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- 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.
- 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.
- 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.
- ItemMicro- and nano-scale engineering and structures shape architecture at nucleation from In-As-Sb-P composition liquid phase on an InAs(100) surface(Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2020) Gambaryan, Karen M.; Marquardt, Oliver; Boeck, Torsten; Trampert, AchimIn this review paper we present results of the growth, characterization and electronic properties of In(As,Sb,P) composition strain-induced micro- and nanostructures. Nucleation is performed from In-As-Sb-P quaternary composition liquid phase in Stranski--Krastanow growth mode using steady-state liquid phase epitaxy. Growth features and the shape transformation of pyramidal islands, lens-shape and ellipsoidal type-II quantum dots (QDs), quantum rings and QD-molecules are under consideration. It is shown that the application of a quaternary In(As,Sb,P) composition wetting layer allows not only more flexible control of lattice-mismatch between the wetting layer and an InAs(100) substrate, but also opens up new possibilities for nanoscale engineering and nanoarchitecture of several types of nanostructures. HR-SEM, AFM, TEM and STM are used for nanostructure characterization. Optoelectronic properties of the grown structures are investigated by FTIR and photoresponse spectra measurements. Using an eight-band $mathbfkcdotmathbfp$ model taking strain and built-in electrostatic potentials into account, the electronic properties of a wide range of InAs$_1-x-y$Sb$_x$P$_y$ QDs and QD-molecules are computed. Two types of QDs mid-infrared photodetectors are fabricated and investigated. It is shown that the incorporation of QDs allows to improve some output device characteristics, in particularly sensitivity, and to broaden the spectral range.
- ItemMorphology and Microstructure Evolution of Gold Nanostructures in the Limited Volume Porous Matrices(Basel : MDPI, 2020) Yakimchuk, Dzmitry V.; Bundyukova, Victoria D.; Ustarroz, Jon; Terryn, Herman; Baert, Kitty; Kozlovskiy, Artem L.; Zdorovets, Maxim V.; Khubezhov, Soslan A.; Trukhanov, Alex V.; Trukhanov, Sergei V.; Panina, Larissa V.; Arzumanyan, Grigory M.; Mamatkulov, Kahramon Z.; Tishkevich, Daria I.; Kaniukov, Egor Y.; Sivakov, VladimirThe modern development of nanotechnology requires the discovery of simple approaches that ensure the controlled formation of functional nanostructures with a predetermined morphology. One of the simplest approaches is the self-assembly of nanostructures. The widespread implementation of self-assembly is limited by the complexity of controlled processes in a large volume where, due to the temperature, ion concentration, and other thermodynamics factors, local changes in diffusion-limited processes may occur, leading to unexpected nanostructure growth. The easiest ways to control the diffusion-limited processes are spatial limitation and localized growth of nanostructures in a porous matrix. In this paper, we propose to apply the method of controlled self-assembly of gold nanostructures in a limited pore volume of a silicon oxide matrix with submicron pore sizes. A detailed study of achieved gold nanostructures' morphology, microstructure, and surface composition at different formation stages is carried out to understand the peculiarities of realized nanostructures. Based on the obtained results, a mechanism for the growth of gold nanostructures in a limited volume, which can be used for the controlled formation of nanostructures with a predetermined geometry and composition, has been proposed. The results observed in the present study can be useful for the design of plasmonic-active surfaces for surface-enhanced Raman spectroscopy-based detection of ultra-low concentration of different chemical or biological analytes, where the size of the localized gold nanostructures is comparable with the spot area of the focused laser beam.
- 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.
- 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).