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- ItemLighting the Path: Light Delivery Strategies to Activate Photoresponsive Biomaterials In Vivo(Weinheim : Wiley-VCH, 2021) Pearson, Samuel; Feng, Jun; del Campo, AránzazuPhotoresponsive biomaterials are experiencing a transition from in vitro models to in vivo demonstrations that point toward clinical translation. Dynamic hydrogels for cell encapsulation, light-responsive carriers for controlled drug delivery, and nanomaterials containing photosensitizers for photodynamic therapy are relevant examples. Nonetheless, the step to the clinic largely depends on their combination with technologies to bring light into the body. This review highlights the challenge of photoactivation in vivo, and presents strategies for light management that can be adopted for this purpose. The authors’ focus is on technologies that are materials-driven, particularly upconversion nanoparticles that assist in “direct path” light delivery through tissue, and optical waveguides that “clear the path” between external light source and in vivo target. The authors’ intention is to assist the photoresponsive biomaterials community transition toward medical technologies by presenting light delivery concepts that can be integrated with the photoresponsive targets. The authors also aim to stimulate further innovation in materials-based light delivery platforms by highlighting needs and opportunities for in vivo photoactivation of biomaterials. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.
- ItemBioinspired Underwater Adhesion to Rough Substrates by Cavity Collapse of Cupped Microstructures(Weinheim : Wiley-VCH, 2021) Wang, Yue; Hensel, RenéUnderwater or wet adhesion is highly desirable for numerous applications but is counteracted by the liquids in the contact which weaken intermolecular attraction. The problem is exacerbated in conjunction with surface roughness when liquids partially remain in grooves or dimples of the substrate. In the present study, a cupped microstructure with a cavity inspired by suction organs of aquatic animals is proposed. The microstructures (cup radius of 100 µm) are made from polyurethane using two-photon lithography followed by replica molding. Adhesion to rough substrates is emulated experimentally by a micropatterned model substrate with varying channel widths. Pull-off stresses are found to be about 200 kPa, i.e., twice atmospheric pressure. Evaluation of force–displacement curves together with in situ observations reveal the adhesion mechanism, which involves adaptation to surface roughness and an elastic force induced by the collapse of the cavity that holds sealed contact with the substrate during retraction. This new microarchitecture may pave the way for next generation microstructures applicable to real, rough surfaces under wet conditions.
- ItemEngineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications(Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, EduardReversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
- ItemIn Situ Observation Reveals Local Detachment Mechanisms and Suction Effects in Micropatterned Adhesives(Weinheim : Wiley-VCH, 2019) Tinnemann, Verena; Hernández, Luissé; Fischer, Sarah C.L.; Arzt, Eduard; Bennewitz, Roland; Hensel, RenéFibrillar adhesion pads of insects and geckoes have inspired the design of high-performance adhesives enabling a new generation of handling devices. Despite much progress over the last decade, the current understanding of these adhesives is limited to single contact pillars and the behavior of whole arrays is largely unexplored. In the study reported here, a novel approach is taken to gain insight into the detachment mechanisms of whole micropatterned arrays. Individual contacts are imaged by frustrated total internal reflection, allowing in situ observation of contact formation and separation during adhesion tests. The detachment of arrays is found to be governed by the distributed adhesion strength of individual pillars, but no collaborative effect mediated by elastic interactions can be detected. At the maximal force, about 30% of the mushroom structures are already detached. The adhesive forces decrease with reduced air pressure by 20% for the smooth and by 6% for the rough specimen. These contributions are attributed to a suction effect, whose strength depends critically on interfacial defects controlling the sealing quality of the contact. This dominates the detachment process and the resulting adhesion strength. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemHighly Tunable Nanostructures in a Doubly pH-Responsive Pentablock Terpolymer in Solution and in Thin Films(Weinheim : Wiley-VCH, 2021) Jung, Florian A.; Schart, Maximilian; Bührend, Lukas; Meidinger, Elisabeth; Kan, Jia-Jhen; Niebuur, Bart-Jan; Ariaee, Sina; Molodenskiy, Dmitry S.; Posselt, Dorthe; Amenitsch, Heinz; Tsitsilianis, Constantinos; Papadakis, Christine M.Multiblock copolymers with charged blocks are complex systems that show great potential for enhancing the structural control of block copolymers. A pentablock terpolymer PMMA-b-PDMAEMA-b-P2VP-b-PDMAEMA-b-PMMA is investigated. It contains two types of midblocks, which are weak cationic polyelectrolytes, namely poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) and poly(2-vinylpyridine) (P2VP). Furthermore, these are end-capped with short hydrophobic poly(methyl methacrylate) (PMMA) blocks in dilute aqueous solution and thin films. The self-assembly behavior depends on the degrees of ionization α of the P2VP and PDMAEMA blocks, which are altered in a wide range by varying the pH value. High degrees of ionization of both blocks prevent structure formation, whereas microphase-separated nanostructures form for a partially charged and uncharged state. While in solutions, the nanostructure formation is governed by the dependence of the P2VP block solubility of the and the flexibility of the PDMAEMA blocks on α, in thin films, the dependence of the segregation strength on α is key. Furthermore, the solution state plays a crucial role in the film formation during spin-coating. Overall, both the mixing behavior of the 3 types of blocks and the block sequence, governing the bridging behavior, result in strong variations of the nanostructures and their repeat distances.