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- ItemCharge‐Compensated N‐Doped π ‐Conjugated Polymers: Toward both Thermodynamic Stability of N‐Doped States in Water and High Electron Conductivity(Weinheim : Wiley-VCH, 2022) Borrmann, Fabian; Tsuda, Takuya; Guskova, Olga; Kiriy, Nataliya; Hoffmann, Cedric; Neusser, David; Ludwigs, Sabine; Lappan, Uwe; Simon, Frank; Geisler, Martin; Debnath, Bipasha; Krupskaya, Yulia; Al‐Hussein, Mahmoud; Kiriy, AntonThe understanding and applications of electron-conducting π-conjugated polymers with naphtalene diimide (NDI) blocks show remarkable progress in recent years. Such polymers demonstrate a facilitated n-doping due to the strong electron deficiency of the main polymer chain and the presence of the positively charged side groups stabilizing a negative charge of the n-doped backbone. Here, the n-type conducting NDI polymer with enhanced stability of its n-doped states for prospective “in-water” applications is developed. A combined experimental–theoretical approach is used to identify critical features and parameters that control the doping and electron transport process. The facilitated polymer reduction ability and the thermodynamic stability in water are confirmed by electrochemical measurements and doping studies. This material also demonstrates a high conductivity of 10−2 S cm−1 under ambient conditions and 10−1 S cm−1 in vacuum. The modeling explains the stabilizing effects for various dopants. The simulations show a significant doping-induced “collapse” of the positively charged side chains on the core bearing a partial negative charge. This explains a decrease in the lamellar spacing observed in experiments. This study fundamentally enables a novel pathway for achieving both thermodynamic stability of the n-doped states in water and the high electron conductivity of polymers.
- ItemIs there more than one stickiness criterion?(Berlin ; Heidelberg : Springer, 2022) Wang, Anle; Müser, Martin H.Adhesion between an elastic body and a smooth, rigid substrate can lead to large tensile stresses between them. However, most macroscopic objects are microscopically rough, which strongly suppresses adhesion. A fierce debate has unfolded recently as to whether local or global parameters determine the crossover between small and large adhesion. Here, we report simulations revealing that the dependence of the pull-off force Fn on the surface energy γ does not only have two regimes of high and low adhesion but up to four regimes. They are related to contacts, which at the moment of rupture consist of (i) the last individual Hertzian-shaped contact, in which is linear in γ, (ii) a last meso-scale, individual patches with super-linear scaling, (iii) many isolated contact patches with extremely strong scaling, and (iv) a dominating largest contact patch, for which the pull-off stress is no longer negligible compared to the maximum, microscopic pull-off stress. Regime (iii) can be seen as a transition domain. It is located near the point where the surface energy is half the elastic energy per unit area in conformal contact. A criterion for the transition between regimes (i) and (ii) appears difficult to grasp. [Figure not available: see fulltext.].
- ItemInfluence of structural depth of laser-patterned steel surfaces on the solid lubricity of carbon nanoparticle coatings(Berlin ; Heidelberg : Springer, 2022) Maclucas, Timothy; Daut, Lukas; Grützmacher, Philipp; Guitar, Maria Agustina; Presser, Volker; Gachot, Carsten; Suarez, Sebastian; Mücklich, FrankCarbon nanoparticle coatings on laser-patterned stainless-steel surfaces present a solid lubrication system where the pattern’s recessions act as lubricant-retaining reservoirs. This study investigates the influence of the structural depth of line patterns coated with multi-walled carbon nanotubes (CNTs) and carbon onions (COs) on their respective potential to reduce friction and wear. Direct laser interference patterning (DLIP) with a pulse duration of 12 ps is used to create line patterns with three different structural depths at a periodicity of 3.5 µm on AISI 304 steel platelets. Subsequently, electrophoretic deposition (EPD) is applied to form homogeneous carbon nanoparticle coatings on the patterned platelets. Tribological ball-on-disc experiments are conducted on the as-described surfaces with an alumina counter body at a load of 100 mN. The results show that the shallower the coated structure, the lower its coefficient of friction (COF), regardless of the particle type. Thereby, with a minimum of just below 0.20, CNTs reach lower COF values than COs over most of the testing period. The resulting wear tracks are characterized by scanning electron microscopy, transmission electron microscopy, and energy-dispersive X-ray spectroscopy. During friction testing, the CNTs remain in contact, and the immediate proximity, whereas the CO coating is largely removed. Regardless of structural depth, no oxidation occurs on CNT-coated surfaces, whereas minor oxidation is detected on CO-coated wear tracks. [Figure not available: see fulltext.].
- ItemData-Driven Discovery of Stochastic Differential Equations(Beijing : Engineering Sciences Press, 2022) Wang, Yasen; Fang, Huazhen; Jin, Junyang; Ma, Guijun; He, Xin; Dai, Xing; Yue, Zuogong; Cheng, Cheng; Zhang, Hai-Tao; Pu, Donglin; Wu, Dongrui; Yuan, Ye; Gonçalves, Jorge; Kurths, Jürgen; Ding, HanStochastic differential equations (SDEs) are mathematical models that are widely used to describe complex processes or phenomena perturbed by random noise from different sources. The identification of SDEs governing a system is often a challenge because of the inherent strong stochasticity of data and the complexity of the system's dynamics. The practical utility of existing parametric approaches for identifying SDEs is usually limited by insufficient data resources. This study presents a novel framework for identifying SDEs by leveraging the sparse Bayesian learning (SBL) technique to search for a parsimonious, yet physically necessary representation from the space of candidate basis functions. More importantly, we use the analytical tractability of SBL to develop an efficient way to formulate the linear regression problem for the discovery of SDEs that requires considerably less time-series data. The effectiveness of the proposed framework is demonstrated using real data on stock and oil prices, bearing variation, and wind speed, as well as simulated data on well-known stochastic dynamical systems, including the generalized Wiener process and Langevin equation. This framework aims to assist specialists in extracting stochastic mathematical models from random phenomena in the natural sciences, economics, and engineering fields for analysis, prediction, and decision making.
- ItemOptical photothermal infrared spectroscopy with simultaneously acquired Raman spectroscopy for two-dimensional microplastic identification([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Böke, Julia Sophie; Popp, Jürgen; Krafft, ChristophIn recent years, vibrational spectroscopic techniques based on Fourier transform infrared (FTIR) or Raman microspectroscopy have been suggested to fulfill the unmet need for microplastic particle detection and identification. Inter-system comparison of spectra from reference polymers enables assessing the reproducibility between instruments and advantages of emerging quantum cascade laser-based optical photothermal infrared (O-PTIR) spectroscopy. In our work, IR and Raman spectra of nine plastics, namely polyethylene, polypropylene, polyvinyl chloride, polyethylene terephthalate, polycarbonate, polystyrene, silicone, polylactide acid and polymethylmethacrylate were simultaneously acquired using an O-PTIR microscope in non-contact, reflection mode. Comprehensive band assignments were presented. We determined the agreement of O-PTIR with standalone attenuated total reflection FTIR and Raman spectrometers based on the hit quality index (HQI) and introduced a two-dimensional identification (2D-HQI) approach using both Raman- and IR-HQIs. Finally, microplastic particles were prepared as test samples from known materials by wet grinding, O-PTIR data were collected and subjected to the 2D-HQI identification approach. We concluded that this framework offers improved material identification of microplastic particles in environmental, nutritious and biological matrices.
- ItemTopological transitions in ac/dc-driven superconductor nanotubes([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Fomin, Vladimir M.; Rezaev, Roman O.; Dobrovolskiy, Oleksandr V.Extending of nanostructures into the third dimension has become a major research avenue in condensed-matter physics, because of geometry- and topology-induced phenomena. In this regard, superconductor 3D nanoarchitectures feature magnetic field inhomogeneity, non-trivial topology of Meissner currents and complex dynamics of topological defects. Here, we investigate theoretically topological transitions in the dynamics of vortices and slips of the phase of the order parameter in open superconductor nanotubes under a modulated transport current. Relying upon the time-dependent Ginzburg–Landau equation, we reveal two distinct voltage regimes when (i) a dominant part of the tube is in either the normal or superconducting state and (ii) a complex interplay between vortices, phase-slip regions and screening currents determines a rich FFT voltage spectrum. Our findings unveil novel dynamical states in superconductor open nanotubes, such as paraxial and azimuthal phase-slip regions, their branching and coexistence with vortices, and allow for control of these states by superimposed dc and ac current stimuli.
- ItemLabel-free multimodal imaging of infected Galleria mellonella larvae([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Quansah, Elsie; Ramoji, Anuradha; Thieme, Lara; Mirza, Kamran; Goering, Bianca; Makarewicz, Oliwia; Heutelbeck, Astrid; Meyer-Zedler, Tobias; Pletz, Mathias W.; Schmitt, Michael; Popp, JürgenNon-linear imaging modalities have enabled us to obtain unique morpho-chemical insights into the tissue architecture of various biological model organisms in a label-free manner. However, these imaging techniques have so far not been applied to analyze the Galleria mellonella infection model. This study utilizes for the first time the strength of multimodal imaging techniques to explore infection-related changes in the Galleria mellonella larvae due to massive E. faecalis bacterial infection. Multimodal imaging techniques such as fluorescent lifetime imaging (FLIM), coherent anti-Stokes Raman scattering (CARS), two-photon excited fluorescence (TPEF), and second harmonic generation (SHG) were implemented in conjunction with histological HE images to analyze infection-associated tissue damage. The changes in the larvae in response to the infection, such as melanization, vacuolization, nodule formation, and hemocyte infiltration as a defense mechanism of insects against microbial pathogens, were visualized after Enterococcus faecalis was administered. Furthermore, multimodal imaging served for the analysis of implant-associated biofilm infections by visualizing biofilm adherence on medical stainless steel and ePTFE implants within the larvae. Our results suggest that infection-related changes as well as the integrity of the tissue of G. mellonella larvae can be studied with high morphological and chemical contrast in a label-free manner.
- ItemPlatelet Membrane-Coated Nanocarriers Targeting Plaques to Deliver Anti-CD47 Antibody for Atherosclerotic Therapy([Beijing] : China Association for Science and Technology, 2022) Chen, Liang; Zhou, Zhongyi; Hu, Cheng; Maitz, Manfred F.; Yang, Li; Luo, Rifang; Wang, YunbingAtherosclerosis, the principle cause of cardiovascular disease (CVD) worldwide, is mainly characterized by the pathological accumulation of diseased vascular cells and apoptotic cellular debris. Atherogenesis is associated with the upregulation of CD47, a key antiphagocytic molecule that is known to render malignant cells resistant to programmed cell removal, or "efferocytosis." Here, we have developed platelet membrane-coated mesoporous silicon nanoparticles (PMSN) as a drug delivery system to target atherosclerotic plaques with the delivery of an anti-CD47 antibody. Briefly, the cell membrane coat prolonged the circulation of the particles by evading the immune recognition and provided an affinity to plaques and atherosclerotic sites. The anti-CD47 antibody then normalized the clearance of diseased vascular tissue and further ameliorated atherosclerosis by blocking CD47. In an atherosclerosis model established in ApoE-/- mice, PMSN encapsulating anti-CD47 antibody delivery significantly promoted the efferocytosis of necrotic cells in plaques. Clearing the necrotic cells greatly reduced the atherosclerotic plaque area and stabilized the plaques reducing the risk of plaque rupture and advanced thrombosis. Overall, this study demonstrated the therapeutic advantages of PMSN encapsulating anti-CD47 antibodies for atherosclerosis therapy, which holds considerable promise as a new targeted drug delivery platform for efficient therapy of atherosclerosis.
- ItemAdhesive and Self-Healing Polyurethanes with Tunable Multifunctionality([Beijing] : China Association for Science and Technology, 2022) Zhou, Lei; Zhang, Lu; Li, Peichuang; Maitz, Manfred F.; Wang, Kebing; Shang, Tengda; Dai, Sheng; Fu, Yudie; Zhao, Yuancong; Yang, Zhilu; Wang, Jin; Li, XinMany polyurethanes (PUs) are blood-contacting materials due to their good mechanical properties, fatigue resistance, cytocompatibility, biosafety, and relatively good hemocompatibility. Further functionalization of the PUs using chemical synthetic methods is especially attractive for expanding their applications. Herein, a series of catechol functionalized PU (CPU-PTMEG) elastomers containing variable molecular weight of polytetramethylene ether glycol (PTMEG) soft segment are reported by stepwise polymerization and further introduction of catechol. Tailoring the molecular weight of PTMEG fragment enables a regulable catechol content, mobility of the chain segment, hydrogen bond and microphase separation of the C-PU-PTMEG elastomers, thus offering tunability of mechanical strength (such as breaking strength from 1.3 MPa to 5.7 MPa), adhesion, self-healing efficiency (from 14.9% to 96.7% within 2 hours), anticoagulant, antioxidation, anti-inflammatory properties and cellular growth behavior. As cardiovascular stent coatings, the C-PU-PTMEGs demonstrate enough flexibility to withstand deformation during the balloon dilation procedure. Of special importance is that the C-PU-PTMEG-coated surfaces show the ability to rapidly scavenge free radicals to maintain normal growth of endothelial cells, inhibit smooth muscle cell proliferation, mediate inflammatory response, and reduce thrombus formation. With the universality of surface adhesion and tunable multifunctionality, these novel C-PU-PTMEG elastomers should find potential usage in artificial heart valves and surface engineering of stents.
- ItemOn Curie temperature of B20-MnSi films([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Li, Zichao; Yuan, Ye; Begeza, Viktor; Rebohle, Lars; Helm, Manfred; Nielsch, Kornelius; Prucnal, Slawomir; Zhou, ShengqiangB20-type MnSi is the prototype magnetic skyrmion material. Thin films of MnSi show a higher Curie temperature than their bulk counterpart. However, it is not yet clear what mechanism leads to the increase of the Curie temperature. In this work, we grow MnSi films on Si(100) and Si(111) substrates with a broad variation in their structures. By controlling the Mn thickness and annealing parameters, the pure MnSi phase of polycrystalline and textured nature as well as the mixed phase of MnSi and MnSi1.7 are obtained. Surprisingly, all these MnSi films show an increased Curie temperature of up to around 43 K. The Curie temperature is likely independent of the structural parameters within our accessibility including the film thickness above a threshold, strain, cell volume and the mixture with MnSi1.7. However, a pronounced phonon softening is observed for all samples, which can tentatively be attributed to slight Mn excess from stoichiometry, leading to the increased Curie temperature.