Hydrogels are able to mimic the flexibility of biological tissues or skin, but they still cannot achieve satisfactory strength and toughness, greatly limiting their scope of application. Natural wood can offer inspiration for designing high-strength hydrogels attributed to its anisotropic structure. Herein, we propose an integrated strategy for efficient preparation of ultrastrong hydrogels using a salting-assisted prestretching treatment. The as-prepared poly(vinyl alcohol)/cellulose nanofiber hybrid hydrogels show distinct wood-like anisotropy, including oriented molecular fiber bundles and extended grain size, which endows materials with extraordinarily comprehensive mechanical properties of ultimate breaking strength exceeding 40 MPa, strain approaching 250%, and toughness exceeding 60 MJ·m–3, and outstanding tear resistance. Impressively, the breaking strength and toughness of the reswollen preoriented hydrogels approach 10 MPa and 25 MJ·m–3, respectively. In vitro and in vivo tests demonstrate that the reswollen hydrogels do not affect the growth and viability of the cells, nor do they cause the inflammation or rejection of the mouse tissue, implying extremely low biotoxicity and perfect histocompatibility, showcasing bright prospects for application in artificial ligaments or tendons. The strategy provided in this study can be generalized to a variety of biocompatible polymers for the fabrication of high-performance hydrogels with anisotropic structures.

“Structure subserves function” is one fundamental biological maxim, and so the biological membrane that delimits the regions primarily serves as the margin between life and death for individual cells. Here, an Oswald ripening mechanism-guided solvothermal method was proposed for the synthesis of uniform MnS nanocapsules assembled with metastable γ-MnS nanocrystals. Through designing the physicochemical properties, MnS nanocapsules would disaggregate into small γ-MnS nanocrystals in a tumor acidic environment, with the surface potential switched from negative to positive, thus showing conspicuous delivery performance. More significantly, the specific accumulation of Mn2+ in mitochondria was promoted due to the downregulation of mitochondrial calcium uptake 1 (MICU1) by the formed H2S, thus leading to serious mitochondrial Mn-poisoning for membrane permeability increase and then tumor apoptosis. This study provides a synthesis strategy of metal sulfide nanocapsules and encourages multidisciplinary researchers to focus on ion–cancer crosstalk for the development of an antitumor strategy.

Machine learning (ML) algorithms will be enablers in revolutionizing traditional methods of materials optimization. Here, we broaden the use of ML to assist the construction of Fenton-like single-atom catalysts (SACs) by developing a methodology including model building, training, and prediction. Our approach can efficiently extract synthesis parameters that exert a substantial influence on Fenton activity and accurately predict the phenol degradation rate k of SACs with a mean error of ±0.018 min–1. The extended synthesis window with accelerated learning enables the realization that the heating temperatures during SAC synthesis significantly influence the Fe–N coordination number, which ultimately dictates their performance. Through ML-guided optimization, a highly efficient SAC dominated by Fe–N5 sites with exceptional Fenton activity (k = 0.158 min–1) is identified. Our work provides an example for ML-assisted optimization of single-atom coordination environments and illuminates the feasibility of ML in accelerating the development of high-performance catalysts.

Ferroptosis, as a type of programmed cell death process, enables effective damage to various cancer cells. However, we discovered that persistent oxidative stress during ferroptosis can upregulate the apurinic/apyrimidinic endonuclease 1 (APE1) protein that induces therapeutic resistance (“ferroptosis resistance”), resulting in an unsatisfactory treatment outcome. To address APE1-induced therapeutic resistance, we developed a GSH/APE1 cascade activated therapeutic nanoplatform (GAN). Specifically, the GAN is self-assembled by DNA-functionalized ultrasmall iron oxide nanoparticles and further loaded with drug molecules (drug-GAN). GSH-triggered GAN disassembly can “turn on” the catalysis of GAN to induce efficient lipid peroxidation (LPO) for ferroptosis toward the tumor, which could upregulate APE1 expression. Subsequently, upregulated APE1 can further trigger accurate drug release for overcoming ferroptosis resistance and inducing the recovery of near-infrared fluorescence for imaging the dynamics of APE1. Importantly, adaptive drug release can overcome the adverse effects of APE1 upregulation by boosting intracellular ROS yield and increasing DNA damage, to offset APE1’s functions of antioxidant and DNA repair, thus leading to adaptive ferroptosis. Moreover, with overexpressed GSH and upregulated APE1 in the tumor as stimuli, the therapeutic specificity of ferroptosis toward the tumor is greatly improved, which minimized nonspecific activation of catalysis and excessive drug release in normal tissues. Furthermore, a switchable MRI contrast from negative to positive is in sync with ferroptosis activation, which is beneficial for monitoring the ferroptosis process. Therefore, this adapted imaging and therapeutic nanoplatform can not only deliver GSH/APE1-activated lipid peroxide mediated adaptive synergistic therapy but also provided a switchable MRI/dual-channel fluorescence signal for monitoring ferroptosis activation, drug release, and therapy resistance dynamics in vivo, leading to high-specificity and high-efficiency adaptive ferroptosis therapy.

“Magic-sized” nanocrystals (MSNCs) grow in discrete jumps between a series of specific sizes. Consequently, MSNCs have been explored as an alternative route to uniform semiconductor particles, potentially with atomic precision. However, because the growth mechanism has been poorly understood, the best strategies to control MSNC syntheses and obtain desired sizes are unknown. Experiments have found that common parameters, such as growth time and temperature, have limited utility. Here, we theoretically and experimentally investigate reactant supersaturation as a tool to control MSNC growth. We compare direct synthesis of CdSe MSNCs with ripening of isolated MSNCs or their mixtures. Surprisingly, we find that MSNCs readily synchronize to the same growth trajectory, even starting from distinct initial conditions, explaining the robustness of MSNC growth. Further, by understanding the synchronization mechanism, we demonstrate methods to control the final MSNC size. These results deepen our knowledge of MSNCs and indicate strategies to tailor their growth.

Today’s huge amount of data generation and transfer induced an urgent requirement for long-term data storage. Here, we demonstrate and discuss a concept for long-term storage using NV centers inside nanodiamonds. The approach is based upon the radiation-induced generation of additional vacancies (so-called GR1 states), which quench the initial NV centers, resulting in a reduced overall fluorescence lifetime of the NV center. Using the tailored fluorescence lifetime of the NV center to code the information, we demonstrate a “beyond binary” data storage density per bit. We also demonstrate that this process is reversible by heating the sample or the spot of information. This proof of principle shows that our technique may be a promising alternative data storage technology, especially in terms of long-term storage, due to the high stability of the involved color centers. In addition to the proof-of-principle demonstration using macroscopic samples, we suggest and discuss the usage of focused electron beams to write information in nanodiamond materials, to read it out with focused low-intensity light, and to erase it on the macro-, micro-, or nanoscale.

Integrated, on-chip lasers are vital building blocks in future optoelectronic and nanophotonic circuitry. Specifically, III–V materials that are of technological relevance have attracted considerable attention. However, traditional microcavity laser fabrication techniques, including top-down etching and bottom-up catalytic growth, often result in undesirable cavity geometries with poor scalability and reproducibility. Here, we utilize the selective area epitaxy method to deterministically engineer thousands of microring lasers on a single chip. Specifically, we realize a catalyst-free, epitaxial growth of a technologically critical material, InAsP/InP, in a ring-like cavity with embedded multi-quantum-well heterostructures. We elucidate a detailed growth mechanism and leverage the capability to deterministically control the adatom diffusion lengths on selected crystal facets to reproducibly achieve ultrasmooth cavity sidewalls. The engineered devices exhibit a tunable emission wavelength in the telecommunication O-band and show low-threshold lasing with over 80% device efficacy across the chip. Our work marks a significant milestone toward the implementation of a fully integrated III–V materials platform for next-generation high-density integrated photonic and optoelectronic circuits.

As chondrocytes from osteoarthritic cartilage usually exhibit aging and senescent characteristics, targeting aging chondrocytes could be a potential therapeutic strategy. In this study, exosomes derived from umbilical cord-derived mesenchymal stem cells (UCMSC-EXOs) combined with the chondrocyte-targeting capacity and controlled-release system were proposed for osteoarthritis (OA) treatment via rejuvenating aging chondrocytes. The essential functional miRNAs within UCMSC-EXOs were investigated, with the p53 signaling pathway identified as the key factor. To improve the therapeutic efficiency and retention time of UCMSC-EXOs in vivo, the exosomes (EXOs) were engineered on membranes with a designed chondrocyte-targeting polymers, and encapsulated within thiolated hyaluronic acid microgels to form a “two-phase” releasing system, which synergistically facilitated the repair of OA cartilage in a rat model. Together, this study highlighted the rejuvenating effects of UCMSC-EXOs on OA chondrocytes and the potential to combine with chondrocyte-targeting and sustained-release strategies toward a future cell-free OA treatment.

Digital immunoassays with multiplexed capacity, ultrahigh sensitivity, and broad affordability are urgently required in clinical diagnosis, food safety, and environmental monitoring. In this work, a multidimensional digital immunoassay has been developed through microparticle-based encoding and artificial intelligence-based decoding, enabling multiplexed detection with high sensitivity and convenient operation. The information encoded in the features of microspheres, including their size, number, and color, allows for the simultaneous identification and accurate quantification of multiple targets. Computer vision-based artificial intelligence can analyze the microscopy images for information decoding and output identification results visually. Moreover, the optical microscopy imaging can be well integrated with the microfluidic platform, allowing for encoding-decoding through the computer vision-based artificial intelligence. This microfluidic digital immunoassay can simultaneously analyze multiple inflammatory markers and antibiotics within 30 min with high sensitivity and a broad detection range from pg/mL to μg/mL, which holds great promise as an intelligent bioassay for next-generation multiplexed biosensing.

Exploring the effect of porphin tautomerism on the regioselectivity of its derivatives is a big challenge, which is significant for the development and application of porphyrin drugs. In this work, we demonstrate the regioselectivity of 2H-diphenylporphyrin (H2-DPP) in the planarization reaction on Au(111) and Ag(111) substrates. H2-DPP monomer forms two configurations (anti- and syn-) via a dehydrogenation coupling, between which the yield of the anti-configuration exceeds 90%. Using high-resolution scanning tunneling microscopy, we visualize the reaction processes from the H2-DPP monomer to the final two planar products. Combined with DFT calculations of the potential reaction pathway and comparative experiments on Au(111) and Ag(111) substrates. Using M-DPP (M = Cu and Fe), we confirm that the regioselectivity of H2-DPP is derived from the reaction energy barrier during the cyclodehydrogenation reaction of different tautomers. This work reveals the regioselectivity mechanism of H2-DPP on the atomic scale, which holds great significance for understanding the chemical conversion process of organic macrocyclic molecules.

Incipient soot early in the flame was studied by high-resolution atomic force microscopy and scanning tunneling microscopy to resolve the atomic structure and orbital densities of single soot molecules prepared on bilayer NaCl on Cu(111). We resolved extended catacondensed and pentagonal-ring linked (pentalinked) species indicating how small aromatics cross-link and cyclodehydrogenate to form moderately sized aromatics. In addition, we resolved embedded pentagonal and heptagonal rings in flame aromatics. These nonhexagonal rings suggest simultaneous growth through aromatic cross-linking/cyclodehydrogenation and hydrogen abstraction acetylene addition. Moreover, we observed three classes of open-shell π-radical species. First, radicals with an unpaired π-electron delocalized along the molecule’s perimeter. Second, molecules with partially localized π-electrons at zigzag edges of a π-radical. Third, molecules with strong localization of a π-electron at pentagonal- and methylene-type sites. The third class consists of π-radicals localized enough to enable thermally stable bonds, as well as multiradical species such as diradicals in the open-shell triplet state. These π-diradicals can rapidly cluster through barrierless chain reactions enhanced by van der Waals interactions. These results improve our understanding of soot formation and the products formed by combustion and could provide insights for cleaner combustion and the production of hydrogen without CO2 emissions.

We study the early time carrier drift dynamics in CsPbI3 nanocrystal thin films with a sub 25 ps time resolution. Prior to trapping, carriers exhibit band-like transport characteristics, which is similar to those of traditional semiconductor solar absorbers including Si and GaAs due to optical phonon and carrier scattering at high temperatures. In contrast to the popular polaron scattering mechanism, the CsPbI3 nanocrystal thin film demonstrates the strongest optical phonon scattering mechanism among other inorganic–organic hybrid perovskites, Si, and GaAs. This ultrafast dynamics study establishes a foundation for understanding the fundamental carrier drift properties that drive perovskite nanocrystal optoelectronics.

Inflammatory infiltration and bone destruction are important pathological features of rheumatoid arthritis (RA), which originate from the disturbed niche of macrophages. Here, we identified a niche-disrupting process in RA: due to overactivation of complement, the barrier function of VSIg4+ lining macrophages is disrupted and mediates inflammatory infiltration within the joint, thereby activating excessive osteoclastogenesis and bone resorption. However, complement antagonists have poor biological applications due to superphysiologic dose requirements and inadequate effects on bone resorption. Therefore, we developed a dual-targeted therapeutic nanoplatform based on the MOF framework to achieve bone-targeted delivery of the complement inhibitor CRIg–CD59 and pH-responsive sustained release. The surface-mineralized zoledronic acid (ZA) of ZIF8@CRIg–CD59@HA@ZA targets the skeletal acidic microenvironment in RA, and the sustained release of CRIg–CD59 can recognize and prevent the complement membrane attack complex (MAC) from forming on the surface of healthy cells. Importantly, ZA can inhibit osteoclast-mediated bone resorption, and CRIg–CD59 can promote the repair of the VSIg4+ lining macrophage barrier to achieve sequential niche remodeling. This combination therapy is expected to treat RA by reversing the core pathological process, circumventing the pitfalls of traditional therapy.

Extensive macroscale two-dimensional (2-D) platinum (Pt) nanowire network (NWN) sheets are created through a hierarchical self-assembly process with the aid of biomolecular ligands. The Pt NWN sheet is assembled from the attachment growth of 1.9 nm-sized 0-D nanocrystals into 1-D nanowires featuring a high density of grain boundaries, which then interconnect to form monolayer network structures extending into centimeter-scale size. Further investigation into the formation mechanism reveals that the initial emergence of NWN sheets occurs at the gas/liquid interfaces of the bubbles produced by sodium borohydride (NaBH4) during the synthesis process. Upon the rupture of these bubbles, an exocytosis-like process releases the Pt NWN sheets at the gas/liquid surface, which subsequently merge into a continuous monolayer Pt NWN sheet. The Pt NWN sheets exhibit outstanding oxygen reduction reaction (ORR) activities, with specific and mass activities 12.0 times and 21.2 times greater, respectively, than those of current state-of-the-art commercial Pt/C electrocatalysts.

Graphdiyne (GDY), a rising star of carbon allotropes, features a two-dimensional all-carbon network with the cohybridization of sp and sp2 carbon atoms and represents a trend and research direction in the development of carbon materials. The sp/sp2-hybridized structure of GDY endows it with numerous advantages and advancements in controlled growth, assembly, and performance tuning, and many studies have shown that GDY has been a key material for innovation and development in the fields of catalysis, energy, photoelectric conversion, mode conversion and transformation of electronic devices, detectors, life sciences, etc. In the past ten years, the fundamental scientific issues related to GDY have been understood, showing differences from traditional carbon materials in controlled growth, chemical and physical properties and mechanisms, and attracting extensive attention from many scientists. GDY has gradually developed into one of the frontiers of chemistry and materials science, and has entered the rapid development period, producing large numbers of fundamental and applied research achievements in the fundamental and applied research of carbon materials. For the exploration of frontier scientific concepts and phenomena in carbon science research, there is great potential to promote progress in the fields of energy, catalysis, intelligent information, optoelectronics, and life sciences. In this review, the growth, self-assembly method, aggregation structure, chemical modification, and doping of GDY are shown, and the theoretical calculation and simulation and fundamental properties of GDY are also fully introduced. In particular, the applications of GDY and its formed aggregates in catalysis, energy storage, photoelectronic, biomedicine, environmental science, life science, detectors, and material separation are introduced.

Zn anodes of aqueous Zn metal batteries face challenges from dendrite growth and side reactions. Building Zn(002) texture mitigates the issues but does not eradicate them. Zn(002) still faces severe challenges from corrosive electrolytes and dendrite growth, especially after hundreds of cycles. Therefore, it is necessary to have a passivation layer covering Zn(002). Here, Zn(002) texture and surface coating are achieved on Zn foils by an one-step annealing process, as demonstrated by ZnS, ZnSe, ZnF2, Zn3(PO4)2 (ZPO), etc. Using ZPO as a model, the coupling between surface coating and Zn(002) is illustrated in terms of dendrite-suppressing ability and diffusion energy barrier of Zn2+. The modified Zn foils (Zn(002)@ZPO) exhibit the excellent electrochemical performance, far superior to Zn(002) or ZPO alone. In the full cells, the performance is greatly improved even under harsh conditions, i.e., high areal capacity and limited Zn resource. This work achieves crystal engineering and surface coating on Zn anodes simultaneously and discloses the in-depth insights about the synergy of crystal orientation and passivation layers.

Microrobots are being explored for biomedical applications, such as drug delivery, biological cargo transport, and minimally invasive surgery. However, current efforts largely focus on proof-of-concept studies with nontranslatable materials through a “design-and-apply” approach, limiting the potential for clinical adaptation. While these proof-of-concept studies have been key to advancing microrobot technologies, we believe that the distinguishing capabilities of microrobots will be most readily brought to patient bedsides through a “design-by-problem” approach, which involves focusing on unsolved problems to inform the design of microrobots with practical capabilities. As outlined below, we propose that the clinical translation of microrobots will be accelerated by a judicious choice of target applications, improved delivery considerations, and the rational selection of translation-ready biomaterials, ultimately reducing patient burden and enhancing the efficacy of therapeutic drugs for difficult-to-treat diseases.

Although biodegradable, transient electronic devices must dissolve or decompose via environmental factors, an effective waterproofing or encapsulation system is essential for reliable, durable operation for a desired period of time. Existing protection approaches use multiple or alternate layers of electrically inactive organic/inorganic elements combined with polymers; however, their high mechanical stiffness is not suitable for soft, time-dynamic biological tissues/skins/organs. Here, we introduce a stretchable, bioresorbable encapsulant using nanoparticle-incorporated elastomeric composites with modifications of surface morphology. Nature-inspired micropatterns reduce the diffusion area for water molecules, and embedded nanoparticles impede water permeation, which synergistically enhances the water-barrier performance. Empirical and theoretical evaluations validate the encapsulation mechanisms under strains. Demonstration of a soft, degradable shield with an optical component under a biological solution highlights the potential applicability of the proposed encapsulation strategy.

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast time scale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of the Floquet formalism (which is defined for an infinite periodic drive) through the switching process and to what extent the transient changes can be driven adiabatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the K and K′ valleys in monolayer WS2. With a circularly polarized, red-detuned pump pulse, the degeneracy of the K and K′ excitons can be lifted, and the phase of the coherence rotated. We directly measure phase rotations greater than π during the 100 fs driving pulse and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and the Bloch–Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the nonresonant pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the nonresonant pump pulse we show that there is additional decoherence caused by power broadening in the presence of the nonresonant pump. This nonadiabaticity arises as a result of interactions with the otherwise adiabatic Floquet states and may be a problem for many applications, such as manipulating qubits in quantum information processing; however, these measurements also suggest ways such effects can be minimized or eliminated.

The Chirality Induced Spin Selectivity (CISS) effect describes the capability of chiral molecules to act as spin filters discriminating flowing electrons according to their spin state. Within molecular spintronics, efforts are focused on developing chiral-molecule-based technologies to control the injection and coherence of spin-polarized currents. Herein, for this purpose, we study spin selectivity properties of a monolayer of a thioalkyl derivative of a thia-bridged triarylamine hetero[4]helicene chemisorbed on a gold surface. A stacked device assembled by embedding a monolayer of these molecules between ferromagnetic and diamagnetic electrodes exhibits asymmetric magnetoresistance with inversion of the signal according to the handedness of molecules, in line with the presence of the CISS effect. In addition, magnetically conductive atomic force microscopy reveals efficient electron spin filtering even at unusually low potentials. Our results demonstrate that thia[4]heterohelicenes represent key candidates for the development of chiral spintronic devices.