AbstractDielectric substances exhibit great potential for high-power capacitors due to their high stability and fast charge–discharge; however, a long-term challenge is to enhance energy density. Here, we propose a poly(vinylidene fluoride) (PVDF) composite utilizing BaTiO3 nanoparticle@TiO2 nanosheet (BT@TO ns) 2D nanohybrids as fillers, aiming at combining the interfacial strategy of using a core–shell filler and the electron scattering of a 2D filler to improve the energy density. With 4 wt% filler, the composite possesses the largest breakdown strength (Eb) of 561.2 MV m−1, which is significantly enhanced from the 407.6 MV m−1 of PVDF, and permittivity of 12.6 at 1 kHz, which is a 23% increase from that of PVDF. A superhigh energy density of 21.3 J cm−3 with an efficiency of 61% is obtained at 550 MV m−1. The 2D BT@TO ns-filled composite exhibits a higher energy density than composites filled with core–shell 1D BT@TO nws or non-core–shell 0D BT, 1D TO, or 2D TO particles. The Eb and energy density improvements are attributed to the buffer layer-based interface engineering and enhanced area scattering of electrons caused by the 2D hybrids, an effect similar to that of a ping-pong paddle to scatter electric field-induced charge migrations in composites. Thus, an effective hybrid strategy is presented for achieving high-performance polymer composites that can be used in energy storage devices.
AbstractAmid the COVID-19 pandemic, cancer continues to be the most devastating disease worldwide. Liquid biopsy of circulating tumor cells (CTCs) has recently become a painless and noninvasive tool for obtaining carcinoma cell samples for molecular profiling. Here, we report efficient detection and collection of cancer cells in blood samples by combining stem cell antigen (CD44)-specific immunosilica particles and immunofluorescent quantum dots with spectrally and temporally resolved single-photon counting. We accurately detect 1–10 cells among 100 cancer cells of the breast, lungs, or cervix in 1 mL blood samples. In addition, the bright and narrowband emission of CdSe/ZnS quantum dots enables temporally and spectrally resolved photon counting for multiplexed cancer cell detection. The cancer cell-specific and large immunosilica particles helped us collect the specific cells. We validate the detection efficiency and multimodality of this strategy by time-stamped and energy-dispersed single-photon counting of orange- and red-emitting quantum dots and green-fluorescing nuclei stained with Syto-13/25 dye. Thus, the present work highlights the prospects of multimodal CTC detection for noninvasive cancer screening and postsurgical or therapeutic follow-up.
AbstractExcessive epidural fibrosis attached to the dura mater is the major cause of recurrent failed back surgery syndrome after spine surgery. Neutrophil extracellular traps (NETs) promote epidural fibrosis, raising the possibility that the DNA backbone of NETs may be a potential target in the therapy of epidural fibrosis. Human body temperature-sensitive hydroxypropyl chitin hydrogel solutions were prepared to encapsulate DNase I, which gradually decomposed in vivo. DNase I, which was released from temperature-sensitive hydrogels, destroyed the DNA backbone of NETs and dispersed the clustering of myeloperoxidase (MPO) in NETs. Evidence from MRI, H&E and Masson staining supported that hydroxypropyl chitin hydrogels loaded with DNase I were nontoxic and reduced epidural fibrosis. As expected, fibronectin in the wound was significantly abridged in the mice treated with hydrogels loaded with DNase I. Compared with the gelatin sponge absorbing DNase I, temperature-sensitive hydroxypropyl chitin hydrogels loaded with DNase I were more powerful in the therapy of epidural fibrosis. These results indicate that temperature-sensitive hydroxypropyl chitin hydrogels were effective in DNase I encapsulation and alleviation of epidural fibrosis in a mouse model of laminectomy.
AbstractSustained and controllable local gene therapy is a potential method for treating osteoarthritis (OA) through the delivery of therapeutic microRNAs (miRNAs) to targeted cells. However, direct injection of crude miRNAs for local gene therapy is limited due to its inadequate transfection efficiency, easy inactivation, and short half-life. Here, a multifunctional gene vector, arginine, histidine, and phenylalanine-modified generation 5 polyamidoamine (named G5-AHP), was employed to form G5-AHP/miR-140 nanoparticles by forming a complex with microRNA-140 (miR-140). Then, the nanoparticles were entrapped in hydrogel microspheres (MSs) to construct a “nano-micron” combined gene hydrogel to alleviate the degradation of articular cartilage. Monodisperse gelatin methacryloyl hydrogel MSs were produced under ultraviolet light using one-step innovative microfluidic technology. Evenly dispersed MSs showed better injectability in sustainable and matrix metalloproteinases (MMPs)-responsive degradation methods for local gene delivery. The G5-AHP/miR-140 nanoparticles released from the MSs exhibited high gene transfection efficacy and long-term bioactivity, facilitated endocytosis, and thus maintained the metabolic balance of cartilage matrix by promoting the expression of type II collagen and inhibiting the expression of a disintegrin and metalloproteinase with thrombospondin motifs-5 and MMP13 in chondrocytes. After injection of the “nano-micron” combined gene hydrogel into the articular cavity of the OA model, the gene hydrogel increased G5-AHP/miR-140 nanoparticle retention, prevented articular cartilage degeneration, and reduced osteophyte formation in a surgically induced mouse model of OA. The present study provides a novel cell-free approach to alleviate the progression of OA that shows potential for locally injected gene delivery systems.
AbstractExosomes, as one type of extracellular vesicle derived from multiple cells, have much potential as cancer biomarkers in clinical applications, but their enrichment and detection remain a huge challenge. Herein, inspired by the burr-like structure of the hedgehog, we present a new nanoparticle with a nanoneedle-assembled shell and a magnetic core for the effective capture and detection of exosomes. The unique nanoneedle structures endowed the magnetic nanoparticles with a large surface area for antibody modification so that the nanoparticles could serve as a platform for efficient exosome capture. In addition, the controllable movement of exosome-combined nanoparticles, which is due to the magnetic iron oxide cores, provides tremendous convenience for separating exosomes. The practical value of these nanoparticles in exosome analyses of serum from healthy patients and patients with liver cancer has also been demonstrated. Thus, we believe that bioinspired hierarchical nanoparticles are promising for biomedical and clinical applications.
AbstractTopological spin textures such as magnetic skyrmions have attracted considerable interest due to their potential application in spintronic devices. However, there still remain several challenges to overcome before their practical application, for instance, achieving high scalability and thermal stability. Recent experiments have proposed a new class of skyrmion materials in the Heusler family, Mn1.4Pt0.9Pd0.1Sn and Mn2Rh0.95Ir0.05Sn, which possess noncollinear magnetic structures. Motivated by these experimental results, we suggest another Heusler compound hosted by Mn3Ga to overcome the above limitations. We fabricate Mn3-xPdxGa thin films, focusing on the magnetic compensation point. In Mn2.3Pd0.7Ga, we find a spin-reorientation transition around TSR = 320 K. Below the TSR, we observe the topological Hall effect and a positive magnetic entropy change, which are the hallmarks of a chiral noncollinear spin texture. By integrating all the data, we determine the magnetic phase diagram, displaying a wide chiral noncollinear spin phase even at room temperature. We believe that this compensated ferrimagnet shows promise for opening a new avenue toward chiral spin-based, high-density, and low-power devices.
AbstractFerroelectricity can reduce the subthreshold swing (SS) of metal-oxide-semiconductor field-effect transistors (MOSFETs) to below the room-temperature Boltzmann limit of ~60 mV/dec and provides an important strategy to achieve a steeper SS. Surprisingly, by carefully tuning the polarization switching dynamics of BiFeO3 ferroelectric capacitors the SS of a commercial power MOSFET can even be tuned to zero or a negative value, i.e., the drain current increases with a constant or decreasing gate voltage. In particular, in addition to the positive SS of lower than 60 mV/dec, the zero and negative SS can be established with a drain current spanning for over seven orders of magnitude. These intriguing phenomena are explained by the ferroelectric polarization switching dynamics, which change the charge redistributions and accordingly affect the voltage drops across the ferroelectric capacitor and MOSFET. This study provides deep insights into understanding the steep SS in ferroelectric MOSFETs, which could be promising for designing advanced MOSFETs with an ultralow and tunable SS.
AbstractThe moisture-induced shape memory effect (SME) is one of the most intriguing phenomena of wood, where wood can stably retain a certain deformed shape and, upon moisture sorption, can recover the original shape. Despite the long history of wood utilization, the SME is still not fully understood. Combining molecular dynamics (MD) and finite-element (FE) modeling, a possible mechanism of the SME of wood cell walls is explored, emphasizing the role of interface mechanics, a factor previously overlooked. Interface mechanics extracted from molecular simulations are implemented in different mechanical models solved by FEs, representing three configurations encountered in wood cell walls. These models incorporate moisture-dependent elastic moduli of the matrix and moisture-dependent behavior of the interface. One configuration, denoted as a mechanical hotspot with a fiber–fiber interface, is found to particularly strengthen the SME. Systematic parametric studies reveal that interface mechanics could be the source of shape memory. Notably, upon wetting, the interface is weak and soft, and the material can be easily deformed. Upon drying, the interface becomes strong and stiff, and composite deformation can be locked. When the interface is wetted again and weakened, the previously locked deformation cannot be sustained, and recovery occurs. The elastic energy and topological information stored in the cellulose fiber network is the driving force of the recovery process. This work proposes an interface behaving as a moisture-induced molecular switch.
AbstractThe terahertz (THz)-wave absorption properties in organic-inorganic hybrid perovskite (OHP) materials are investigated with the in-depth development of OHP-based THz applications. In the THz range from 0.5 to 3 THz, OHPs typically show several interesting phonon modes such as transverse, longitudinal, and halogen self-vibrations. To modulate these frequencies, the density changes in defect-incorporated structures and element mixtures were tested and confirmed. In the literature, the origin of phonon modes in OHP materials have been mostly explained. However, we found new phonon vibration modes in formamidinium (FA)-based hybrid perovskite structures. FAPbI3 single crystals, organic–inorganic hybrid perovskites, of the δ-, δ/α-mixed-, and α-phases were prepared. We intriguingly found that the δ/α-mixed-phase exhibited significant THz-wave absorption peaks at 2.0 and 2.2 THz that were not related to any phonon modes from either the δ- or α-phases, although the δ/α-mixed-phase sample was confirmed to be formed by a physical combination of the δ- and α-phases without the creation of any new chemical states. Our theoretical study performed with ab initio calculations provides an explanation for these unusual THz-wave absorption behaviors; they originate from the novel vibration modes excited at the seamless interfaces in the mixed phase of FAPbI3.
AbstractMost studies of the Rashba effect have focused on interfacial Rashba spin–orbit coupling. Recently, bulk Rashba materials have attracted considerable interest owing to their potential to enhance the Rashba spin–orbit torque. By employing a bulk Rashba material, GeTe, as a spin–orbit channel in GeTe/NiFe bilayers, a large field-like spin–orbit torque up to 15.8 mT/(107 A cm−2) is measured. This value is one of the largest reported field-like torques and is attributed to the interfacial spin–orbit coupling being enhanced by the bulk Rashba effect in the GeTe channel. Furthermore, the large field-like torque is maintained even for a 20-nm-thick NiFe layer. This unconventional dependence on the thickness of both the GeTe and NiFe layers cannot be described by conventional theory, but it is believed to stem from the additional bulk Rashba effect-induced term. The large field-like torque over a wide range of ferromagnet thicknesses results in scalable in-plane spin–orbit torque devices. This result calls for a further theoretical study on spin transport in heterostructures, including bulk Rashba materials.