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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.
- 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.
- 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.
- ItemIn-vivo Raman spectroscopy: from basics to applications(Bellingham, Wash. : SPIE, 2018) Cordero, Eliana; Latka, Ines; Matthäus, Christian; Schie, Iwan W.; Popp, JürgenFor more than two decades, Raman spectroscopy has found widespread use in biological and medical applications. The instrumentation and the statistical evaluation procedures have matured, enabling the lengthy transition from ex-vivo demonstration to in-vivo examinations. This transition goes hand-in-hand with many technological developments and tightly bound requirements for a successful implementation in a clinical environment, which are often difficult to assess for novice scientists in the field. This review outlines the required instrumentation and instrumentation parameters, designs, and developments of fiber optic probes for the in-vivo applications in a clinical setting. It aims at providing an overview of contemporary technology and clinical trials and attempts to identify future developments necessary to bring the emerging technology to the clinical end users. A comprehensive overview of in-vivo applications of fiber optic Raman probes to characterize different tissue and disease types is also given.
- ItemLooking for a perfect match: multimodal combinations of Raman spectroscopy for biomedical applications(Bellingham, Wash. : SPIE, 2021) Schie, Iwan; Stiebing, Clara; Popp, JürgenRaman spectroscopy has shown very promising results in medical diagnostics by providing label-free and highly specific molecular information of pathological tissue ex vivo and in vivo. Nevertheless, the high specificity of Raman spectroscopy comes at a price, i.e., low acquisition rate, no direct access to depth information, and limited sampling areas. However, a similar case regarding advantages and disadvantages can also be made for other highly regarded optical modalities, such as optical coherence tomography, autofluorescence imaging and fluorescence spectroscopy, fluorescence lifetime microscopy, second-harmonic generation, and others. While in these modalities the acquisition speed is significantly higher, they have no or only limited molecular specificity and are only sensitive to a small group of molecules. It can be safely stated that a single modality provides only a limited view on a specific aspect of a biological specimen and cannot assess the entire complexity of a sample. To solve this issue, multimodal optical systems, which combine different optical modalities tailored to a particular need, become more and more common in translational research and will be indispensable diagnostic tools in clinical pathology in the near future. These systems can assess different and partially complementary aspects of a sample and provide a distinct set of independent biomarkers. Here, we want to give an overview on the development of multimodal systems that use RS in combination with other optical modalities to improve the diagnostic performance.
- ItemCompact, Watt-class 785 nm dual-wavelength master oscillator power amplifiers(Bristol ; Philadelphia, PA : IOP Publishing Ltd., 2022) Müller, André; Maiwald, Martin; Sumpf, Bernd785 nm micro-integrated, dual-wavelength master oscillator power amplifiers with a footprint of 5 mm × 25 mm are presented. They are based on Y-branch distributed Bragg reflector ridge waveguide diode lasers and anti-reflection coated tapered amplifiers. In order to reduce the impact of potential optical feedback, devices with master oscillator front facet reflectivities of 5% and 30% as well as with an integrated miniaturized optical isolator have been realized. A comparison up to 1 W shows narrowband dual wavelength laser emission with a spectral distance of 0.6 nm (10 cm−1) and individual spectral widths <20 pm. As expected, a higher front facet reflectivity leads to a significant reduction of feedback related mode hops. Longitudinal modes corresponding to the master oscillator resonator length remain within spectral windows <0.15 nm (3 cm−1), suitable for applications such as Raman spectroscopy and especially shifted excitation Raman difference spectroscopy. Integrating a compact 30 dB optical isolator completely eliminates the observed optical feedback effects. Lateral beam propagation ratios of 1.2 (1/e2) enable easy beam shaping and fiber coupling. Outside of the experimental comparison, the developed MOPAs provide up to 2.7 W of optical output power available for applications.
- ItemRaman spectroscopy in layered hybrid organic-inorganic metal halide perovskites(Bristol : IOP Publishing, 2022) Spirito, Davide; Asensio, Yaiza; Hueso, Luis E.; Martín-García, BeatrizThe continuous progress in the synthesis and characterization of materials in the vast family of hybrid organic-inorganic metal halide perovskites (HOIPs) has been pushed by their exceptional properties mainly in optoelectronic applications. These works highlight the peculiar role of lattice vibrations, which strongly interact with electrons, resulting in coupled states affecting the optical properties. Among these materials, layered (2D) HOIPs have emerged as a promising material platform to address some issues of their three-dimensional counterparts, such as ambient stability and ion migration. Layered HOIPs consist of inorganic layers made of metal halide octahedra separated by layers composed of organic cations. They have attracted much interest not only for applications, but also for their rich phenomenology due to their crystal structure tunability. Here, we give an overview of the main experimental findings achieved via Raman spectroscopy in several configurations and set-ups, and how they contribute to shedding light on the complex structural nature of these fascinating materials. We focus on how the phonon spectrum comes from the interplay of several factors. First, the inorganic and organic parts, whose motions are coupled, contribute with their typical modes which are very different in energy. Nonetheless, the interaction between them is relevant, as it results in low-symmetry crystal structures. Then, the role of external stimuli, such as temperature and pressure, which induce phase transitions affecting the spectrum through change in symmetry of the lattice, octahedral tilting and arrangement of the molecules. Finally, the relevant role of the coupling between the charge carriers and optical phonons is highlighted.
- ItemCompact diode laser based light source with alternating dual-wavelength emission at 532 nm(Berlin ; Heidelberg : Springer, 2020) Müller, André; Sumpf, BerndCompact nonlinear frequency conversion of a Y-branch distributed Bragg reflector (DBR) diode laser for alternating dual-wavelength laser emission at 532 nm is presented for the very first time. The developed light source, realized on a 5 × 25 mm2 micro-optical bench, is based on single-pass second harmonic generation of a 1064 nm Y-branch DBR diode laser in a periodically poled lithium niobate waveguide crystal with superimposed poling periods. Phase-matching is obtained by intrinsic wavelength stabilization of the laser and wavelength tuning by implemented heater elements above the DBR gratings. Obtained optical output powers of 5.6 mW at 532.45 nm and 6.7 mW at 531.85 nm are limited by central lobe power contents of 52% available for waveguide coupling. With a spectral performance showing narrowband emission with spectral widths of 0.01 nm (0.4 cm−1) limited by the spectral resolution of the spectrum analyzer and a spectral spacing of 0.6 nm (20 cm−1), the developed light source is suitable for applications such as Raman spectroscopy and shifted excitation Raman difference spectroscopy (SERDS). Separate electrical contacts of the Y-branch diode laser enable alternating operation at both wavelengths.
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