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Metamaterials are emerging as an unconventional platform to perform computing abstractions in physical systems by processing environmental stimuli into information. While computation functions have been demonstrated in mechanical systems, they rely on compliant mechanisms to achieve predefined states, which impose inherent design restrictions that limit their miniaturization, deployment, reconfigurability, and functionality. Here, a metamaterial system is described based on responsive magnetoactive Janus particle (MAJP) swarms with multiple programmable functions. MAJPs are designed with tunable structure and properties in mind, that is, encoded swarming behavior and fully reversible switching mechanisms, to enable programmable dynamic display, non-volatile and semi-volatile memory, Boolean logic, and information encryption functions in soft, wearable devices. MAJPs and their unique swarming behavior open new functions for the design of multifunctional and reconfigurable display devices, and constitute a promising building block to develop the next generation of soft physical computing devices, with growing applications in security, defense, anti-counterfeiting, camouflage, soft robotics, and human-robot interaction., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Molecular structuring of soft matter with precise arrangements over multiple hierarchical levels, especially on polymer surfaces, and enabling their post-synthetic modulation has tremendous potential for application in molecular engineering and interfacial science. Here, recent research and developments in design strategies for structurally controlled polymer surfaces via cyclophane-based chemical vapor deposition (CVD) polymerization with precise control over chemical functionalities and post-CVD fabrication via orthogonal surface functionalization that facilitates the formation of designable biointerfaces are summarized. Particular discussion about innovative approaches for the templated synthesis of shape-controlled CVD polymers, ranging from 1D to 3D architecture, including inside confined nanochannels, nanofibers/nanowires synthesis into an anisotropic media such as liquid crystals, and CVD polymer nanohelices via hierarchical chirality transfer across multiple length scales is provided. Aiming at multifunctional polymer surfaces via CVD copolymerization of multiple precursors, the structural and functional design of the fundamental [2.2]paracyclophane (PCP) precursor molecules, that is, functional CVD monomer chemistry is also described. Technologically advanced and innovative surface deposition techniques toward topological micro- and nanostructuring, including microcontact printing, photopatterning, photomask, and lithographic techniques such as dip-pen nanolithography, showcasing research from the authors' laboratories as well as other's relevant important findings in this evolving field are highlighted that have introduced new programmable CVD polymerization capabilities. Perspectives, current limitations, and future considerations are provided., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

The development of simple and accurate methods to predict mutations in proteins remains an unsolved challenge in modern biochemistry. It is discovered that critical information about primary and secondary peptide structures can be inferred from the stains left behind by their drying droplets. To analyze the complex stain patterns, deep-learning neuronal networks are challenged with polarized light microscopy images derived from the drying droplet deposits of a range of amyloid beta (1-42) (Aβ 42 ) peptides. These peptides differ in a single amino acid residue and represent hereditary mutants of Alzheimer's disease. Stain patterns are not only reproducible but also result in comprehensive stratification of eight amyloid beta (Aβ) variants with predictive accuracies above 99%. Similarly, peptide stains of a range of distinct Aβ 42 peptide conformations are identified with accuracies above 99%. The results suggest that a method as simple as drying a droplet of a peptide solution onto a solid surface may serve as an indicator of minute, yet structurally meaningful differences in peptides' primary and secondary structures. Scalable and accurate detection schemes for stratification of conformational and structural protein alterations are critically needed to unravel pathological signatures in many human diseases such as Alzheimer's and Parkinson's disease., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Mesoscale chiral materials are prepared by lithographic methods, assembly of chiral building blocks, and through syntheses in the presence of polarized light. Typically, these processes result in micrometer-sized structures, require complex top-down manipulation, or rely on tedious asymmetric separation. Chemical vapor deposition (CVD) polymerization of chiral precursors into supported films of liquid crystals (LCs) are discovered to result in superhierarchical arrangements of enantiomorphically pure nanofibers. Depending on the molecular chirality of the 1-hydroxyethyl [2.2]paracyclophane precursor, extended arrays of enantiomorphic nanohelices are formed from achiral nematic templates. Arrays of chiral nanohelices extend over hundreds of micrometers and consistently display enantiomorphic micropatterns. The pitch of individual nanohelices depends on the enantiomeric excess and the purity of the chiral precursor, consistent with the theoretical model of a doubly twisted LC director configuration. During CVD of chiral precursors into cholesteric LC films, aspects of molecular and mesoscale asymmetry combine constructively to form regularly twisted nanohelices. Enantiomorphic surfaces permit the tailoring of a wide range of functional properties, such as the asymmetric induction of weak chiral systems., (© 2022 Wiley-VCH GmbH.)

Adjuvants play a critical role in the design and development of novel vaccines. Despite extensive research, only a handful of vaccine adjuvants have been approved for human use. Currently used adjuvants are mostly composed of components that are non-native to the human body, such as aluminum salt, bacterial lipids, or foreign genomic material. Here, a new ionic-liquid-based adjuvant is explored, synthesized using two metabolites of the body, choline and lactic acid (ChoLa). ChoLa distributes the antigen efficiently upon injection, maintains antigen integrity, enhances immune infiltration at the injection site, and leads to a potent immune response against the antigen. Thus, it can serve as a promising safe adjuvant platform that can help to protect against pandemics and future infectious threats., (© 2020 Wiley-VCH GmbH.)

Extracellular matrix (ECM) proteins, and most prominently, fibronectin (Fn), are routinely used in the form of adsorbed pre-coatings in an attempt to create a cell-supporting environment in both two- and three-dimensional cell culture systems. However, these protein coatings are typically deposited in a form which is structurally and functionally distinct from the ECM-constituting fibrillar protein networks naturally deposited by cells. Here, the cell-free and scalable synthesis of freely suspended and mechanically robust three-dimensional (3D) networks of fibrillar fibronectin (fFn) supported by tessellated polymer scaffolds is reported. Hydrodynamically induced Fn fibrillogenesis at the three-phase contact line between air, an Fn solution, and a tessellated scaffold microstructure yields extended protein networks. Importantly, engineered fFn networks promote cell invasion and proliferation, enable in vitro expansion of primary cancer cells, and induce an epithelial-to-mesenchymal transition in cancer cells. Engineered fFn networks support the formation of multicellular cancer structures cells from plural effusions of cancer patients. With further work, engineered fFn networks can have a transformative impact on fundamental cell studies, precision medicine, pharmaceutical testing, and pre-clinical diagnostics., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Synthetic biological systems are used for a myriad of applications, including tissue engineered constructs for in vivo use and microengineered devices for in vitro testing. Recent advances in engineering complex biological systems have been fueled by opportunities arising from the combination of bioinspired materials with biological and computational tools. Driven by the availability of large datasets in the "omics" era of biology, the design of the next generation of tissue equivalents will have to integrate information from single-cell behavior to whole organ architecture. Herein, recent trends in combining multiscale processes to enable the design of the next generation of biomaterials are discussed. Any successful microprocessing pipeline must be able to integrate hierarchical sets of information to capture key aspects of functional tissue equivalents. Micro- and biofabrication techniques that facilitate hierarchical control as well as emerging polymer candidates used in these technologies are also reviewed., (© 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Bioinspiration has emerged as an important design principle in the rapidly growing field of materials science and especially its subarea, soft matter science. For example, biological cells form hierarchically organized tissues that not only are optimized and designed for durability, but also have to adapt to their external environment, undergo self-repair, and perform many highly complex functions. Being able to create artificial soft materials that mimic those highly complex functions will enable future materials applications. Herein, soft matter technologies that are used to realize bioinspired material structures are described, and potential pathways to integrate these into a comprehensive soft matter research environment are addressed. Solutions become available because soft matter technologies are benefitting from the synergies between organic synthesis, polymer chemistry, and materials science., (© 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The advent of adaptive manufacturing techniques supports the vision of cell-instructive materials that mimic biological tissues. 3D jet writing, a modified electrospinning process reported herein, yields 3D structures with unprecedented precision and resolution offering customizable pore geometries and scalability to over tens of centimeters. These scaffolds support the 3D expansion and differentiation of human mesenchymal stem cells in vitro. Implantation of these constructs leads to the healing of critical bone defects in vivo without exogenous growth factors. When applied as a metastatic target site in mice, circulating cancer cells home in to the osteogenic environment simulated on 3D jet writing scaffolds, despite implantation in an anatomically abnormal site. Through 3D jet writing, the formation of tessellated microtissues is demonstrated, which serve as a versatile 3D cell culture platform in a range of biomedical applications including regenerative medicine, cancer biology, and stem cell biotechnology., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Molecules can be immobilized onto biomaterials by a chemical vapor deposition (CVD) coating strategy. Pentafluorophenolester groups react with amine side chains on antibodies, which can selectively immobilize adenoviral vectors for gene delivery of growth factors. These vectors can produce functional proteins within defined regions of biomaterials to produce customizable structures for targeted tissue regeneration., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The precise modulation of fluorescence interference contrast is achieved by introducing a nanoscopically engineered spacer layer prepared by chemical vapor deposition (CVD) of functional polymers. These novel imaging substrates are chemically identical throughout their entire detection area, yet present patterns of nanoscale thickness. A protein binding cascade is studied in real time and in the presence of high background noise., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Biohybrid microcylinders are fabricated using electrohydrodynamic cojetting followed by a surface chemistry approach to maximize cell-adhesive characteristics. As proper cell alignment and mechanical stiffness are important components of bioactuator design, spatial cell selectivity and stress/strain properties of microcylinders are characterized to demonstrate their capability of response to rat cardio-myocyte contraction. These microcylinders can find applications in a host of micromechanical systems., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Selective growth of metal organic framework materials on the surface of compartmentalized polymer microparticles is achieved by electro-hydrodynamic co-jetting, selective surface modification, and anisotropic crystal growth., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Biocompatible anisotropic polymer particles with bipolar affinity towards human endothelial cells are a novel type of building blocks for microstructured biohybrid materials, report Joerg Lahann and co-workers on p. 4920. Functional polarity due to two biologically distinct hemispheres has been achieved by synthesis of anisotropic particles via electro-hydrodynamic co-jetting of two different polymer solutions and subsequent selective surface modification., (Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Biocompatible anisotropic polymer particles with bipolar affinity towards human endothelial cells are a novel type of building blocks for microstructured bio-hybrid materials. Functional polarity due to two biologically distinct hemispheres has been achieved by synthesis of anisotropic particles via electro-hydrodynamic co-jetting of two different polymer solutions and subsequent selective surface modification., (Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)