The discovery of two-dimensional electron gases at the heterointerface between two insulating perovskite-type oxides, such as LaAlO 3 and SrTiO 3 , provides opportunities for a new generation of all-oxide electronic devices. Key challenges remain for achieving interfacial electron mobilities much beyond the current value of approximately 1,000 cm 2 V -1 s -1 (at low temperatures). Here we create a new type of two-dimensional electron gas at the heterointerface between SrTiO 3 and a spinel g-Al 2 O 3 epitaxial film with compatible oxygen ions sublattices. Electron mobilities more than one order of magnitude higher than those of hitherto-investigated perovskite-type interfaces are obtained. The spinel/perovskite twodimensional electron gas, where the two-dimensional conduction character is revealed by quantum magnetoresistance oscillations, is found to result from interface-stabilized oxygen vacancies confined within a layer of 0.9 nm in proximity to the interface. Our findings pave the way for studies of mesoscopic physics with complex oxides and design of high-mobility all-oxide electronic devices.
Vaccines aim to elicit a robust, yet targeted, immune response. Failure of a vaccine to elicit such a response arises in part from inappropriate temporal control over antigen and adjuvant presentation to the immune system. In this work, we sought to exploit the immune system’s natural response to extended pathogen exposure during infection by designing an easily administered slow-delivery vaccine platform. We utilized an injectable and self-healing polymer–nanoparticle (PNP) hydrogel platform to prolong the codelivery of vaccine components to the immune system. We demonstrated that these hydrogels exhibit unique delivery characteristics, whereby physicochemically distinct compounds (such as antigen and adjuvant) could be codelivered over the course of weeks. When administered in mice, hydrogel-based sustained vaccine exposure enhanced the magnitude, duration, and quality of the humoral immune response compared to standard PBS bolus administration of the same model vaccine. We report that the creation of a local inflammatory niche within the hydrogel, coupled with sustained exposure of vaccine cargo, enhanced the magnitude and duration of germinal center responses in the lymph nodes. This strengthened germinal center response promoted greater antibody affinity maturation, resulting in a more than 1000-fold increase in antigen-specific antibody affinity in comparison to bolus immunization. In summary, this work introduces a simple and effective vaccine delivery platform that increases the potency and durability of subunit vaccines.
The successful incorporation of active proteins into synthetic polymers could lead to a new class of materials with functions found only in living systems. However, proteins rarely function under the conditions suitable for polymer processing. On the basis of an analysis of trends in protein sequences and characteristic chemical patterns on protein surfaces, we designed four-monomer random heteropolymers to mimic intrinsically disordered proteins for protein solubilization and stabilization in non-native environments. The heteropolymers, with optimized composition and statistical monomer distribution, enable cell-free synthesis of membrane proteins with proper protein folding for transport and enzyme-containing plastics for toxin bioremediation. Controlling the statistical monomer distribution in a heteropolymer, rather than the specific monomer sequence, affords a new strategy to interface with biological systems for protein-based biomaterials.
Magnetocaloric materials with a Curie temperature near room temperature have attracted significant interest for some time due to their possible application for high‐efficiency refrigeration devices. This review focuses on a number of key issues of relevance for the characterization, performance and implementation of such materials in actual devices. The phenomenology and fundamental thermodynamics of magnetocaloric materials is discussed, as well as the hysteresis behavior often found in first‐order materials. A number of theoretical and experimental approaches and their implications are reviewed. The question of how to evaluate the suitability of a given material for use in a magnetocaloric device is covered in some detail, including a critical assessment of a number of common performance metrics. Of particular interest is which non‐magnetocaloric properties need to be considered in this connection. An overview of several important materials classes is given before considering the performance of materials in actual devices. Finally, an outlook on further developments is presented.
Synthetic polymers are ubiquitous in the modern world, but our ability to exert control over the molecular conformation of individual polymers is very limited. In particular, although the programmable self-assembly of oligonucleotides and proteins into artificial nanostructures has been demonstrated, we currently lack the tools to handle other types of synthetic polymers individually and thus the ability to utilize and study their single-molecule properties. Here we show that synthetic polymer wires containing short oligonucleotides that extend from each repeat can be made to assemble into arbitrary routings. The wires, which can be more than 200 nm in length, are soft and bendable, and the DNA strands allow individual polymers to self-assemble into predesigned routings on both two- and three-dimensional DNA origami templates. The polymers are conjugated and potentially conducting, and could therefore be used to create molecular-scale electronic or optical wires in arbitrary geometries.
Poly(vinyl alcohol), PVA, and physical hydrogels derived thereof have an excellent safety profile and a successful history of biomedical applications. However, these materials are hardly in the focus of biomedical research, largely due to poor opportunities in nano- and micro-scale design associated with PVA hydrogels in their current form. In this review we aim to demonstrate that with PVA, a (sub)molecular control over polymer chemistry translates into fine-tuned supramolecular association of chains and this, in turn, defines macroscopic properties of the material. This nano- to micro- to macro- translation of control is unique for PVA and can now be accomplished using modern tools of macromolecular design. We believe that this strategy affords functionalized PVA physical hydrogels which meet the demands of modern nanobiotechnology and have a potential to become an indispensable tool in the design of biomaterials.
Stem cell therapies have emerged as promising treatments for injuries and diseases in regenerative medicine. Yet, delivering stem cells therapeutically can be complicated by invasive administration techniques, heterogeneity in the injection media, and/or poor cell retention at the injection site. Despite these issues, traditional administration protocols using bolus injections in a saline solution or surgical implants of cellladen hydrogels have highlighted the promise of cell administration as a treatment strategy. To address these limitations, we have designed an injectable polymernanoparticle (PNP) hydrogel platform exploiting multivalent, noncovalent interactions between modified biopolymers and biodegradable nanoparticles for encapsulation and delivery of human mesenchymal stem cells (hMSCs). hMSC-based therapies have shown promise due to their broad differentiation capacities and production of therapeutic paracrine signaling molecules. In this work, the fundamental hydrogel mechanical properties that enhance hMSC delivery processes are elucidated using basic in vitro models. Further, in vivo studies in immunocompetent mice reveal that PNP hydrogels enhance hMSC retention at the injection site and retain administered hMSCs locally for upwards of 2 weeks. Through both in vitro and in vivo experiments, we demonstrate a novel scalable, synthetic, and biodegradable hydrogel system that overcomes current limitations and enables effective cell delivery. K E Y W O R D Scell delivery, human mesenchymal stem cell, hydrogel, injectable
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