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  1. Abstract

    Manufacturing of low‐density‐high‐strength carbon foams can benefit the construction, transportation, and packaging industries. One successful route to lightweight and mechanically strong carbon foams involves pyrolysis of polymeric architectures, which is inevitably accompanied by drastic volumetric shrinkage (usually >98%). As such, a challenge of these materials lies in maintaining bulk dimensions of building struts that span orders of magnitude difference in length scale from centimeters to nanometers. This work demonstrates fabrication of macroscale low‐density‐high‐strength carbon foams that feature exceptional dimensional stability through pyrolysis of robust template‐coating pairs. The template serves as the architectural blueprint and contains strength‐imparting properties (e.g., high node density and small strut dimensions); it is composed of a low char‐yielding porous polystyrene backbone with a high carbonization‐onset temperature. The coating serves to imprint and transcribe the template architecture into pyrolytic carbon; it is composed of a high char‐yielding conjugated polymer with a relatively low carbonization‐onset temperature. The designed carbonization mismatch enables structural inheritance, while the decomposition mismatch affords hollow struts, minimizing density. The carbons synthesized through this new framework exhibit remarkable dimensional stability (≈80% dimension retention; ≈50% volume retention) and some of the highest specific strengths (≈0.13 GPa g−1cm3) among reported carbon foams derived from porous polymer templates.

     
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  2. Abstract

    Although sonodynamic therapy (SDT) has shown promise for cancer treatment, the lack of efficient sonosensitizers (SSs) has limited the clinical application of SDT. Here, a new strategy is reported for designing efficient nano‐sonosensitizers based on 2D nanoscale metal–organic layers (MOLs). Composed of Hf‐oxo secondary building units (SBUs) and iridium‐based linkers, the MOL is anchored with 5,10,15,20‐tetra(p‐benzoato)porphyrin (TBP) sensitizers on the SBUs to afford TBP@MOL. TBP@MOL shows 14.1‐ and 7.4‐fold higher singlet oxygen (1O2) generation than free TBP ligands and Hf‐TBP, a 3D nanoscale metal–organic framework, respectively. The1O2generation of TBP@MOL is enhanced by isolating TBP SSs on the SBUs of the MOL, which prevents aggregation‐induced quenching of the excited sensitizers, and by triplet–triplet Dexter energy transfer between excited iridium‐based linkers and TBP SSs, which more efficiently harnesses broad‐spectrum sonoluminescence. Anchoring TBP on the MOL surface also enhances the energy transfer between the excited sensitizer and ground‐state triplet oxygen to increase1O2generation efficacy. In mouse models of colorectal and breast cancer, TBP@MOL demonstrates significantly higher SDT efficacy than Hf‐TBP and TBP. This work uncovers a new strategy to design effective nano‐sonosensitizers by facilitating energy transfer to efficiently capture broad‐spectrum sonoluminescence and enhance1O2generation.

     
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  3. Abstract

    Poly(lactic acid) (PLA) is a commercially available bio‐based polymer that is a potential alternative to many commodity petrochemical‐based polymers. However, PLA's thermomechanical properties limit its use in many applications. Incorporating polymer‐grafted cellulose nanocrystals (CNCs) is one potential route to improving these mechanical properties. One key challenge in using these polymer‐grafted nanoparticles is to understand which variables associated with polymer grafting are most important for improving composite properties. In this work, poly(ethylene glycol)‐grafted CNCs are used to study the effects of polymer grafting density and molecular weight on the properties of PLA composites. All CNC nanofillers are found to reinforce PLA above the glass transition temperature, but non‐grafted CNCs and CNCs grafted with short PEG chains (<2 kg mol−1) are found to cause significant embrittlement, generally resulting in less than 3% elongation‐at‐break. By grafting higher molecular weight PEG (10 kg mol−1) onto the CNCs at a grafting density where the polymer chains are predicted to be in the semi‐dilute polymer brush conformation (~0.1 chains nm−2), embrittlement can be avoided.

     
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  4. Abstract

    Surface acoustic waves are commonly used in classical electronics applications, and their use in quantum systems is beginning to be explored, as evidenced by recent experiments using acoustic Fabry–Pérot resonators. Here we explore their use for quantum communication, where we demonstrate a single-phonon surface acoustic wave transmission line, which links two physically separated qubit nodes. Each node comprises a microwave phonon transducer, an externally controlled superconducting variable coupler, and a superconducting qubit. Using this system, precisely shaped individual itinerant phonons are used to coherently transfer quantum information between the two physically distinct quantum nodes, enabling the high-fidelity node-to-node transfer of quantum states as well as the generation of a two-node Bell state. We further explore the dispersive interactions between an itinerant phonon emitted from one node and interacting with the superconducting qubit in the remote node. The observed interactions between the phonon and the remote qubit promise future quantum-optics-style experiments with itinerant phonons.

     
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  5. Abstract

    The highly intricate structures of biological systems make the precise probing of biological behaviors at the cellular‐level particularly difficult. As an advanced toolset capable of exploring diverse biointerfaces, high‐aspect‐ratio nanowires stand out with their unique mechanical, optical, and electrical properties. Specifically, semiconductor nanowires show much promise in their tunability and feasibility for synthesis and fabrication. Thus far, semiconductor nanowires have shown favorable results in deciphering biological communications and translating this cellular language through the nanowire‐based biointerfaces. In this perspective, the synthesis and fabrication methods for different kinds of nanowires and nanowire‐based structures are first surveyed. Next, several cellular‐level nanowire‐enabled applications in biophysical dynamics probing, physiological or biochemical sensing, and biological activity modulation are highlighted. Then, the progress of functionalized nanowires in drug delivery and bioenergy production is reviewed. Finally, the current limitations of nanowires and an outlook into the next generation of nanowire‐based devices at the biointerfaces are concluded.

     
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  6. Abstract

    The proteins that make up the actin cytoskeleton can self-assemble into a variety of structures. In vitro experiments and coarse-grained simulations have shown that the actin crosslinking proteins α-actinin and fascin segregate into distinct domains in single actin bundles with a molecular size-dependent competition-based mechanism. Here, by encapsulating actin, α-actinin, and fascin in giant unilamellar vesicles (GUVs), we show that physical confinement can cause these proteins to form much more complex structures, including rings and asters at GUV peripheries and centers; the prevalence of different structures depends on GUV size. Strikingly, we found that α-actinin and fascin self-sort into separate domains in the aster structures with actin bundles whose apparent stiffness depends on the ratio of the relative concentrations of α-actinin and fascin. The observed boundary-imposed effect on protein sorting may be a general mechanism for creating emergent structures in biopolymer networks with multiple crosslinkers.

     
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  7. Abstract

    Biocompatible and nanoscale devices for biological modulation of cells and tissues possess the potential for tremendous impact on medical and industrial technologies. Typical medical devices and therapies tend to be macroscale, comprised of nonbiocompatible materials, and broadly targeted, resulting in imprecise treatments and adverse effects such as chronic immune response and tissue damage. The development of nanoenabled and biocompatible technologies—ranging from biodegradable nanoparticles for localized drug delivery to transient electronic devices for stimulation therapy to engineered biofilms with applications to nanomedicine—will continue to enable the advent of personalized medicine and precision therapies. In this review, recent research into this frontier is reviewed, first analyzing the synthesis of nanoenabled and biocompatible technologies and then presenting significant considerations regarding the development of such materials. Lastly, the latest advancements in biocompatible, nanoenabled devices are examined, followed by a discussion of the direction of future research in the field.

     
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  8. Abstract

    The actin cytoskeleton is important for maintaining mechanical homeostasis in adherent cells, largely through its regulation of adhesion and cortical tension. The LIM (Lin‐11,Isl1,MEC‐3) domain‐containing proteins are involved in a myriad of cellular mechanosensitive pathways. Recent work has discovered that LIM domains bind to mechanically stressed actin filaments, suggesting a novel and widely conserved mechanism of mechanosensing. This review summarizes the current state of knowledge of LIM protein mechanosensitivity.

     
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  9. Abstract

    Conjugated polymer‐based block copolymers (CP‐BCPs) are an unexplored class of materials for organic thermoelectrics. Herein, the authors report on the electronic conductivity (σ) and Seebeck coefficient (α) of a newly synthesized CP‐BCP, poly(3‐hexylthiophene)‐block‐poly (oligo‐oxyethylene methacrylate) (P3HT‐b‐POEM), upon solution co‐processing with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and subsequently vapor‐doping with a molecular dopant, 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4TCNQ). It is found that the addition of the hydrophilic block POEM greatly enhances the processability of P3HT, enabling homogeneous solution‐mixing with LiTFSI. Notably, interactions between P3HT‐b‐POEM with ionic species significantly improve molecular order and unexpectedly cause electrical oxidizing doping of P3HT block both in solution and solid‐states, a phenomenon that has not been previously observed in Li‐salt containing P3HT. Vapor doping of P3HT‐b‐POEM‐LiTFSI thin films with F4TCNQ further enhances σ and yields a thermoelectric power factorPF=α2σ of 13.0 µW m−1 K−2, which is more than 20 times higher than salt‐free P3HT‐b‐POEM sample. Through modeling thermoelectric behaviors of P3HT‐b‐POEM with the Kang‐Snyder transport model, the improvement inPFis attributed to higher electronic charge mobility originating from the enhanced molecular ordering of P3HT. The results demonstrate that solution co‐processing CP‐BCPs with a salt is a powerful method to control structure and performance of organic thermoelectric materials.

     
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  10. Abstract

    Precise patterning of quantum dot (QD) layers is an important prerequisite for fabricating QD light‐emitting diode (QLED) displays and other optoelectronic devices. However, conventional patterning methods cannot simultaneously meet the stringent requirements of resolution, throughput, and uniformity of the pattern profile while maintaining a high photoluminescence quantum yield (PLQY) of the patterned QD layers. Here, a specially designed nanocrystal ink is introduced, “photopatternable emissive nanocrystals” (PENs), which satisfies these requirements. Photoacid generators in the PEN inks allow photoresist‐free, high‐resolution optical patterning of QDs through photochemical reactions and in situ ligand exchange in QD films. Various fluorescence and electroluminescence patterns with a feature size down to ≈1.5 µm are demonstrated using red, green, and blue PEN inks. The patterned QD films maintain ≈75% of original PLQY and the electroluminescence characteristics of the patterned QLEDs are comparable to thopse of non‐patterned control devices. The patterning mechanism is elucidated by in‐depth investigation of the photochemical transformations of the photoacid generators and changes in the optical properties of the QDs at each patterning step. This advanced patterning method provides a new way for additive manufacturing of integrated optoelectronic devices using colloidal QDs.

     
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