscatter coefficient profiles from their measurements two examples of the comparison results are shown. Two cases, a daytime case with high background noise and a less noisy night-time case, are chosen. In both cases the ceilometer profiles compare well with the lidar profiles in atmospheric structures like aerosol layers or the boundary layer top height. However, the determination of the correct magnitude of the particle backscatter coefficient needs a calibration of the ceilometer data with an independent measurement of the aerosol optical depth by a sun photometer. To characterizes the ceilometers signal performance with increasing altitude a comprehensive signal-to-noise ratio study was performed. During daytime the signal-to-noise ratio is higher than 1 up to 4–5 km depending on the aerosol content. In our night-time case the SNR is higher than 1 even up to 8.5 km, so that also aerosol layers in the upper troposphere had been detected by the ceilometer.
- ItemCoincident measurements of PMSE and NLC above ALOMAR (69° N, 16° E) by radar and lidar from 1999-2008(Göttingen : Copernicus, 2011) Kaifler, N.; Baumgarten, G.; Fiedler, J.; Latteck, R.; Lübken, F.-J.; Rapp, M.Polar Mesosphere Summer Echoes (PMSE) and Noctilucent Clouds (NLC) have been routinely measured at the ALOMAR research facility in Northern Norway (69° N, 16° E) by lidar and radar, respectively. 2900 h of lidar measurements by the ALOMAR Rayleigh/Mie/Raman lidar were combined with almost 18 000 h of radar measurements by the ALWIN VHF radar, all taken during the years 1999 to 2008, to study simultaneous and common-volume observations of both phenomena. PMSE and NLC are known from both theory and observations to be positively linked. We quantify the occurrences of PMSE and/or NLC and relations in altitude, especially with respect to the lower layer boundaries. The PMSE occurrence rate is with 75.3% considerably higher than the NLC occurrence rate of 19.5%. For overlapping PMSE and NLC observations, we confirm the coincidence of the lower boundaries and find a standard deviation of 1.26 km, hinting at very fast sublimation rates. However, 10.1% of all NLC measurements occur without accompanying PMSE. Comparison of occurrence rates with solar zenith angle reveals that NLC without PMSE mostly occur around midnight indicating that the ice particles were not detected by the radar due to the reduced electron density.
- ItemQuantification of waves in lidar observations of noctilucent clouds at scales from seconds to minutes(Göttingen : Copernicus, 2013) Kaifler, N.; Baumgarten, G.; Fiedler, J.We present small-scale structures and waves observed in noctilucent clouds (NLC) by lidar at an unprecedented temporal resolution of 30 s or less. The measurements were taken with the Rayleigh/Mie/Raman lidar at the ALOMAR observatory in northern Norway (69 N) in the years 2008-2011. We find multiple layer NLC in 7.9% of the time for a brightness threshold of δ β 12 × 10-10 m-1 sr-1. In comparison to 10 min averaged data, the 30 s dataset shows considerably more structure. For limited periods, quasi-monochromatic waves in NLC altitude variations are common, in accord with ground-based NLC imagery. For the combined dataset, on the other hand, we do not find preferred periods but rather significant periods at all timescales observed (1 min to 1 h). Typical wave amplitudes in the layer vertical displacements are 0.2 km with maximum amplitudes up to 2.3 km. Average spectral slopes of temporal altitude and brightness variations are-2.01 ± 0.25 for centroid altitude,-1.41 ± 0.24 for peak brightness and-1.73 ± 0.25 for integrated brightness. Evaluating a new single-pulse detection system, we observe altitude variations of 70 s period and spectral slopes down to a scale of 10 s. We evaluate the suitability of NLC parameters as tracers for gravity waves.
- ItemA novel engineered oxide buffer approach for fully lattice-matched SOI heterostructures(College Park, MD : Institute of Physics Publishing, 2010) Giussani, A.; Zaumseil, P.; Seifarth, O.; Storck, P.; Schroeder, T.Epitaxial (epi) oxides on silicon can be used to integrate novel device concepts on the canonical Si platform, including functional oxides, e.g. multiferroics, as well as alternative semiconductor approaches. For all these applications, the quality of the oxide heterostructure is a key figure of merit. In this paper, it is shown that, by co-evaporating Y2O3 and Pr2O3 powder materials, perfectly lattice-matched PrYO3(111) epilayers with bixbyite structure can be grown on Si(111) substrates. A high-resolution x-ray diffraction analysis demonstrates that the mixed oxide epi-films are single crystalline and type B oriented. Si epitaxial overgrowth of the PrYO3(111)/Si(111) support system results in flat, continuous and fully lattice-matched epi-Si(111)/PrYO3(111)/Si(111) silicon-on-insulator heterostructures. Raman spectroscopy proves the strain-free nature of the epi-Si films. A Williamson-Hall analysis of the mixed oxide layer highlights the existence of structural defects in the buffer, which can be explained by the thermal expansion coefficients of Si and PrYO3. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.
- ItemNanostructured silver substrates with stable and universal sers properties: Application to organic molecules and semiconductor nanoparticles(New York, NY [u.a.] : Springer, 2010) Chursanova, M.V.; Dzhagan, V.M.; Yukhymchuk, V.O.; Lytvyn, O.S.; Valakh, M.Y.; Khodasevich, I.A.; Lehmann, D.; Zahn, D.R.T.; Waurisch, C.; Hickey, S.G.Nanostructured silver films have been prepared by thermal deposition on silicon, and their properties as SERS substrates investigated. The optimal conditions of the post-growth annealing of the substrates were established. Atomic force microscopy study revealed that the silver films with relatively dense and homogeneous arrays of 60-80-nm high pyramidal nanoislands are the most efficient for SERS of both organic dye and inorganic nanoparticles analytes. The noticeable enhancement of the Raman signal from colloidal nanoparticles with the help of silver island films is reported for the first time. © 2009 The Author(s).
- ItemTemperature-dependent Raman investigation of rolled up InGaAs/GaAs microtubes(New York, NY [u.a.] : Springer, 2012) Rodriguez, R.D.; Sheremet, E.; Thurmer, D.J.; Lehmann, D.; Gordan, O.D.; Seidel, F.; Milekhin, A.; Schmidt, O.G.; Hietschold, M.; Zahn, D.R.T.Large arrays of multifunctional rolled-up semiconductors can be mass-produced with precisely controlled size and composition, making them of great technological interest for micro- and nano-scale device fabrication. The microtube behavior at different temperatures is a key factor towards further engineering their functionality, as well as for characterizing strain, defects, and temperature-dependent properties of the structures. For this purpose, we probe optical phonons of GaAs/InGaAs rolled-up microtubes using Raman spectroscopy on defect-rich (faulty) and defect-free microtubes. The microtubes are fabricated by selectively etching an AlAs sacrificial layer in order to release the strained InGaAs/GaAs bilayer, all grown by molecular beam epitaxy. Pristine microtubes show homogeneity of the GaAs and InGaAs peak positions and intensities along the tube, which indicates a defect-free rolling up process, while for a cone-like microtube, a downward shift of the GaAs LO phonon peak along the cone is observed. Formation of other type of defects, including partially unfolded microtubes, can also be related to a high Raman intensity of the TO phonon in GaAs. We argue that the appearance of the TO phonon mode is a consequence of further relaxation of the selection rules due to the defects on the tubes, which makes this phonon useful for failure detection/prediction in such rolled up systems. In order to systematically characterize the temperature stability of the rolled up microtubes, Raman spectra were acquired as a function of sample temperature up to 300°C. The reversibility of the changes in the Raman spectra of the tubes within this temperature range is demonstrated.
- ItemHydrogen bonding in ionic liquids probed by linear and nonlinear vibrational spectroscopy(Bristol : IOP, 2012) Roth, C.; Chatzipapadopoulos, S.; Kerlé, D.; Friedriszik, F.; Lütgens, M.; Lochbrunner, S.; Kühn, O.; Ludwig, R.Three imidazolium-based ionic liquids of the type [Cnmim] [NTf2] with different alkyl chain lengths (n = 1, 2 and 8) at the first position of the imidazolium ring were studied applying infrared, linear Raman and multiplex coherent anti-Stokes Raman scattering spectroscopy. The focus has been on the CH-stretching region of the imidazolium ring, which is supposed to carry information about a possible hydrogen bonding network in the ionic liquid. The measurements are compared with calculations of the corresponding anharmonic vibrational spectra for a cluster of [C 2mim][NTf2] consisting of four ion pairs. The results support the hypothesis of weak hydrogen bonding involving the C(4)-H and C(5)-H groups and somewhat stronger hydrogen bonds of the C(2)-H groups.