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- ItemActive Plasmonic Colloid-to-Film-Coupled Cavities for Tailored Light-Matter Interactions(Washington, DC : Soc., 2019) Goßler, Fabian R.; Steiner, Anja Maria; Stroyuk, Oleksandr; Raevskaya, Alexandra; König, Tobias A.F.For large-scale fabrication of optical circuits, tailored subwavelength structures are required to modulate the refractive index. Here, we introduce a colloid-to-film-coupled nanocavity whose refractive index can be tailored by various materials, shapes, and cavity volumes. With this colloidal nanocavity setup, the refractive index can be adjusted over a wide visible wavelength range. For many nanophotonic applications, specific values for the extinction coefficient are crucial to achieve optical loss and gain. We employed bottom-up self-assembly techniques to sandwich optically active ternary metal-chalcogenides between a metallic mirror and plasmonic colloids. The spectral overlap between the cavity resonance and the broadband emitter makes it possible to study the tunable radiative properties statistically. For flat cavity geometries of silver nanocubes with sub-10 nm metallic gap, we found a fluorescence enhancement factor beyond 1000 for 100 cavities and a 112 meV Rabi splitting. In addition, we used gold spheres to extend the refractive index range. By this easily scalable colloidal nanocavity setup, gain and loss building blocks are now available, thereby leading to new generation of optical devices. Copyright © 2019 American Chemical Society.
- ItemTuning the Properties and Self-Healing Behavior of Ionically Modified Poly(isobutylene-co-isoprene) Rubber(Washington, DC : Soc., 2017) Suckow, Marcus; Mordvinkin, Anton; Roy, Manta; Singha, Nikhil K.; Heinrich, Gert; Voit, Brigitte; Saalwächter, Kay; Böhme, FrankThe focus of this work is on the nature of self-healing of ionically modified rubbers obtained by reaction of brominated poly(isobutylene-co-isoprene) rubber (BIIR) with various alkylimidazoles such as 1-methylimidazole, 1-butylimidazole, 1-hexylimidazole, 1-nonylimidazole, and 1-(6-chlorohexyl)-1H-imidazole. Based on stress-strain and temperature dependent DMA measurements, a structural influence of the introduced ionic imidazolium moieties on the formation of ionic clusters and, as a consequence, on the mechanical strength and self-healing behavior of the samples could be evidenced. These results are fully supported by a molecular-level assessment of the network structure (cross-link and constraint density) and the dynamics of the ionic clusters using an advanced proton low-field NMR technique. The results show distinct correlations between the macroscopic behavior and molecular chain dynamics of the modified rubbers. In particular, it is shown that the optimization of material properties with regard to mechanical and self-healing behavior is limited by opposing tendencies. Samples with reduced chain dynamics exhibit superior mechanical behavior but lack on self-healing behavior. In spite of these limitations, the overall performance of some of our samples including self-healing behavior exceeds distinctly that of other self-healing rubbers described in the literature so far.
- ItemRevealing Fast Proton Transport in Condensed Matter by Means of Density Scaling Concept(Washington, DC : Soc., 2020) Wojnarowska, Zaneta; Musiał, Małgorzata; Cheng, Shinian; Gapinski, Jacek; Patkowski, Adam; Pionteck, Jürgen; Paluch, MarianHerein, we investigate the charge transport and structural dynamics in the supercooled and glassy state of protic ionic material with an efficient interionic Grotthuss mechanism. We found that superprotonic properties of studied acebutolol hydrochloride (ACB-HCl) depend on thermodynamic conditions with the most favorable regions being close to the glass-transition temperature (Tg) and glass-transition pressure (Pg). To quantify the contribution of fast proton hopping to overall charge transport over a broad T–P space, we employed the density scaling concept, one of the most important experimental findings in the field of condensed matter physics. We found that isothermal and isobaric dc-conductivity (σdc) and dynamic light scattering (τα) data of ACB-HCl plotted as a function of (TVγ)−1 satisfy the thermodynamic scaling criterion with the ratio γσ/γα appearing as a new measure of fast charge transport in protic ionic glass-formers in the T–P plane. Such a universal factor becomes an alternative to the well-known Walden rule being limited to ambient pressure conditions.
- ItemHierarchical Sticker and Sticky Chain Dynamics in Self-Healing Butyl Rubber Ionomers(Washington, DC : Soc., 2019) Mordvinkin, Anton; Suckow, Marcus; Böhme, Frank; Colby, Ralph H.; Creton, Costantino; Saalwächter, KayWe present a detailed comparison of the microscopic dynamics and the macroscopic mechanical behavior of novel butyl rubber ionomers with tunable dynamics of sparse sticky imidazole-based sidegroups that form clusters of about 20 units separated by essentially unperturbed chains. This material platform shows promise for application as self-healing elastomers. Size and thermal stability of the ionic clusters were probed by small-angle X-ray scattering, and the chain and sticker dynamics were studied by a combination of broadband dielectric spectroscopy (BDS) and advanced NMR methods. The results are correlated with the rheological behavior characterized by dynamic-mechanical analysis (DMA). While the NMR-detected chain relaxation and DMA results agree quantitatively and confirm relevant aspects of the sticky-reptation picture on a microscopic level, we stress and explain that apparent master curves are of limited use for such a comparison. The cluster-related relaxation time detected by BDS is much shorter than the elastic chain relaxation time, although the weak conductivity does follow the latter. The systematic trends across the sample series suggest that all relaxations are dominated by a cluster-related activation barrier, but also that the BDS-based cluster relaxation does not seem to be directly associated with the effective sticker lifetime. Nonlinear stress-strain experiments demonstrate a reduction of sticker lifetime on stretching and that the stored stress and the elastic recovery depend on the deformation rate. © 2019 American Chemical Society.