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- ItemDetection of Protein Glycosylation Using Tip-Enhanced Raman Scattering(Columbus, Ohio : American Chemical Society, 2016) Cowcher, David P.; Deckert-Gaudig, Tanja; Brewster, Victoria L.; Ashton, Lorna; Deckert, Volker; Goodacre, RoystonThe correct glycosylation of biopharmaceutical glycoproteins and their formulations is essential for them to have the desired therapeutic effect on the patient. It has recently been shown that Raman spectroscopy can be used to quantify the proportion of glycosylated protein from mixtures of native and glycosylated forms of bovine pancreatic ribonuclease (RNase). Here we show the first steps toward not only the detection of glycosylation status but the characterization of glycans themselves from just a few protein molecules at a time using tip-enhanced Raman scattering (TERS). While this technique generates complex data that are very dependent on the protein orientation, with the careful development of combined data preprocessing, univariate and multivariate analysis techniques, we have shown that we can distinguish between the native and glycosylated forms of RNase. Many glycoproteins contain populations of subtly different glycoforms; therefore, with stricter orientation control, we believe this has the potential to lead to further glycan characterization using TERS, which would have use in biopharmaceutical synthesis and formulation research.
- ItemOptimized diamond inverted nanocones for enhanced color center to fiber coupling(Melville, NY : American Inst. of Physics, 2021) Torun, Cem Güney; Schneider, Philipp-Immanuel; Hammerschmidt, Martin; Burger, Sven; Munns, Joseph H. D.; Schröder, TimNanostructures can be used for boosting the light outcoupling of color centers in diamond; however, the fiber coupling performance of these nanostructures is rarely investigated. Here, we use a finite element method for computing the emission from color centers in inverted nanocones and the overlap of this emission with the propagation mode in a single-mode fiber. Using different figures of merit, the inverted nanocone parameters are optimized to obtain maximal fiber coupling efficiency, free-space collection efficiency, or rate enhancement. The optimized inverted nanocone designs show promising results with 66% fiber coupling or 83% free-space coupling efficiency at the tin-vacancy center zero-phonon line wavelength of 619 nm. Moreover, when evaluated for broadband performance, the optimized designs show 55% and 76% for fiber coupling and free-space efficiencies, respectively, for collecting the full tin-vacancy emission spectrum at room temperature. An analysis of fabrication insensitivity indicates that these nanostructures are robust against imperfections. For maximum emission rate into a fiber mode, a design with a Purcell factor of 2.34 is identified. Finally, possible improvements offered by a hybrid inverted nanocone, formed by patterning into two different materials, are investigated and increase the achievable fiber coupling efficiency to 71%. © 2021 Author(s).
- ItemPatterning and control of the nanostructure in plasma thin films with acoustic waves: mechanical vs. electrical polarization effects(Cambridge : RSC Publ., 2021) GarcÃa-Valenzuela, Aurelio; Fakhfouri, Armaghan; Oliva-RamÃrez, Manuel; Rico-Gavira, Victor; Rojas, Teresa Cristina; Alvarez, Rafael; Menzel, Siegfried B.; Palmero, Alberto; Winkler, Andreas; González-Elipe, AgustÃn R.Nanostructuration and 2D patterning of thin films are common strategies to fabricate biomimetic surfaces and components for microfluidic, microelectronic or photonic applications. This work presents the fundamentals of a surface nanotechnology procedure for laterally tailoring the nanostructure and crystalline structure of thin films that are plasma deposited onto acoustically excited piezoelectric substrates. Using magnetron sputtering as plasma technique and TiO2 as case example, it is demonstrated that the deposited films depict a sub-millimetre 2D pattern that, characterized by large lateral differences in nanostructure, density (up to 50%), thickness, and physical properties between porous and dense zones, reproduces the wave features distribution of the generated acoustic waves (AW). Simulation modelling of the AW propagation and deposition experiments carried out without plasma and under alternative experimental conditions reveal that patterning is not driven by the collision of ad-species with mechanically excited lattice atoms of the substrate, but emerges from their interaction with plasma sheath ions locally accelerated by the AW-induced electrical polarization field developed at the substrate surface and growing film. The possibilities of the AW activation as a general approach for the tailored control of nanostructure, pattern size, and properties of thin films are demonstrated through the systematic variation of deposition conditions and the adjustment of AW operating parameters.
- ItemCurled cation structures accelerate the dynamics of ionic liquids(Cambridge : RSC Publ., 2021) Rauber, Daniel; Philippi, Frederik; Kuttich, Björn; Becker, Julian; Kraus, Tobias; Hunt, Patricia; Welton, Tom; Hempelmann, Rolf; Kay, Christopher W.M.Ionic liquids are modern liquid materials with potential and actual implementation in many advanced technologies. They combine many favourable and modifiable properties but have a major inherent drawback compared to molecular liquids – slower dynamics. In previous studies we found that the dynamics of ionic liquids are significantly accelerated by the introduction of multiple ether side chains into the cations. However, the origin of the improved transport properties, whether as a result of the altered cation conformation or due to the absence of nanostructuring within the liquid as a result of the higher polarity of the ether chains, remained to be clarified. Therefore, we prepared two novel sets of methylammonium based ionic liquids; one set with three ether substituents and another set with three butyl side chains, in order to compare their dynamic properties and liquid structures. Using a range of anions, we show that the dynamics of the ether-substituted cations are systematically and distinctly accelerated. Liquefaction temperatures are lowered and fragilities increased, while at the same time cation–anion distances are slightly larger for the alkylated samples. Furthermore, pronounced liquid nanostructures were not observed. Molecular dynamics simulations demonstrate that the origin of the altered properties of the ether substituted ionic liquids is primarily due to a curled ether chain conformation, in contrast to the alkylated cations where the alkyl chains retain a linear conformation. Thus, the observed structure–property relations can be explained by changes in the geometric shape of the cations, rather than by the absence of a liquid nanostructure. Application of quantum chemical calculations to a simplified model system revealed that intramolecular hydrogen-bonding is responsible for approximately half of the stabilisation of the curled ether-cations, whereas the other half stems from non-specific long-range interactions. These findings give more detailed insights into the structure–property relations of ionic liquids and will guide the development of ionic liquids that do not suffer from slow dynamics.
- ItemProcess flow to integrate nanostructures on silicon grass in surface micromachined systems(Bristol : IOP Publ., 2016) Mehner, H.; Müller, L.; Biermann, S.; Hänschke, F.; Hoffmann, M.The process flow to integrate metallic nanostructures in surface micromachining processes is presented. The nanostructures are generated by evaporation of microstructured silicon grass with metal. The process flow is based on the lift-off of a thin amorphous silicon layer deposited using a CVD process. All steps feature a low temperature load beneath 120 °C and high compatibility with many materials as only well-established chemicals are used. As a result metallic nanostructures usable for optical applications can be generated as part of multilayered microsystems fabricated in surface micromachining.
- ItemInfluence of Controlled Epoxidation of an Asymmetric Styrene/Butadiene Star Block Copolymer on Structural and Mechanical Properties(Basel : MDPI, 2020) Khatiwada, Shankar P.; Staudinger, Ulrike; Jehnichen, Dieter; Heinrich, Gert; Adhikari, RameshwarThe chemical modification (namely the epoxidation) of a star shaped block copolymer (BCP) based on polystyrene (PS) and polybutadiene (PB) and its effect on structural and mechanical properties of the polymer were investigated. Epoxidation degrees of 37 mol%, 58 mol%, and 82 mol% were achieved by the reaction of the copolymer with meta-chloroperoxy benzoic acid (m-CPBA) under controlled conditions. The BCP structure was found to change from lamellae-like to mixed-type morphologies for intermediate epoxidation level while leading to quite ordered cylindrical structures for the higher level of chemical modification. As a consequence, the glass transition temperature (Tg) of the soft PB component of the BCP shifted towards significantly higher temperature. A clear increase in tensile modulus and tensile strength with a moderate decrease in elongation at break was observed. The epoxidized BCPs are suitable as reactive templates for the fabrication of nanostructured thermosetting resins.
- ItemTowards a life-time-limited 8-octave-infrared photoconductive germanium detector(Bristol : IOP Publ., 2015) Pavlov, S.G.; Deßmann, N.; Pohl, A.; Abrosimov, N.V.; Mittendorff, M.; Winnerl, S.; Zhukavin, R.K; Tsyplenkov, V.V.; Shengurov, D.V.; Shastin, V.N.; Hübers, H.-W.Ultrafast, ultra-broad-band photoconductive detector based on heavily doped and highly compensated germanium has been demonstrated. Such a material demonstrates optical sensitivity in the more than 8 octaves, in the infrared, from about 2 mm to about 8 μm. The spectral sensitivity peaks up between 2 THz and 2.5 THz and is slowly reduced towards lower and higher frequencies. The life times of free electrons/holes measured by a pump-probe technique approach a few tenths of picoseconds and remain almost independent on the optical input intensity and on the temperature of a detector in the operation range. During operation, a detector is cooled down to liquid helium temperature but has been approved to detect, with a reduced sensitivity, up to liquid nitrogen temperature. The response time is shorter than 200 ps that is significantly faster than previously reported times.
- ItemThe new ultra high-speed all-optical coherent streak-camera(Bristol : IOP Publ., 2015) Arkhipov, R.M.; Arkhipov, M.V.; Egorov, V.S.; Chekhonin, I.A.; Chekhonin, M.A.; Bagayev, S.N.In the present paper a new type of ultra high-speed all-optical coherent streak-camera was developed. It was shown that a thin resonant film (quantum dots or molecules) could radiate the angular sequence of delayed ultra-short pulses if a transverse spatial periodic distribution of the laser pump field amplitude has a triangle shape.
- ItemTerahertz emission from lithium doped silicon under continuous wave interband optical excitation(Bristol : IOP Publ., 2015) Andrianov, A.V.; Zakhar'in, A.O.; Zhukavin, R.K.; Shastin, V.N.; Abrosimov, N.V.We report on experimental observation and study of terahertz emission from lithium doped silicon crystals under continuous wave band-to-band optical excitation. It is shown that radiative transitions of electrons from 2P excited states of lithium donor to the 1S(A1) donor ground state prevail in the emission spectrum. The terahertz emission occurs due to capture of nonequilibrium electrons to charged donors, which in turn are generated in the crystal as a result of impurity assisted electron-hole recombination. Besides the intracentre radiative transitions the terahertz emission spectrum exhibits also features at about 12.7 and 15.27 meV, which could be related to intraexciton transitions and transitions from the continuum to the free exciton ground state.
- ItemSTM induced manipulation of azulene-based molecules and nanostructures: the role of the dipole moment(Cambridge : RSC Publ., 2020) Kühne, Tim; Au-Yeung, Kwan Ho; Eisenhut, Frank; Aiboudi, Oumaima; Ryndyk, Dmitry A.; Cuniberti, Gianaurelio; Lissel, Franziska; Moresco, FrancescaAmong the different mechanisms that can be used to drive a molecule on a surface by the tip of a scanning tunneling microscope at low temperature, we used voltage pulses to move azulene-based single molecules and nanostructures on Au(111). Upon evaporation, the molecules partially cleave and form metallo-organic dimers while single molecules are very scarce, as confirmed by simulations. By applying voltage pulses to the different structures under similar conditions, we observe that only one type of dimer can be controllably driven on the surface, which has the lowest dipole moment of all investigated structures. Experiments under different bias and tip height conditions reveal that the electric field is the main driving force of the directed motion. We discuss the different observed structures and their movement properties with respect to their dipole moment and charge distribution on the surface.