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- ItemOptimizing the Geometry of Photoacoustically Active Gold Nanoparticles for Biomedical Imaging(Washington, DC : ACS, 2020) García-Álvarez, Rafaela; Chen, Lisa; Nedilko, Alexander; Sánchez-Iglesias, Ana; Rix, Anne; Lederle, Wiltrud; Pathak, Vertika; Lammers, Twan; von Plessen, Gero; Kostarelos, Kostas; Liz-Marzán, Luis M.; Kuehne, Alexander J.C.; Chigrin, Dmitry N.Photoacoustics is an upcoming modality for biomedical imaging, which promises minimal invasiveness at high penetration depths of several centimeters. For superior photoacoustic contrast, imaging probes with high photothermal conversion efficiency are required. Gold nanoparticles are among the best performing photoacoustic imaging probes. However, the geometry and size of the nanoparticles determine their photothermal efficiency. We present a systematic theoretical analysis to determine the optimum nanoparticle geometry with respect to photoacoustic efficiency in the near-infrared spectral range, for superior photoacoustic contrast. Theoretical predictions are illustrated by experimental results for two of the most promising nanoparticle geometries, namely, high aspect ratio gold nanorods and gold nanostars. Copyright © 2020 American Chemical Society.
- ItemHierarchical fibrous guiding cues at different scales influence linear neurite extension([Amsterdam] : Elsevier, 2020) Omidinia-Anarkoli, Abdolrahman; Ephraim, John Wesley; Rimal, Rahul; De Laporte, LauraSurface topographies at micro- and nanoscales can influence different cellular behavior, such as their growth rate and directionality. While different techniques have been established to fabricate 2-dimensional flat substrates with nano- and microscale topographies, most of them are prone to high costs and long preparation times. The 2.5-dimensional fiber platform presented here provides knowledge on the effect of the combination of fiber alignment, inter-fiber distance (IFD), and fiber surface topography on contact guidance to direct neurite behavior from dorsal root ganglia (DRGs) or dissociated primary neurons. For the first time, the interplay of the micro-/nanoscale topography and IFD is studied to induce linear nerve growth, while controlling branching. The results demonstrate that grooved fibers promote a higher percentage of aligned neurite extension, compensating the adverse effect of increased IFD. Accordingly, maximum neurite extension from primary neurons is achieved on grooved fibers separated by an IFD of 30 μm, with a higher percentage of aligned neurons on grooved fibers at a large IFD compared to porous fibers with the smallest IFD of 10 µm. We further demonstrate that the neurite “decision-making” behavior on whether to cross a fiber or grow along it is not only dependent on the IFD but also on the fiber surface topography. In addition, axons growing in between the fibers seem to have a memory after leaving grooved fibers, resulting in higher linear growth and higher IFDs lead to more branching. Such information is of great importance for new material development for several tissue engineering applications. Statement of Significance: One of the key aspects of tissue engineering is controlling cell behavior using hierarchical structures. Compared to 2D surfaces, fibers are an important class of materials, which can emulate the native ECM architecture of tissues. Despite the importance of both fiber surface topography and alignment to direct growing neurons, the current state of the art did not yet study the synergy between both scales of guidance. To achieve this, we established a solvent assisted spinning process to combine these two crucial features and control neuron growth, alignment, and branching. Rational design of new platforms for various tissue engineering and drug discovery applications can benefit from such information as it allows for fabrication of functional materials, which selectively influence neurite behavior. © 2020
- ItemNarrow Stimulated Resonance Raman Scattering and WGM Lasing in Small Conjugated Polymer Particles for Live Cell Tagging and Tracking(Weinheim : Wiley-VCH, 2020) Haehnle, Bastian; Lamla, Markus; Sparrer, Konstantin M.J.; Gather, Malte C.; Kuehne, Alexander J.C.Conjugated polymer particles are brightly fluorescing and stable materials for live cell imaging. Combination of conjugated polymers with a whispering gallery mode (WGM) resonator allows laser emission from microscale particles. Once internalized by cells, the mode pattern of the laser emission can be used for tagging and tracking, as each laser spectrum represents a bar code to identify individual cells. However, currently these particle systems are limited by their large size, which might interfere with cellular functions. Here, stimulated resonance Raman scattering (SRRS) in small conjugated polymer microparticles is presented as a new method for generating narrow emission as an alternative to WGM-based laser emission. This opens up spectral range for multiplexing optical readout and multicolor imaging of live cells. The synthesis of monodisperse micrometer-sized poly(fluorene-co-divinylbenzene) particles is discussed and their WGM and SRRS emission are characterized. Finally, how these particles and their emission can be employed in live cell imaging and tagging is showcased. © 2020 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemThe Potential of Combining Thermal Scanning Probes and Phase-Change Materials for Tunable Metasurfaces(Weinheim : Wiley-VCH, 2020) Michel, Ann-Katrin U.; Meyer, Sebastian; Essing, Nicolas; Lassaline, Nolan; Lightner, Carin R.; Bisig, Samuel; Norris, David J.; Chigrin, Dmitry N.Metasurfaces allow for the spatiotemporal variation of amplitude, phase, and polarization of optical wavefronts. Implementation of active tunability of metasurfaces promises compact flat optics capable of reconfigurable wavefront shaping. Phase-change materials (PCMs) are a prominent material class enabling reconfigurable metasurfaces due to their large refractive index change upon structural transition. However, commonly employed laser-induced switching of PCMs limits the achievable feature sizes and restricts device miniaturization. Thermal scanning-probe-induced local switching of the PCM germanium telluride is proposed to realize near-infrared metasurfaces with feature sizes far below what is achievable with diffraction-limited optical switching. The design is based on a planar multilayer and does not require fabrication of protruding resonators as commonly applied in the literature. Instead, it is numerically demonstrated that a broad-band tuning of perfect absorption can be realized by the localized tip-induced crystallization of the PCM. The spectral response of the metasurface is explained using resonance mode analysis and numerical simulations. To facilitate experimental realization, a theoretical description of the tip-induced crystallization employing multiphysics simulations is provided to demonstrate the great potential for fabricating compact reconfigurable metasurfaces. The concept can be applied not only for plasmonic sensing and spatial frequency filtering, but also be transferred to all-dielectric metasurfaces. © 2020 Wiley-VCH GmbH
- ItemQuantifying Rate-and Temperature-Dependent Molecular Damage in Elastomer Fracture(College Park, Md. : APS, 2020) Slootman, Juliette; Waltz, Victoria; Yeh, C. Joshua; Baumann, Christoph; Göstl, Robert; Comtet, Jean; Creton, CostantinoElastomers are highly valued soft materials finding many applications in the engineering and biomedical fields for their ability to stretch reversibly to large deformations. Yet their maximum extensibility is limited by the occurrence of fracture, which is currently still poorly understood. Because of a lack of experimental evidence, current physical models of elastomer fracture describe the rate and temperature dependence of the fracture energy as being solely due to viscoelastic friction, with chemical bond scission at the crack tip assumed to remain constant. Here, by coupling new fluorogenic mechanochemistry with quantitative confocal microscopy mapping, we are able to quantitatively detect, with high spatial resolution and sensitivity, the scission of covalent bonds as ordinary elastomers fracture at different strain rates and temperatures. Our measurements reveal that, in simple networks, bond scission, far from being restricted to a constant level near the crack plane, can both be delocalized over up to hundreds of micrometers and increase by a factor of 100, depending on the temperature and stretch rate. These observations, permitted by the high fluorescence and stability of the mechanophore, point to an intricate coupling between strain-rate-dependent viscous dissipation and strain-dependent irreversible network scission. These findings paint an entirely novel picture of fracture in soft materials, where energy dissipated by covalent bond scission accounts for a much larger fraction of the total fracture energy than previously believed. Our results pioneer the sensitive, quantitative, and spatially resolved detection of bond scission to assess material damage in a variety of soft materials and their applications. © 2020 authors. Published by the American Physical Society.
- ItemUsing Active Surface Plasmons in a Multibit Optical Storage Device to Emulate Long-Term Synaptic Plasticity(Weinheim : Wiley-VCH, 2020) Rhim, Seon-Young; Ligorio, Giovanni; Hermerschmidt, Felix; Hildebrandt, Jana; Pätzel, Michael; Hecht, Stefan; List-Kratochvil, Emil J.W.Artificial intelligence takes inspiration from the functionalities and structure of the brain to solve complex tasks and allow learning. Yet, hardware realization that simulates the synaptic activities realized with electrical devices still lags behind computer software implementation, which has improved significantly during the past decade. Herein, the capability to emulate synaptic functionalities by exploiting surface plasmon polaritons (SPPs) is shown. By depositing photochromic switching molecules (diarylethene) on a thin film of gold, it is possible to reliably control the electronic configuration of the molecules upon illumination cycles with UV and visible light. These reversible changes modulate the dielectric function of the photochromic film and thus enable the effective control of the SPP dispersion relation at the molecule/gold interface. The plasmonic device displays fundamental functions of a synapse such as potentiation, depression, and long-term plasticity. The integration of such plasmonic devices in an artificial neural network is deployed in plasmonic neuroinspired circuits for optical computing and data transmission. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemRaman-Kerr Comb Generation Based on Parametric Wave Mixing in Strongly Driven Raman Molecular Gas Medium(2020) Benoît, Aurélien; Husakou, Anton; Beaudou, Benoît; Debord, Benoît; Gérôme, Frédéric; Benabid, FetahWe report on experimental and theoretical demonstrations of an optical comb spectrum based on a combination of cascaded stimulated Raman scattering and four-wave mixing mediated by Raman-induced nonresonant Kerr-type nonlinearity. This combination enabled us to transform a conventional quasiperiodic Raman comb into a comb with a single and smaller frequency spacing. This phenomenon is achieved using a hollow-core photonic crystal fiber filled with 40 bars of deuterium and pumped with a high-power picosecond laser. The resultant comb shows more than 100 spectral lines spanning over 220 THz from 800 nm to 1710 nm, with a total output power of 7.1 W. In contrast to a pure Raman comb, a 120 THz wide portion of the spectrum exhibits denser and equally spaced spectral lines with a frequency spacing of around 1.75 THz, which is much smaller than the lowest frequency of the three excited deuterium Raman resonances. A numerical solution of the generalized nonlinear Schrödinger equation in the slowly varying envelope approximation provides very good agreement with the experimental data. The additional sidebands are explained by cascaded four-wave mixing between preexisting spectral lines, mediated by the large Raman-induced optical nonlinearity. The use of such a technique for coherent comb generation is discussed. The results show a route to the generation of optical frequency combs that combine large bandwidth and high power controllable frequency spacing.
- ItemFreestanding PAC/CNT microtubes remove sulfamethoxazole from water through a temperature-assisted cyclic process(New York, NY [u.a.] : Science Direct, 2020) Mohseni, Mojtaba; Postacchini, Pietro; Demeestere, Kristof; Du Laing, Gijs; Yüce, Süleyman; Wessling, Matthias[No abstract available]
- ItemMultiphysics simulations of adaptive metasurfaces at the meta-atom length scale(Berlin : de Gruyter, 2020) Meyer, Sebastian; Tan, Zhi Yang; Chigrin, Dmitry N.Adaptive metasurfaces (MSs) provide immense control over the phase, amplitude and propagation direction of electromagnetic waves. Adopting phase-change materials (PCMs) as an adaptive medium allows us to tune functionality of MSs at the meta-atom length scale providing full control over MS (re-)programmability. Recent experimental progress in the local switching of PCM-based MSs promises to revolutionize adaptive photonics. Novel possibilities open new challenges, one of which is a necessity to understand and be able to predict the phase transition behavior at the sub-micrometer scale. A meta-atom can be switched by a local deposition of heat using optical or electrical pulses. The deposited energy is strongly inhomogeneous and the resulting phase transition is spatially non-uniform. The drastic change of the material properties during the phase transition leads to time-dependent changes in the absorption rate and heat conduction near the meta-atom. These necessitate a self-consistent treatment of electromagnetic, thermal and phase transition processes. Here, a self-consistent multiphysics description of an optically induced phase transition in MSs is reported. The developed model is used to analyze local tuning of a perfect absorber. A detailed understanding of the phase transition at the meta-atom length scale will enable a purposeful design of programmable adaptive MSs. © 2020 Sebastian Meyer, Dmitry N. Chigrin et al., published by De Gruyter, Berlin/Boston 2020.
- ItemImpact of Reactive Amphiphilic Copolymers on Mechanical Properties and Cell Responses of Fibrin-Based Hydrogels(Weinheim : Wiley-VCH, 2020) Al Enezy-Ulbrich, Miriam Aischa; Malyaran, Hanna; de Lange, Robert Dirk; Labude, Norina; Plum, René; Rütten, Stephan; Terefenko, Nicole; Wein, Svenja; Neuss, Sabine; Pich, AndrijMechanical properties of hydrogels can be modified by the variation of structure and concentration of reactive building blocks. One promising biological source for the synthesis of biocompatible hydrogels is fibrinogen. Fibrinogen is a glycoprotein in blood, which can be transformed enzymatically to fibrin playing an important role in wound healing and clot formation. In the present work, it is demonstrated that hybrid hydrogels with their improved mechanical properties, tunable internal structure, and enhanced resistance to degradation can be synthesized by a combination of fibrinogen and reactive amphiphilic copolymers. Water-soluble amphiphilic copolymers with tunable molecular weight and controlled amounts of reactive epoxy side groups are used as reactive crosslinkers to reinforce fibrin hydrogels. In the present work, copolymers that can influence the mechanical properties of fibrin-based hydrogels are used. The reactive copolymers increase the storage modulus of the hydrogels from 600 Pa to 30 kPa. The thickness of fibrin fibers is regulated by the copolymer concentration. It could be demonstrated that the fibrin-based hydrogels are biocompatible and support cell proliferation. Their degradation rate is considerably slower than that of native fibrin gels. In conclusion, fibrin-based hydrogels with tunable elasticity and fiber thickness useful to direct cell responses like proliferation and differentiation are produced. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim