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- ItemMacroscopic Self-Evolution of Dynamic Hydrogels to Create Hollow Interiors(Weinheim : Wiley-VCH Verlag, 2020) Han, L.; Zheng, Y.; Luo, H.; Feng, J.; Engstler, R.; Xue, L.; Jing, G.; Deng, X.; del Campo, A.; Cui, J.A solid-to-hollow evolution in macroscopic structures is challenging in synthetic materials. A fundamentally new strategy is reported for guiding macroscopic, unidirectional shape evolution of materials without compromising the material's integrity. This strategy is based on the creation of a field with a “swelling pole” and a “shrinking pole” to drive polymers to disassemble, migrate, and resettle in the targeted region. This concept is demonstrated using dynamic hydrogels containing anchored acrylic ligands and hydrophobic long alkyl chains. Adding water molecules and ferric ions (Fe3+) to induce a swelling–shrinking field transforms the hydrogels from solid to hollow. The strategy is versatile in the generation of various closed hollow objects (for example, spheres, helix tubes, and cubes with different diameters) for different applications.
- ItemSqualenyl Hydrogen Sulfate Nanoparticles for Simultaneous Delivery of Tobramycin and an Alkylquinolone Quorum Sensing Inhibitor Enable the Eradication of P. aeruginosa Biofilm Infections(Weinheim : Wiley-VCH Verlag, 2020) Ho, D.-K.; Murgia, X.; De Rossi, C.; Christmann, R.; Hüfner de Mello Martins, A.G.; Koch, M.; Andreas, A.; Herrmann, J.; Müller, R.; Empting, M.; Hartmann, R.W.; Desmaele, D.; Loretz, B.; Couvreur, P.; Lehr, C.-M.Elimination of pulmonary Pseudomonas aeruginosa (PA) infections is challenging to accomplish with antibiotic therapies, mainly due to resistance mechanisms. Quorum sensing inhibitors (QSIs) interfering with biofilm formation can thus complement antibiotics. For simultaneous and improved delivery of both active agents to the infection sites, self-assembling nanoparticles of a newly synthesized squalenyl hydrogen sulfate (SqNPs) were prepared. These nanocarriers allowed for remarkably high loading capacities of hydrophilic antibiotic tobramycin (Tob) and a novel lipophilic QSI at 30 % and circa 10 %, respectively. The drug-loaded SqNPs showed improved biofilm penetration and enhanced efficacy in relevant biological barriers (mucin/human tracheal mucus, biofilm), leading to complete eradication of PA biofilms at circa 16-fold lower Tob concentration than Tob alone. This study offers a viable therapy optimization and invigorates the research and development of QSIs for clinical use.
- ItemWaveguide-Integrated Broadband Spectrometer Based on Tailored Disorder(Weinheim : Wiley-VCH Verlag, 2020) Hartmann, Wladick; Varytis, Paris; Gehring, Helge; Walter, Nicolai; Beutel, Fabian; Busch, Kurt; Pernice, WolframCompact, on-chip spectrometers exploiting tailored disorder for broadband light scattering enable high-resolution signal analysis while maintaining a small device footprint. Due to multiple scattering events of light in the disordered medium, the effective path length of the device is significantly enhanced. Here, on-chip spectrometers are realized for visible and near-infrared wavelengths by combining an efficient broadband fiber-to-chip coupling approach with a scattering area in a broadband transparent silicon nitride waveguiding structure. Air holes etched into a structured silicon nitride slab terminated with multiple waveguides enable multipath light scattering in a diffusive regime. Spectral-to-spatial mapping is performed by determining the transmission matrix at the waveguide outputs, which is then used to reconstruct the probe signals. Direct comparison with theoretical analyses shows that such devices can be used for high-resolution spectroscopy from the visible up to the telecom wavelength regime. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemBenchmark of Simplified Time-Dependent Density Functional Theory for UV–Vis Spectral Properties of Porphyrinoids(Weinheim : Wiley-VCH Verlag, 2019) Batra, Kamal; Zahn, Stefan; Heine, ThomasTime-dependent density functional theory is thoroughly benchmarked for the predictive calculation of UV–vis spectra of porphyrin derivatives. With the aim to provide an approach that is computationally feasible for large-scale applications such as biological systems or molecular framework materials, albeit performing with high accuracy for the Q-bands, the results given by various computational protocols, including basis sets, density-functionals (including gradient corrected local functionals, hybrids, double hybrids and range-separated functionals), and various variants of time-dependent density functional theory, including the simplified Tamm–Dancoff approximation, are compared. An excellent choice for these calculations is the range-separated functional CAM-B3LYP in combination with the simplified Tamm–Dancoff approximation and a basis set of double-ζ quality def2-SVP (mean absolute error [MAE] of ≈0.05 eV). This is not surpassed by more expensive approaches, not even by double hybrid functionals, and solely systematic excitation energy scaling slightly improves the results (MAE ≈0.04 eV).
- ItemQuinoidal Azaacenes: 99 % Diradical Character(Weinheim : Wiley-VCH Verlag, 2020) Intorp, S.N.; Hodecker, M.; Müller, M.; Tverskoy, O.; Rosenkranz, M.; Dmitrieva, E.; Popov, A.A.; Rominger, F.; Freudenberg, J.; Dreuw, A.; Bunz, U.H.F.Quinoidal azaacenes with almost pure diradical character (y=0.95 to y=0.99) were synthesized. All compounds exhibit paramagnetic behavior investigated by EPR and NMR spectroscopy, and SQUID measurements, revealing thermally populated triplet states with an extremely low-energy gap ΔEST′ of 0.58 to 1.0 kcal mol−1. The species are persistent in solution (half-life≈14–21 h) and in the solid state they are stable for weeks.
- ItemMagnetic Micromotors for Multiple Motile Sperm Cells Capture, Transport, and Enzymatic Release(Weinheim : Wiley-VCH Verlag, 2020) Xu, H.; Medina-Sánchez, M.; Schmidt, O.G.An integrated system combining a magnetically-driven micromotor and a synthetized protein-based hyaluronic acid (HA) microflake is presented for the in situ selection and transport of multiple motile sperm cells (ca. 50). The system appeals for targeted sperm delivery in the reproductive system to assist fertilization or to deliver drugs. The binding mechanism between the HA microflake and sperm relies on the interactions between HA and the corresponding sperm HA receptors. Once sperm are captured within the HA microflake, the assembly is trapped and transported by a magnetically-driven helical microcarrier. The trapping of the sperm-microflake occurs by a local vortex induced by the microcarrier during rotation-translation under a rotating magnetic field. After transport, the microflake is enzymatically hydrolyzed by local proteases, allowing sperm to escape and finally reach the target location. This cargo-delivery system represents a new concept to transport not only multiple motile sperm but also other actively moving biological cargoes.
- ItemModulating Myeloid Immune Cell Migration Using Multivalently Presented Monosaccharide Ligands for Advanced Immunotherapy(Weinheim : Wiley-VCH Verlag, 2019) Taverno, I.; Rodrigo, A.M.; Kandziora, M.; Kuntz, S.; Dernedde, J.; Trautwein, C.; Tacke, F.; Blas-Garcia, A.; Bartneck, M.Due to their importance for the outcome of the inflammatory response, the motile myeloid cells are a focus of novel treatment options. The interplay of selectins and their ligands with leukocytes and endothelial cells, which mediate endothelial attachment and transmigration of immune cells, can be modulated by selectin‐binding structures. Here, a library of selectin‐targeting ligands coupled to either gold, silver, iron oxide nanospheres, or quantum dots of 5–10 nm in size is used to systematically study their impact on immune cell motility. The multivalent presentation of the carbohydrate mimetics results in very low sub‐nanomolar binding to L ‐selectin. Using human primary monocytes, granulocytes, lymphocytes, and macrophages, it is shown that the ligands exhibit only minor effects on uptake, whereas the motility of leukocytes is critically affected as observed in migration assays evaluated by flow cytometry. The carbohydrate mimetic ring structure, sulfation, in particular, and the degree of ligand presentation, are constituents which cohere in this process. Specific carbohydrate ligands can thus selectively regulate leukocyte subsets. These data form the basis for advanced immunotherapy which inhibits the amplification of inflammation by restricting leukocyte influx to injured tissue sites. Furthermore, the targeting ligands may complement existing treatment options for inflammatory diseases.
- ItemHigh-Resolution Inkjet Printing of Quantum Dot Light-Emitting Microdiode Arrays(Weinheim : Wiley-VCH Verlag, 2020) Yang, P.; Zhang, L.; Kang, D.J.; Strahl, R.; Kraus, T.The direct printing of microscale quantum dot light-emitting diodes (QLEDs) is a cost-effective alternative to the placement of pre-formed LEDs. The quality of printed QLEDs currently is limited by nonuniformities in droplet formation, wetting, and drying during inkjet printing. Here, optimal ink formulation which can suppress nonuniformities at the pixel and array levels is demonstrated. A solvent mixture is used to tune the ejected droplet size, ensure wetting, and provoke Marangoni flows that prevent coffee stain rings. Arrays of green QLED devices are printed at a resolution of 500 pixels in.−1 with a maximum luminance of ≈3000 cd m−2 and a peak current efficiency of 2.8 cd A−1. The resulting array quality is sufficient to print displays at state-of-the-art resolutions.
- ItemStress-Induced 3D Chiral Fractal Metasurface for Enhanced and Stabilized Broadband Near-Field Optical Chirality(Weinheim : Wiley-VCH Verlag, 2019) Tseng M.L.; Lin Z.-H.; Kuo H.Y.; Huang T.-T.; Huang Y.-T.; Chung T.L.; Chu C.H.; Huang J.-S.; Tsai D.P.Metasurfaces comprising 3D chiral structures have shown great potential in chiroptical applications such as chiral optical components and sensing. So far, the main challenges lie in the nanofabrication and the limited operational bandwidth. Homogeneous and localized broadband near-field optical chirality enhancement has not been achieved. Here, an effective nanofabrication method to create a 3D chiral metasurface with far- and near-field broadband chiroptical properties is demonstrated. A focused ion beam is used to cut and stretch nanowires into 3D Archimedean spirals from stacked films. The 3D Archimedean spiral is a self-similar chiral fractal structure sensitive to the chirality of light. The spiral exhibits far- and near-field broadband chiroptical responses from 2 to 8 µm. With circularly polarized light (CPL), the spiral shows superior far-field transmission dissymmetry and handedness-dependent near-field localization. With linearly polarized excitation, homogeneous and highly enhanced broadband near-field optical chirality is generated at a stably localized position inside the spiral. The effective yet straightforward fabrication strategy allows easy fabrication of 3D chiral structures with superior broadband far-field chiroptical response as well as strongly enhanced and stably localized broadband near-field optical chirality. The reported method and chiral metasurface may find applications in broadband chiral optics and chiral sensing. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemLiquid-Phase Electron Microscopy for Soft Matter Science and Biology(Weinheim : Wiley-VCH Verlag, 2020) Wu, H.; Friedrich, H.; Patterson, J.P.; Sommerdijk, N.A.J.M.; de Jonge, N.Innovations in liquid-phase electron microscopy (LP-EM) have made it possible to perform experiments at the optimized conditions needed to examine soft matter. The main obstacle is conducting experiments in such a way that electron beam radiation can be used to obtain answers for scientific questions without changing the structure and (bio)chemical processes in the sample due to the influence of the radiation. By overcoming these experimental difficulties at least partially, LP-EM has evolved into a new microscopy method with nanometer spatial resolution and sub-second temporal resolution for analysis of soft matter in materials science and biology. Both experimental design and applications of LP-EM for soft matter materials science and biological research are reviewed, and a perspective of possible future directions is given.
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