Advanced Materials

Wireless miniature soft actuators are promising for various potential high‐impact applications in medical, robotic grippers, and artificial muscles. However, these miniature soft actuators are currently constrained by a small output force and low work capacity. To address such challenges, we report a miniature magnetic phase‐change soft composite actuator. This soft actuator exhibits an expanding deformation and enables up to a 70 N output force and 175.2 J/g work capacity under remote magnetic radio frequency heating, which are 106–107 times that of traditional magnetic soft actuators. To demonstrate its capabilities, we first design a wireless soft robotic device that can withstand 0.24 m/s fluid flows in an artery phantom. By integrating it with a thermally‐responsive shape‐memory polymer and bistable metamaterial sleeve, we design a wireless reversible bistable stent towards for future potential angioplasty applications. Moreover, it can additionally locomote inside and jump out of granular media. At last, the phase‐change actuator can realize programmable bending deformations when a specifically designed magnetization profile is encoded, enhancing its shape‐programming capability. Such a miniature soft actuator provides an approach to enhance the mechanical output and versatility of magnetic soft robots and devices, extending their medical and other potential applications. This article is protected by copyright. All rights reserved

Chiral metasurfaces can exhibit a strong circular dichroism, but it is limited by the complicated fabrication procedure and alignment errors. Here, we demonstrate a new type of self‐aligned suspended chiral bilayer metasurface with only one‐step electron beam lithography exposure. A significant optical chirality of 221°/μm can be realized using suspended metasurfaces with a thickness of 100 nm. Furthermore, we experimentally demonstrate that such a structure is capable of label‐free discrimination of the chiral molecules at zeptomole level, exhibiting a much higher sensitivity (orders of magnitude) compared to the conventional circular dichroism spectroscopy. The fundamental principles for chiral sensing using molecules‒metasurfaces interactions have been explored. Benefiting from the giant chiroptical response, our proposed meta‐device may offer promising applications for ultrathin circular polarizers, chiral molecular detectors, and asymmetry information processing. This article is protected by copyright. All rights reserved

Growth of Cu(In,Ga)Se2 (CIGS) absorbers under Cu‐poor conditions gives rise to incorporation of numerous defects into the bulk, whereas the same absorber grown under Cu‐rich conditions leads to a stoichiometric bulk with minimum defects. This suggests that CIGS absorbers grown under Cu‐rich conditions are more suitable for solar cell applications. However, the CIGS solar cell devices with record efficiencies have all been fabricated under Cu‐poor conditions, despite the expectations. Therefore, in the present work, we investigate both Cu‐poor and Cu‐rich CIGS cells and show that the superior properties of internal interfaces of Cu‐poor CIGS cells, such as p‐n junction and grain boundaries, makes them always the record‐efficiency devices. More precisely, by employing a correlative microscopy approach, we discover for the first time the typical fingerprints for superior properties of internal interfaces necessary for maintaining a lower recombination activity in the cell. These are a Cu‐depleted and Cd‐enriched CIGS absorber surface near the p‐n junction and the negative Cu factor (∆β) and high Na content (> 1.5 at.%) at the grain boundaries. Thus, this work provides key factors governing the device performance (efficiency), which can be considered in the design of next‐generation solar cells. This article is protected by copyright. All rights reserved

Ga2O3 and its polymorphs are attracting increasing attention. The rich structural space of polymorphic oxide systems such as Ga2O3 offers potential for electronic structure engineering, which is of particular interest for a range of applications, such as power electronics. γ‐Ga2O3 presents a particular challenge across synthesis, characterisation, and theory due to its inherent disorder and resulting complex structure – electronic structure relationship. Here, density functional theory is used in combination with a machine learning approach to screen nearly one million potential structures, thereby developing a robust atomistic model of the γ‐phase. Theoretical results are compared with surface and bulk sensitive soft and hard X‐ray photoelectron spectroscopy, X‐ray absorption spectroscopy, spectroscopic ellipsometry, and photoluminescence excitation spectroscopy experiments representative of the occupied and unoccupied states of γ‐Ga2O3. The first onset of strong absorption at room temperature is found at 5.1 eV from spectroscopic ellipsometry, which agrees well with the excitation maximum at 5.17 eV obtained by PLE spectroscopy, where the latter shifts to 5.33 eV at 5 K. This work presents a leap forward in the treatment of complex, disordered oxides and is a crucial step towards exploring how their electronic structure can be understood in terms of local coordination and overall structure. This article is protected by copyright. All rights reserved

Noncovalent macrocycle‐confined supramolecular purely organic room‐temperature phosphorescence (RTP) is the current research hotspot. Herein, we report a high‐efficiency noncovalent polymerization activated near‐infrared (NIR) emissive RTP‐harvesting system in aqueous solution based on the stepwise confinement of cucurbit[7]uril (CB[7]) and β‐cyclodextrin grafted hyaluronic acid (HACD). Compared with dodecyl chain bridged 6‐bromoisoquinoline derivative (G), the dumbbell‐shaped assembly G⊂CB[7] presents an appeared complexation‐induced RTP signal at 540 nm via the first confinement of CB[7]. Subsequently, benefitting from the stepwise confinement encapsulation of β‐cyclodextrin cavity, the subsequent noncovalent polymerization of the binary G⊂CB[7] assembly enabled by HACD can contribute to the further enhanced RTP emission intensity approximately 8 times in addition to an increased lifetime from 59.0 µs to 0.581 ms. Moreover, upon doping a small amount of two types of organic dyes, Nile blue (NiB) or Tetrakis(4‐sulfophenyl)porphyrin (TPPSS) as an acceptor into the supramolecular confinement assembly G⊂CB[7]@HACD, efficient RTP energy transfer occurs accompanied by a long‐lived NIR emitting performance (680, 710 nm) with a high donor/acceptor ratio. Intriguingly, the prepared RTP‐harvesting system is successfully applied for targeted NIR imaging of living tumor cells by utilizing the targeting ability of hyaluronic acid, which provides a new strategy to create advanced water‐soluble NIR phosphorescent materials. This article is protected by copyright. All rights reserved

Singlet fission is commonly defined as the generation of two triplet excitons from a single absorbed photon. However, ambiguities within this definition arise due to the complexity of the various double triplet states that exist in SF chromophores and corresponding interconversion processes. To clarify this process, singlet fission is frequently depicted as sequential two‐step conversion in which a singlet exciton decays into a bound triplet pair biexciton state which dissociates into two “free” triplet excitons. However, this model discounts the potential for direct harvesting from the coupled biexciton state. Here, we demonstrate that individual triplet excitons can be extracted directly from a bound triplet pair. We demonstrate that due to the requirement for geminate triplet‐triplet annihilation in intramolecular singlet fission compounds, unique spectral and kinetic signatures can be used to quantify triplet pair harvesting yields. We achieve an internal quantum efficiency for triplet exciton transfer from the triplet pair of greater than 50%, limited only by the solubility of the compounds. The harvesting process is not dependent on the net multiplicity of the triplet pair state, suggesting that an explicit, independent dissociation step is not a requirement for using triplet pairs to do chemical or electrical work. This article is protected by copyright. All rights reserved

Auditory sensors have shortcomings with respect to not only personalization with wearability and portability but also detecting a human voice clearly in a noisy environment or when a mask covers the mouth. In this work, we exploited an electret‐powered and hole patterned polymer diaphragm into a skin‐attachable auditory sensor for the first time. The optimized charged electret diaphragm induces a voltage bias of >400 V against the counter electrode, which reduces the necessity of a bulky power source and enables the capacitive sensor to show high sensitivity (2.2 V/Pa) with incorporation of an elastomer nanodroplet seismic mass. The sophisticated capacitive structure with low mechanical damping enabled a flat frequency response (80–3000 Hz) and good linearity (50–80 dBSPL). The hole‐patterned electret diaphragms help our skin‐attachable sensor detect only neck‐skin vibration rather than dynamic air pressure, enabling a person's voice to be detected in a harsh acoustic environment. The sensor operated reliably even in the presence of surrounding noise and when the user was wearing a gas mask. Therefore, our sensor shows strong potential of a communication tool for disaster response and quarantine activities, and of diagnosis tool for vocal healthcare applications such as cough monitoring and voice dosimetry. This article is protected by copyright. All rights reserved

During cerebral ischemia‐reperfusion (I‐R) injury, the infiltration of monocyte/macrophages (Mo/Mφ) into the ischemic penumbra causes inflammatory damage but also regulates tissue repair in the penumbra. The regulation and balance of Mo/Mφ polarization has been considered as a potential therapeutic target for treating cerebral I‐R injury. Herein, our findings demonstrated that glabridin (Gla)‐loaded nanoparticles (i.e., NPGla‐5k) could effectively inhibit M1‐polarization and enhance M2‐polarization of Mo/Mφ. Positron emission tomography (PET) imaging showed that NPGla‐5k could selectively accumulate in the spleen following intravenous injection. Spleen‐targeted Cy5‐NPGla‐5k can colocalize with peripheral macrophages in the penumbra at 24 h after tail vein injection. Interestingly, NPGla‐5k treatment could reduce inflammatory damage, protect dying neurons and improve nervous system function. The protective effect of spleen‐targeted NPGla‐5k against cerebral I‐R injury in mice encourages an exploration of their use for clinical treatment of patients with cerebral I‐R injury. This article is protected by copyright. All rights reserved

Room‐temperature‐operating highly sensitive mid‐wave infrared (MWIR) photodetectors are utilized in a large number of important applications including night vision, communications, and optical radar. Many previous studies have demonstrated uncooled MWIR photodetectors using two‐dimentional narrow‐bandgap semiconductors. To date, most of these works utilize atomically thin flakes, simple van der Waals (vdW) heterostructures, or atomically thin p‐n junctions as absorbers, which have difficulty meeting the requirements for state‐of‐the‐art MWIR photodetectors with a blackbody response. Here, we report a fully depleted self‐aligned MoS2‐BP‐MoS2 vdW heterostructure sandwiched between two electrodes. This new type of photodetector exhibits competitive performance, including a high blackbody peak photoresponsivity up to 0.77 A/W and low noise‐equivalent power of 2.0 × 10−14 W/Hz1/2, in the MWIR region. A peak specific detectivity of 8.61 × 1010 cmHz1/2/W under blackbody radiation was achieved at room temperature in the MWIR region. Importantly, the effective detection range of our device is twice that of state‐of‐the‐art MWIR photodetectors. Furthermore, the device presents an ultra‐fast response of ∼4 μs both in the visible and short‐wavelength infrared bands. These results provide an ideal platform for realizing broadband and highly sensitive room‐temperature MWIR photodetectors. This article is protected by copyright. All rights reserved

Metal‐organic frameworks (MOFs) are hybrid porous crystalline networks with tunable chemical and structural properties. However, their excellent potential is limited in practical applications due to their hard‐to‐shape powder form, making it challenging to assemble MOFs into macroscopic composites with mechanical integrity. While a binder matrix enables hybrid materials, such materials have a limited MOF content and thus limited functionality. To overcome this challenge, nanoMOFs are combined with tailored same‐charge high‐aspect‐ratio cellulose nanofibrils (CNFs) to manufacture robust, wet‐stable, and multifunctional MOF‐based aerogels with 90 wt% nanoMOF loading. The porous aerogel architectures show excellent potential for practical applications such as efficient water purification, CO2 and CH4 gas adsorption and separation, and fire‐safe insulation. Moreover, a one‐step carbonization process enables these aerogels as effective structural energy‐storage electrodes. This work exhibits the unique ability of high‐aspect‐ratio CNFs to bind large amounts of nanoMOFs in structured materials with outstanding mechanical integrity – a quality that is preserved even after carbonization. The demonstrated process is simple and fully discloses the intrinsic potential of the nanoMOFs, resulting in synergetic properties not found in the components alone, thus paving the way for MOFs in macroscopic multifunctional composites. This article is protected by copyright. All rights reserved

Here, we propose a new theoretical framework that enables the use of Differential Dynamic Microscopy (DDM) in fluorescence imaging mode to quantify in situ protein adsorption onto nanoparticles (NP) while simultaneously monitoring for NP aggregation. We use this methodology to elucidate the thermodynamic and kinetic properties of the protein corona (PC) in vitro and in vivo. Our results show that protein adsorption triggers particle aggregation over a wide concentration range and that the formed aggregate structures can be quantified using the proposed methodology. Protein affinity for polystyrene (PS) NPs was observed to be dependent on particle concentration. For complex protein mixtures, our methodology identifies that the PC composition changes with the dilution of serum proteins, demonstrating a Vroman effect never quantitatively assessed in situ on NPs. Finally, DDM allows monitoring of the evolution of the PC in vivo. Our results show that the PC composition evolves significantly over time in zebrafish larvae, confirming the inherently dynamic nature of the PC. The performance of the developed methodology allowed to obtain quantitative insights into nano‐bio interactions in a vast array of physiologically relevant conditions that will serve to further improve the design of nanomedicine. This article is protected by copyright. All rights reserved

Nanostructure engineering is a key strategy for tailoring properties in the fields of batteries, solar cells, thermoelectrics, and so on. Limited by grain coarsening, however, the nanostructure effect gradually degrades during the materials’ manufacturing and in‐service period. Herein, we develop a strategy of cleavage‐fracture for grain shrinking in the Pb0.98Sb0.02Te sample during the sintering, and the grain size remains stable after repeated tests. Moreover, the initial grain boundary is filled by fractured slender grains and enriched by dislocations, evolving into a hierarchical grain‐boundary structure. The lattice thermal conductivity (κlat) is greatly reduced to approach the amorphous limit. As a result, a record‐high ZT value of about 1.9 is obtained at 815 K in the n‐type Pb0.98Sb0.02Te sample and a decent efficiency of 6.7% in thermoelectric device. This strategy for grain shrinking will shed light on the application of nanostructure engineering under high temperature and extreme conditions in other material systems. This article is protected by copyright. All rights reserved

A scalable synthetic route to colloidal atoms has significantly advanced over the past two decades. Recently, colloidal clusters with DNA‐coated cores called “patchy colloidal clusters” have been developed, providing a directional bonding with specific angle of rotation due to the shape complementarity between colloidal clusters. Through a DNA‐mediated interlocking process, they were directly assembled into low‐coordination colloidal structures, such as cubic diamond lattices. This review details the significant progress in recent years in the synthesis of patchy colloidal clusters and their assembly in experiments and simulations. Furthermore, an outlook is given on the emerging approaches to the patchy colloidal clusters and their potential applications in photonic crystals, metamaterials, topological photonic insulators, and separation membranes. This article is protected by copyright. All rights reserved

The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice-mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain-driven control of hierarchical domain structures in Pb1-x Srx TiO3 solid solution thin films wherein two types, c/a and a1 /a2 , of nanodomains can coexist. Combining phase-field simulations, epitaxial thin-film growth, and detailed structural, domain, and physical-property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet-like a1 /a2 domains in a c/a domain matrix, to a connected-labyrinth geometry of c/a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet-like c/a domains in an a1 /a2 domain matrix. A relationship between the different mixed-phase modulation patterns and its topological nature is established. Annealing the connected-labyrinth structure leads to domain coarsening forming distinctive regions of parallel c/a and a1 /a2 domain stripes, offering additional design flexibility. Finally, it is found that the connected-labyrinth domain patterns exhibit the highest dielectric permittivity. This article is protected by copyright. All rights reserved.

Titanium dioxide (TiO2) nanocrystals have attracted great attention in heterogeneous photocatalysis and photoelectricity fields for decades. However, contradictious conclusions on the reporting of crystallographic orientation and exposed facets of TiO2 nanocrystals frequently appeared in the literature. Herein, using anatase TiO2 nanocrystals with highly exposed {001} facets as a model, we clarified the misleading conclusions that exist on anatase nanocrystals. Although the TiO2‐001 nanocrystals are recognized to be dominated by {001} facets, in fact, anatase nanocrystals with both dominating {001} and {111} facets are always co‐existing due to the similarities in lattice fringes and intersection angles between two types of facets (0.38 nm and 90° in [001] direction, 0.35 nm and 82° in [111] direction). We also give a paradigm for determining the crystallographic orientation and exposed facets based on transmission electron microscope (TEM) analysis, which provides a universal methodology to nanomaterials for determining the orientation and exposed facets. This article is protected by copyright. All rights reserved

With recent advances in interactive displays, the development of a stand‐alone interactive display with no electrical interconnection is of great interest. Here, we present a wireless stand‐alone interactive display (WiSID), enabled by direct capacitive coupling, consisting of three layers: two in‐plane metal electrodes separated by a gap, a composite layer for field‐induced electroluminescence (EL) and inverse piezoelectric sound, and a stimuli‐responsive layer, from bottom to top. Alternating current (AC) power necessary for field‐induced EL and inverse piezoelectric sound is wirelessly transferred from a power unit, with two in‐plane electrodes remotely separated from the WiSID. The unique in‐plane power transfer through the stimuli‐sensitive polar bridge allows stand‐alone operation of the WiSID, making it suitable for the wireless dynamic monitoring of medical fluids. Moreover, we demonstrate a haptic wireless stand‐alone trimodal interactive display mounted on a human finger, whereby touch is wirelessly displayed in various outputs of EL, inverse piezoelectric sound, and tactile vibration, making it suitable for a wireless three‐mode smart braille display. This article is protected by copyright. All rights reserved

Poor electronic and ionic conductivities of covalent organic frameworks (COFs) severely restrict the development of COF‐based electrodes for practical rechargeable batteries, therefore inspiring more research interests from the direction of both material synthesis and technology. Herein, a dual‐porous COF, USTB‐6, with good crystallinity and rich redox‐active sites has been conceived and reticulated by the polymerization of 2,3,8,9,14,15‐hexa(4‐formylphenyl)diquinoxalino [2,3‐a:2,3‐c]phenazine and 2,7‐diaminopyrene‐4,5,9,10‐tetraone. In particular, the graphene‐participated heterogeneous polymerization of the same starting materials affords the uniformly dispersed COF nanosheets with the thickness of 8.3 nm on the conductive carbon substrate, effectively enhancing the electronic conductivity of COF‐based electrode. Such graphene‐supported USTB‐6 nanosheets cathode used in lithium‐ion battery exhibits a specific capacity of 285 mA h g−1 at current density of 0.2 C and excellent rate performance with the still prominent capacity of 188 mA h g−1 at 10 C. More importantly, a capacity of 170 mA h g−1 is retained by USTB‐6 nanosheets cathode after 6000 cycles change and discharge measurement at 5 C. This article is protected by copyright. All rights reserved

Precise arrangements of plasmonic nanoparticles on substrates are important for designing optoelectronics, sensors, and metamaterials with rational electronic, optical, and magnetic properties. Bottom‐up synthesis offers unmatched control over morphology and optical response of individual plasmonic building blocks. Usually, the incorporation of nanoparticles made by bottom‐up wet chemistry starts from batch synthesis of colloids, which requires time‐consuming and hard‐to‐scale steps like ligand exchange and self‐assembly. Herein, we develop an unconventional bottom‐up wet‐chemical synthetic approach for producing gold nanoparticle ordered arrays. Water‐processable hydroxypropyl cellulose stencils facilitate the patterning of a reductant chemical ink on which nanoparticle growth selectively occurs. Arrays exhibiting lattice plasmon resonances in the visible region and near infrared (quality factors >20) were produced following a rapid synthetic step (<10 min), all without cleanroom fabrication, specialized equipment, or self‐assembly, constituting a major step forward establishing in situ growth approaches. We further demonstrate the technical capabilities of this method through modulation of the particle size, shape, and array spacings directly on the substrate. Ultimately, establishing a fundamental understanding of in situ growth has the potential to inform the fabrication of plasmonic materials, opening the door for in situ growth fabrication of waveguides, lasing platforms, and plasmonic sensors. This article is protected by copyright. All rights reserved

In cancer radiotherapy, the lack of fixed DNA damages by oxygen in hypoxic microenvironment of solid tumors often lead to severe radioresistance. Nitric oxide (NO) is a potent radiosensitizer that acts in two ways. It can directly react with the radical DNA thus fixes the damage. It also normalizes the abnormal tumor vessels, thereby increasing blood perfusion and oxygen supply. To achieve these functions, the dosage and duration of NO treatment need to be carefully controlled, otherwise it would lead to the exact opposite outcomes. However, a delivery method that fulfills both requirements is still lacking. We designed a NO depot for the control of NO releasing both over quantity and duration for hypoxic tumor vessel normalization and radiosensitization. In B16 tumor‐bearing mice, the depot could provide low dosage NO continuously and release large amount of NO immediately before irradiation for a short period of time. These two modes of treatment worked in synergy to reverse the radioresistance of B16 tumor more efficiently than releasing at single dosage. This article is protected by copyright. All rights reserved

Halogen vacancies are of great concern in blue‐emitting perovskite quantum dot light‐emitting diodes because they affect their efficiency and spectral shift. Here, the enriched‐bromine surface state is realised using a facile strategy that employs a PbBr2 stock solution for anion exchange based on Cd‐doped perovskite quantum dots. We find that the doped Cd ions are expected to reduce the formation energy of halogen vacancies filled by the external bromine ions, and the excess free bromine ions in solution are enriched in the surface by anchoring with halogen vacancies as sites, accompanied with the shedding of surface long‐chain ligands during the anion exchange process, resulting in a Br‐rich and “neat” surface. Moreover, the surface state exhibits good passivation of the surface defects of the controlled perovskite QDs and simultaneously increases the exciton binding energy, leading to excellent optical properties and stability. Finally, the sky‐blue emitting perovskite QLEDs (490 nm) are conducted with a record external quantum efficiency of 14.6% and current efficiency of 19.9 cd/A. Meanwhile, the electroluminescence spectra exhibit great stability with negligible shifts under a constant operating voltage from 3 to 7 V. This strategy paves the way for improving the efficiency and stability of perovskite QLEDs. This article is protected by copyright. All rights reserved

Perovskite quantum dots (PQDs) emerge as competitive optoelectronic materials for photovoltaic applications due to their ideal bandgap energy, high defect tolerance and solution processability. However, the highly dynamic surface and unperfect cubic structure of PQDs generally result in unfavorable charge carrier transport within the PQD solids and serious nonradiative recombination. Herein, the highly orientated PQD solid is demonstrated using precursor engineering accompanied by a chemical stripping treatment (CST). A combination of systematically experimental studies and theoretical calculations is conducted to fundamentally understand the resurfacing of PQDs using the CST approach. The results reveal that highly ordered PQDs could result in a high orientation of PQD solids, significantly promoting the charge carrier transport within the PQD solids. Meanwhile, the ideal cubic‐structured PQD with an iodine‐rich surface dramatically decreases surface trap states, thereby substantially diminishing trap‐assisted nonradiative recombination. Consequently, the inorganic PQD solar cell (PQDSC) delivers a power conversion efficiency of up to 16.25%. This work provides a feasible avenue to construct highly orientated PQD solids with improved photophysical properties for high‐performance optoelectronic devices. This article is protected by copyright. All rights reserved

Advanced cathode materials play an important role in promoting aqueous battery technology for safe energy storage. Transition metal double hydroxides are usually elusive as a stable cathode for aqueous zinc ion batteries (AZIBs) due to their unstable crystal structure, sluggish ion transportation and insufficient active sites for zinc ion storage. Here we report a trinary layered double hydroxide with hydrogen vacancies (Ni3Mn0.7Fe0.3‐LDH) as a new cathode material for AZIBs. A reversible high capacity up to 328 mAh g−1 can be obtained and cycle stably over 500 cycles with a capacity retention of 85%. Experimental and theoretical studies reveal that the hydrogen vacancies in LDH could expose lattice oxygen atoms as active sites for zinc ion storage and accelerate ion diffusion by reducing the electrostatic interactions between zinc ions and the host structure. Besides, the synergy of trinary transitional metal cations can suppress the Jahn‐Teller distortion of manganese (III) oxide octahedron and enable long cycle stability. This work provides not only a series of high performance cathode materials for aqueous zinc ion batteries but also a novel materials design strategy that can be extended to other multi‐valence metal ion batteries. This article is protected by copyright. All rights reserved

The material's properties of biological tissues are unique. Nature is able to spatially and temporally manipulate (mechanical) properties while maintaining responsiveness towards a variety of cues; all without majorly changing the material's composition. Artificial mimics, synthetic or biomaterial‐based are far less advanced and poorly reproduce the natural cell microenvironment. A viable strategy to generate materials with advanced properties combines different materials into nanocomposites. This work describes nanocomposites of a synthetic fibrous hydrogel, based on polyisocyanides (PIC), that is noncovalently linked to a responsive crosslinker. The introduction of the crosslinker transforms the PIC gel from a static fibrous extracellular matrix mimic to a highly dynamic material that maintains biocompatibility, as demonstrated by in situ modification of the (non)linear mechanical properties and efficient self‐healing properties. Key in the materials design is crosslinking at the fibrillar level using nanoparticles, which, simultaneously may be used to introduce more advanced properties. This article is protected by copyright. All rights reserved

Although aqueous Zn batteries have become a more sustainable alternative to lithium‐ion batteries owing to their intrinsic security, their practical applications are limited by dendrite formation and hydrogen reactions. We present the first application of a rare earth metal type addition to Zn batteries, cerium chloride (CeCl3), as an effective, low‐cost, and green electrolyte additive that facilitates the formation of dynamic electrostatic shielding layer around the Zn protuberance to induce the uniform Zn deposition. After introducing CeCl3 additives, the electrochemical characterizations, in‐situ optical microscopy observation, in‐situ differential electrochemical mass spectrometry, along with density functional theory calculations and finite element method simulations reveal resisted Zn dendritic growth and enhanced electrolyte stability. As a result, the Zn‐Zn cells using CeCl3 additive exhibit a long cycling stability of 2600 h at 2 mA cm–2, an impressive cumulative areal capacity of 3.6 Ah cm–2 at 40 mA cm–2 and a high coulombic efficiency of ∼99.7%. The fact that the Zn‐LiFePO4 cells with proposed electrolyte retain capacity significantly better than the additive‐free case is even more exciting. This article is protected by copyright. All rights reserved

Polymers are usually considered thermal insulators; however, significant enhancements in thermal conductivity (k) have been observed in oriented fibers and films. Despite being advantageous in real‐world applications, extending the linear thermal‐transport advantage of polymers into the three‐dimensional space in bulk materials is still limited due to the spatially interfacial phonon‐conduction barriers. Herein, inspired by the structure of tropocollagen, we discovered that weaving hierarchically arranged poly(p‐phenylene benzobisoxazole) (PBO) fibers with a spiral configuration into an epoxy matrix can yield a three‐dimensionally continuous thermal pathway. This achieves both a through‐plane k of 10.85 W/m K and an in‐plane k of 7.15 W/m K. Theoretical molecular simulations in combination with classical nonlinear modeling attribute the above spatially thermally conductive achievement to not only the hierarchical molecular, spiral and weaving structure of PBO, but also the noncrystalline chains that carry overlapping phonon density of states, thus thermally bridging adjacent high‐k crystals in the PBO fiber. Consequently, the interfacial thermal resistance among high‐k PBO crystals is suppressed to be on the order of 10–10 m2 K/W in both the through‐plane and in‐plane directions. Other advantages include being lightweight, mechanically strong, flexible, and non‐combustible. This material creates opportunities for organic polymers in high‐performance thermal management applications. This article is protected by copyright. All rights reserved

As the world steps into the era of Internet of Things (IoT), numerous miniaturized electronic devices requiring autonomous micropower sources will be connected to the internet. All‐solid‐state thin‐film lithium/lithium‐ion microbatteries (TFBs) combining solid‐state battery architecture and thin‐film manufacturing are regarded as ideal on‐chip power sources for IoT‐enabled microelectronic devices. However, unlike commercialized lithium‐ion batteries, TFBs are still in the immature state, and new advances in materials, manufacturing, and structure are required to improve their performance. In this review, we discuss the current status and existing challenges of TFBs for practical application in internet‐connected devices for the IoT. Recent progress in thin‐film deposition, electrode and electrolyte materials, interface modification, and 3D architecture design is comprehensively summarized and discussed, with emphasis on state‐of‐the‐art strategies to improve the areal capacity and cycling stability of TFBs. Moreover, to be suitable power sources for IoT devices, the design of next‐generation TFBs should consider multiple functionalities, including wide working temperature range, good flexibility, high transparency, and integration with energy‐harvesting systems. Perspectives on designing practically accessible TFBs are provided, which may guide the future development of reliable power sources for IoT devices . This article is protected by copyright. All rights reserved

In recent years, traditional antibiotic efficacy has rapidly diminished due to the advent of multidrug‐resistant (MDR) bacteria which pose severe threats to human life and globalized healthcare. Currently, the development cycle of new antibiotics cannot match the ongoing MDR infection crisis. Therefore, novel strategies are required to resensitize MDR bacteria to existing antibiotics. In this study, novel cationic polysaccharide conjugates Dextran‐graft‐Poly(5‐(1,2‐dithiolan‐3‐yl)‐N‐(2‐guanidinoethyl)pentanamide) (Dex‐g‐PSSn) were synthesized using disulfide exchange polymerization. Critically, bacterial membranes and efflux pumps were disrupted by a sub‐inhibitory concentration of Dex‐g‐PSS30, which enhanced rifampicin (RIF) accumulation inside bacteria and restored its efficacy. Combined Dex‐g‐PSS30 and RIF prevented bacterial resistance in bacteria cultured over 30 generations. Furthermore, Dex‐g‐PSS30 restored RIF effectiveness, reduced inflammatory reactions in a pneumonia‐induced mouse model, and exhibited excellent in vivo biological absorption and degradation capabilities. As an antibiotic adjuvant, Dex‐g‐PSS30 provides a novel resensitizing strategy for RIF against MDR bacteria and bacterial resistance. Our Dex‐g‐PSS30 research provides a solid platform for future MDR applications. This article is protected by copyright. All rights reserved

Hydrogen spillover has emerged to upgrade hydrogen evolution reaction (HER) activity of Pt‐support electrocatalysts, but it is not applicable to the deprotonated oxygen evolution reaction (OER). Non‐precious catalysts that can perform well in both hydrogen spillover and deprotonation are extremely desirable for sustainable hydrogen economy. Herein, an affordable MoS2/NiPS3 vertical heterostructure catalyst is presented to synergize hydrogen spillover and deprotonation for efficient water electrolysis. Internal polarization field (IPF) is clarified as the driving force nature of hydrogen spillover in HER electrocatalysis. The hydrogen spillover from MoS2 edge to NiPS3 can activate the NiPS3 basal plane to boost the HER activity of MoS2/NiPS3 heterostructure (112 mV versus RHE at 10 mA cm–2). While for OER, the IPF in the heterostructure can facilitate the hydroxyl diffusion and render the NiPS3‐to‐MoS2/P‐to‐S dual‐pathways for deprotonation. Resultantly, the stacking of OER‐inactive MoS2 on the NiPS3 surface still brings intriguing OER enhancements. Serving them as electrode couples, the overall water splitting is attested stably with a cell voltage of 1.64 V at 10 mA cm–2. This research puts forward IPF as the criterion in the rational design of hydrogen spillover/deprotonation‐unified non‐precious catalysts for efficient water electrolysis. This article is protected by copyright. All rights reserved

Resource‐abundant metal (e.g., zinc) batteries feature intrinsic advantages of safety and sustainability. Their practical feasibility, however, is impeded by the poor reversibility of metal anode, typically caused by the uncontrollable dendrite enlargement. Significant effort has been exerted to completely prevent dendrites from forming, but this seems less effective at high current densities. Herein, we present an alternative dendrite regulation strategy of forming tiny, homogeneously distributed, and identical zinc dendrites by facet matching, which effectively avoids undesirable dendrite enlargement. Confirmed by multiscale theoretical screening and characterization, the regularly exposed Cu(111) facets at the ridges of a copper nanowire are capable of such dendrite regulation by forming a low‐mismatched Zn(002)/Cu(111) interface. Consequently, reversible zinc electroplating/stripping has been achieved at an unprecedentedly high rate of 100 mA cm−2 for over 30,000 cycles, corresponding to an accumulative areal capacity up to 30 Ah cm−2. A full cell using this anode shows a high capacity of 308.3 mAh g−1 and a high capacity retention of 91.4% after 800 cycles. This strategy is also viable for magnesium and aluminum anodes, thus opening up a promising and universal avenue towards long life and high rate metal anodes. This article is protected by copyright. All rights reserved

Zinc‐ion capacitors (ZICs) is promising technology for large‐scale energy storage by integrating the attributes of supercapacitors and zinc‐ion batteries. Unfortunately, the insufficient Zn2+ storage active sites of carbonaceous cathode materials and the mismatch of pore sizes with charge carriers led to unsatisfactory Zn2+ storage capability. Herein, we report new insights for boosting Zn2+ storage capability of activated nitrogen‐doped hierarchical porous carbon materials (ANHPC‐x) by effectively eliminating micropore confinement effect and synchronously elevate the utilization of active sites. Therefore, the best‐performed ANHPC‐2 delivers impressive electrochemical properties for ZICs in terms of excellent capacity (199.1 mAh g−1), energy density (155.2 Wh kg−1), and durability (65000 cycles). Systematic ex situ characterizations together with in situ electrochemical quartz crystal microbalance and Raman spectra measurements manifest that the remarkable electrochemical performance is assigned to the synergism of Zn2+, H+, and SO42− co‐adsorption mechanism and reversible chemical adsorption. Furthermore, the ANHPC‐2‐based quasi‐solid‐state ZIC demonstrates excellent electrochemical capability with ultralong lifespan up to 100 000 cycles. This work not only provides a promising strategy to improve the Zn2+ storage capability of carbonaceous materials but also sheds lights on charge storge mechanism and advanced electrode materials design for ZICs toward practical applications. This article is protected by copyright. All rights reserved

Rechargeable sodium ion micro‐batteries (NIMBs) constructed using low‐cost and abundant raw materials in planar configuration with both cathode and anode on the same substrate, hold promises for powering coplanar microelectronics, but are hindered by the low areal capacity owing to thin microelectrodes. Here, a prototype of planar and flexible 3D‐printed NIMBs is demonstrated with three‐dimensionally interconnected conductive thick microelectrodes for ultrahigh areal capacity and boosted rate capability. Rationally optimized 3D printable inks with appropriate viscosities and high conductivity allowed the multi‐layer printing of NIMB electrodes reaching a very high thickness of ∼1200 μm while maintaining effective ion and electron transfer pathways in them. Consequently, the 3D‐printed NIMBs deliver superior areal capacity of 4.5 mAh cm–2 (2 mA cm–2), outperforming the state‐of‐the‐art printed micro‐batteries. The NIMBs showed enhanced rate capability with 3.6 mAh cm–2 at 40 mA cm–2 and robust long‐term cycle life up to 6000 cycles. Furthermore, the planar NIMB microelectrodes despite the large thickness exhibit decent mechanical flexibility under various bending conditions. This work opens a new avenue for construction of high‐performance NIMBs with thick microelectrodes capable of powering flexible microelectronics. This article is protected by copyright. All rights reserved

We report a new type of an atomically thin synaptic network on van der Waals (vdW) heterostructures, where each ultra‐small cell (∼ 2 nm thick) built with trilayer WS2 semiconductor acts as a gate‐tunable photoactive synapse, i.e., a photo‐memtransistor. A train of ultraviolet (UV) pulses onto the WS2 memristor generates dopants in atomic‐level precision by direct light‐lattice interactions, along with the gate‐tunability, leading to the accurate modulation of the channel conductance for potentiation and depression of the synaptic cells. Such synaptic dynamics can be explained by a parallel atomistic resistor network model. In addition, we show that such device scheme can generally be realized in other two‐dimensional vdW semiconductors, such as MoS2, MoSe2, MoTe2 and WSe2. Demonstration of our atomically thin photo‐memtransistor arrays, where the synaptic weights can be tuned for the atomistic defect density, provides implications for a new type of artificial neural networks for parallel matrix computations with an ultra‐high integration density. This article is protected by copyright. All rights reserved

Recently, ferromagnetic heterostructure spintronic terahertz (THz) emitters have been recognized as one of the most promising candidates for the next‐generation THz sources, owing to their peculiarities of high efficiency, high stability, low cost, ultrabroad bandwidth, controllable polarization, and high scalability. Despite the substantial efforts, they rely on external magnetic fields to initiate the spin‐to‐charge conversion, which hitherto greatly limits its proliferation as practical devices. Here, we innovate a unique antiferromagnetic‐ferromagnetic (IrMn3|CoFeB) heterostructure and demonstrate that it can efficiently generate THz radiation without any external magnetic field. We assign it to the exchange bias or interfacial exchange coupling effect and enhanced anisotropy. By precisely balancing the exchange bias effect and the enhanced THz radiation efficiency, an optimized 5.6‐nm‐thick IrMn3|CoFeB|W tri‐layer heterostructure is successfully realized, yielding an intensity surpassing that of Pt|CoFeB|W. Moreover, the intensity of THz emission is further boosted by togethering the tri‐layer sample and bi‐layer sample Besides, the THz polarization may be flexibly controlled by rotating the sample azimuthal angle, manifesting sophisticated active THz field manipulation capability. The field‐free coherent THz emission we demonstrate here shines light on the development of spintronic THz optoelectronic devices. This article is protected by copyright. All rights reserved

Strain engineering is a promising way to tune the electrical, electrochemical, magnetic, and optical properties of two‐dimensional (2D) materials, with the potential to achieve high‐performance 2D‐material‐based devices ultimately. This review discusses the experimental and theoretical results from recent advances in the strain engineering of 2D materials. We summarize some novel methods to induce strain and then highlight the tunable electrical, and optical/optoelectronic properties of 2D materials via strain engineering including particularly the previously less discussed strain tuning of superconducting, magnetic, and electrochemical properties. Also, the future perspectives of strain engineering are given for its potential applications in functional devices. The state of the survey presents the ever‐increasing advantages and popularity of strain engineering for tuning properties of 2D materials. It provides suggestions and insights for further research and applications in optical, electronic, and spintronic devices. This article is protected by copyright. All rights reserved

Tin‐based perovskites are promising candidates to replace their toxic lead‐based counterparts in optoelectronic applications, such as light‐emitting diodes (LEDs). However, the development of tin perovskite LEDs is slow due to the challenge of obtaining high quality tin perovskite films. Here, a vapor‐assisted spin‐coating (VASC) method is developed to achieve high quality tin perovskites and high efficiency LEDs. It is revealed that solvent vapor can lead to in situ recrystallization of tin perovskites during the film formation process, thus significantly improving the crystalline quality with reduced defects. An antioxidant additive is further introduced to suppress the oxidation of Sn2+ and increase the photoluminescence quantum efficiency up to ∼30%, which is an ∼4‐fold enhancement in comparison with that of the control method. As a result, efficient tin perovskite LEDs are achieved with a peak external quantum efficiency of 5.3%, which is among the highest efficiency of lead‐free perovskite LEDs. This article is protected by copyright. All rights reserved

The ubiquitous nature of atmospheric moisture makes it a significant water resource available at any geographical location. Atmospheric water harvesting (AWH) technology, which extracts moisture from ambient air to generate clean water, is a promising strategy to realize decentralized water production. The high water uptake exhibited by salt‐based sorbents makes them attractive for AWH, especially in low relative humidity (RH) environments. Salt‐based sorbents often have relatively high desorption heat, rendering water release an energy‐intensive process. We proposed a hygroscopic gel, PAM hydrogel controlled incorporated with LiCl, capable of effective moisture harvesting from arid environments. The interactions between the hydrophilic hydrogel network and the captured water enable the PAM‐LiCl to accumulate more free and weakly‐bonded water molecules, significantly lowering the desorption heat compared with conventional neat salt sorbents. Benefiting from the affinity for swelling of the polymer backbones, the developed PAM‐LiCl achieves a high water uptake of ca. 1.1 g/g at 20% RH with fast sorption kinetics of ca. 0.008 g g–1 min–1 and further demonstrates a daily water yield up to ca. 7 g/g at this condition. These findings provide a new pathway for synthesis of materials with efficient water absorption/desorption properties, to reach energy‐efficient water release for AWH in arid climates. This article is protected by copyright. All rights reserved

Changing the solvation sheath of hydrated Zn ions is an effective strategy to stabilize Zn anodes to obtain a practical aqueous Zn‐ion battery. However, key points related to the rational design remain unclear including how the properties of the solvent molecules intrinsically regulate the solvated structure of the Zn ions. We propose using a stability constant (K), namely the equilibrium constant of the complexation reaction, as a universal standard to make an accurate selection of ligands in the electrolyte to improve the anode stability. It is found that K greatly impacts the corrosion current density and nucleation overpotential. Following this, ethylene diamine tetraacetic acid with a superhigh K effectively suppresses Zn corrosion and induces uniform Zn‐ion deposition. As a result, the anode has an excellent stability of over 3000 h. This work presents a general principle to stabilize anodes by regulating the solvation chemistry, guiding the development of novel electrolytes for sustainable aqueous batteries. This article is protected by copyright. All rights reserved

Engineering surface structure can precisely and effectively tune optoelectronic properties of halide perovskites, but are incredibly challenging. Herein, we report the design and fabrication of uniform all–inorganic CsPbBr3 cubes/tetrahedrons single‐crystals with precise control of (100) and (111) surface anisotropy, respectively. By combining theoretical calculations, we demonstrated that the preferred (100) surface engineering of CsPbBr3 single‐crystals enables a lowest surface bandgap energy (2.33 eV) and high‐rate carrier mobility up to 241 μm2 V–1 s–1, inherently boosting their light‐harvesting and carrier transport capability. Whereas, the polar (111) surface induces ∼0.16 eV upward surface‐band bending and ultrahigh surface defect density of 1.49 × 1015 cm–3, which is beneficial for enhancing surface defects‐catalyzed reactions. Our work highlights the anisotropic surface engineering for boosting perovskite optoelectronic devices and beyond. This article is protected by copyright. All rights reserved

A universal atomic layer confined doping strategy is developed to prepare isolated Cu atoms incorporated Bi24O31Br10 materials. The local polarization can be created along Cu‐O‐Bi atomic interface, which enables better electron delocalization for effective N2 activation. The optimized Cu‐Bi24O31Br10 atomic layers show 5.3 and 88.2 times improved photocatalytic nitrogen fixation activity than Bi24O31Br10 atomic layer and bulk Bi24O31Br10, respectively, with the NH3 generation rate arrive 291.1 μmol g−1 h−1 in pure water. The polarized Cu‐Bi site pairs can increase the non‐covalent interaction between catalyst's surface and N2 molecule, then further weaken the covalent bond order in N‐N. As a result, the hydrogenation pathways can be altered from associative distal pathway for Bi24O31Br10 to the alternating pathway for Cu‐Bi24O31Br10. This strategy provides an accessible pathway for designing polarized metal site pairs or tune the non‐covalent interaction and covalent bond order. This article is protected by copyright. All rights reserved

Ruthenium is one of the most active catalysts for ammonia dehydrogenation and is essential for the use of ammonia as a hydrogen storage material. The B5‐type site on the surface of ruthenium is expected to exhibit the highest catalytic activity for ammonia dehydrogenation, but the number of these sites is typically low. Here, we synthesize a B5‐site‐rich ruthenium catalyst by exploiting the crystal symmetry of a hexagonal boron nitride support. In the prepared ruthenium catalyst, ruthenium nanoparticles are formed epitaxially on hexagonal boron nitride sheets with hexagonal planar morphologies, in which the B5 sites predominate along the nanoparticle edges. By activating the catalyst under the reaction condition, the population of B5 sites further increases as the facets of the ruthenium nanoparticles develop. The electron density of the Ru nanoparticles also increases during catalyst activation. The synthesized catalyst shows superior catalytic activity for ammonia dehydrogenation compared to previously reported catalysts. This work demonstrates that morphology control of a catalyst via support‐driven heteroepitaxy can be exploited for synthesizing highly active heterogeneous catalysts with tailored atomic structures. This article is protected by copyright. All rights reserved

Superior fast charging is a desirable capability of lithium‐ion batteries, which can make electric vehicles a strong competition to traditional fuel vehicles. However, the slow transport of solvated lithium ions in liquid electrolytes is a limiting factor. Here, we report a LixCu6Sn5 intermetallic network to address this issue. Based on electrochemical analysis and X‐ray photoelectron spectroscopy mapping, we demonstrate that the reported intermetallic network can form a high‐speed solid‐state lithium transport matrix throughout the electrode, which largely reduces the polarization effect in the graphite anode. Employing this design, we fabricated superior fast‐charging graphite/lithium cobalt oxide full cells and tested them under strict electrode conditions. At the charging rate of 6 C, the fabricated full cells showed a capacity of 145 mAh g−1 with an extraordinary capacity retention of 96.6%. In addition, the full cell also exhibits good electrochemical stability at a high charging rate of 2 C over 100 cycles (96.0% of capacity retention) in comparison to traditional graphite anode based cell (86.1% of capacity retention). This work presents a new strategy for fast charging lithium ion batteries on basis of high speed solid state lithium transport in intermetallic alloy hosts. This article is protected by copyright. All rights reserved

Cu3(HHTT)2 (HHTT: 2,3,7,8,12,13‐hexahydroxytetraazanaphthotetraphene) is a novel two‐dimensional conjugated metal‐organic framework (2D c‐MOF) with efficient in‐plane d‐π conjugations and strong interlayer π‐π interactions while the growth of Cu3(HHTT)2 thin films has never been reported until now. Here, we present the successful fabrication of highly oriented wafer‐scale Cu3(HHTT)2 thin films with a layer‐by‐layer growth method on various substrates. Its semiconducting behavior and carrier transport mechanisms are clarified through temperature and frequency dependent conductivity measurements. Flexible photodetectors based on Cu3(HHTT)2 thin films exhibit reliable photo‐responses at room temperature in a wavelength region from ultraviolet (UV) to mid‐infrared (MIR), which is much broader than those of solution‐processed broadband photodetectors reported previously. Moreover, the photodetectors can show a typical synaptic behavior and excellent data recognition accuracy in artificial neural networks. This work opens a window for the exploration of high‐performance and multi‐functional optoelectronic devices based on 2D c‐MOFs. This article is protected by copyright. All rights reserved

Solid‐state electrolytes (SSEs) formed inside an electrochemical cell by polymerization of a liquid precursor provide a promising strategy for overcoming problems with electrolyte wetting in solid‐state batteries. Hybrid solid‐state polymer electrolytes (HSPEs) created by in situ polymerization of a conventional liquid precursor containing electrochemically inert nanostructures are of particular interest because they offer a mechanism for selectively reinforcing or adding new functionalities to the electrolyte—removing the need for high degrees of polymerization. The synthesis, structure, chemical kinetics, ion‐transport properties and electrochemical characteristics of HSPEs created by Al(OTf)3‐initiated polymerization of 1,3‐dioxolane (DOL) containing hairy, nano‐sized SiO2 particles are reported. Small‐angle X‐ray scattering reveals the particles are well‐dispersed in liquid DOL. Strong interaction between poly(ethylene glycol) molecules tethered to the SiO2 particles and poly(DOL) lead to co‐crystallization—anchoring the nanoparticles in their host It also enables polymerization–depolymerization processes in DOL to be studied and controlled. The utility of the in‐situ‐formed HSPE, is demonstrated first in Li|HSPE|Cu half cells, which manifest Coulombic efficiencies (CE) values approaching 99%. HSPEs are also demonstrated in solid‐state lithium–sulfur–polyacrylonitrile (SPAN) composite full‐cell batteries. The in‐situ‐formed Li|HSPE|SPAN cells show good cycling stability and thus provide a promising path toward all‐solid‐state batteries.

Developing advanced electrocatalysts with exceptional two electron (2e–) selectivity, activity and stability are crucial for driving oxygen reduction reaction (ORR) to produce hydrogen peroxide (H2O2). Herein, a composition engineering strategy has been adapted to flexibly regulate the intrinsic activity of amorphous nickel boride nanoarchitectures for efficient 2e– ORR by oriented reduction of Ni2+ with different amounts of BH4–. Among borides, the amorphous NiB2 delivers the 2e– selectivity close to 99% at 0.4 V and over 93% in a wide potential range, together with a negligible activity decay under prolonged time. Notably, an ultrahigh H2O2 production rate of 4.753 mol gcat−1 h−1 has been achieved upon assembling NiB2 in the practical gas diffusion electrode. The combination of X‐ray absorption and in situ Raman spectroscopy, as well as transient photovoltage measurements with density functional theory unequivocally reveal that the atomic ratio between Ni and B induces the local electronic structure diversity, allowing optimization of the adsorption energy of Ni towards *OOH and reducing the interfacial charge transfer kinetics to inhibit the formation of O‐O. This article is protected by copyright. All rights reserved

Three‐dimensional printing is a powerful manufacturing technology for shaping materials into complex structures. While the palette of printable materials continues to expand, the rheological and chemical requisites for printing are not always easy to fulfill. Here, we report a universal manufacturing platform for shaping materials into intricate geometries without the need for their printability, but instead using light‐based printed salt structures as leachable molds. The salt structures are printed using photocurable resins loaded with NaCl particles. The printing, debinding and sintering steps involved in the process are systematically investigated to identify ink formulations enabling the preparation of crack‐free salt templates. Our experiments reveal that the formation of a load‐bearing network of salt particles is essential to prevent cracking of the mold during the process. By infiltrating the sintered salt molds and leaching the template in water, we create complex‐shaped architectures from diverse compositions such as biomedical silicone, chocolate, light metals, degradable elastomers and fiber composites, thus demonstrating the universal, cost‐effective, and sustainable nature of this new manufacturing platform. This article is protected by copyright. All rights reserved

Recently, electrically conducting heterointerfaces between dissimilar band‐insulators (such as lanthanum aluminate and strontium titanate) have attracted considerable research interest. Charge transport has been thoroughly explored and fundamental aspects of conduction firmly established. Perhaps surprisingly, similar insights into conceptually much simpler conducting homointerfaces, such as the domain walls that separate regions of different orientations of electrical polarisation within the same ferroelectric band‐insulator, are not nearly so well‐developed. Addressing this disparity, we herein report magnetoresistance in approximately conical 180° charged domain walls, which occur in partially switched ferroelectric thin film single crystal lithium niobate. This system is ideal for such measurements: firstly, the conductivity difference between domains and domain walls is extremely and unusually large (a factor of at least 1013) and hence currents driven through the thin film, between planar top and bottom electrodes, are overwhelmingly channelled along the walls; secondly, when electrical contact is made to the top and bottom of the domain walls and a magnetic field is applied along their cone axes (perpendicular to the thin film surface), then the test geometry mirrors that of a Corbino disc, which is a textbook arrangement for geometric magnetoresistance measurement. Our data imply carriers at the domain walls with extremely high room temperature Hall mobilities of up to ∼ 3,700cm2V–1s–1. This is an unparalleled value for oxide interfaces (and for bulk oxides too) and is most comparable to mobilities in other systems typically seen at cryogenic, rather than at room, temperature. This article is protected by copyright. All rights reserved

Black phase formamidinium lead iodide (FAPbI3) with narrow band gap and high thermal stability has emerged as the most promising candidate for highly efficient and stable perovskite photovoltaics. In order to overcome the intrinsic difficulty of black phase crystallization and to eliminate the PbI2 residue, most sequential deposition methods of FAPbI3‐based perovskite would introduce external ions like methylammonium (MA+), cesium (Cs+), and bromide (Br–) ions to the perovskite structure of the light absorbing layer. Here we introduce a zwitterion‐functionalized SnO2 as the electron transport layer (ETL) to induce the crystallization of high quality black phase FAPbI3 on such SnO2 substrate. The SnO2 ETL treated with the zwitterion, formamidine sulfinic acid (FSA), can help rearrange the stack direction, orientation and distribution of residual PbI2 in perovskite layer, which reduces the side effect of the residual PbI2 to the perovskite structure. Besides, the FSA functionalization also modifies SnO2 ETL to suppress the deep‐level defects at the perovskite/SnO2 interface. As a result, the FSA‐FAPbI3 based perovskite solar cells (PSCs) exhibit an excellent power conversion efficiency up to 24.1% with 1000 h long‐term operational stability, which is among the highest values for FAPbI3 PSCs fabricated from sequential deposition. Our findings provide a new interface engineering strategy on the sequential fabrication of black phase FAPbI3 PSCs with improved optoelectronic performance. This article is protected by copyright. All rights reserved

Manipulating ferroic orders and realizing their coupling in multiferroics at room temperature are promising for designing future multifunctional devices. Single external stimulation has been extensively proved to demonstrate the ability of ferroelastic switching in multiferroic oxides, which is crucial to bridge the ferroelectricity and magnetism. However, it is still challenging to directly realize multi‐field driven magnetoelectric coupling in multiferroic oxides as potential multifunctional electrical devices. Here we show novel magneto‐electric‐optical coupling in multiferroic BiFeO3‐based thin films at room temperature mediated by deterministic ferroelastic switching using piezoresponse/magnetic force microscopy and aberration‐corrected transmission electron microscopy. Reversible photoinduced ferroelastic switching exhibiting magnetoelectric responses is confirmed in BiFeO3‐based films, which works at flexible strain states. This work directly demonstrates the room temperature magneto‐electric‐optical coupling in multiferroic films, which provides a framework for designing potential multi‐field driven magnetoelectric devices such as energy conservation memories. This article is protected by copyright. All rights reserved

Multiple resonance (MR) effect‐induced thermally activated delayed fluorescence (TADF) materials have garnered significant attention because they can achieve both high color purity and high external quantum efficiency (EQE). However, the reported green‐emitting MR‐TADF materials exhibit broader emission compared to those of blue‐emitting ones and suffer from severe efficiency roll‐off due to insufficient rate constants of reverse intersystem crossing process (kRISC). Herein, we report a pure green MR‐TADF material (ν‐DABNA‐CN‐Me) with high kRISC of 105 s–1. The key to success is introduction of cyano groups into a blue‐emitting MR‐TADF material (ν‐DABNA), which causes remarkable bathochromic shift without a loss of color purity. The organic light‐emitting diode employing it as an emitter exhibits green emission at 504 nm with a small full‐width at half‐maximum of 23 nm, corresponding to the Commission Internationale d’Éclairage coordinates of (0.13, 0.65). The device achieves a high maximum EQE of 31.9% and successfully suppresses the efficiency roll‐off at a high luminance. This article is protected by copyright. All rights reserved

Organic solar cells (OSCs) have experienced rapid progress with the innovation of near‐infrared (NIR)‐absorbing small‐molecular acceptors (SMAs), while the unique electronic properties of the SMAs raise new challenges in relation to cathode engineering for effective electron collection. To address this issue, we synthesized two fluorinated perylene‐diimides (PDIs), PDINN‐F and PDINN‐2F by a simple fluorination method, for the application as cathode interlayer (CIL) materials. The two bay‐fluorinated PDI based CILs possess lower the lowest unoccupied molecular orbital energy level of ca. −4.0 eV, which improves the energy level alignment at the NIR‐SMAs (such as BTP‐eC9)/cathode interface for a favorable electron extraction efficiency. The mono‐fluorinated PDINN‐F shows higher electron mobility and better improved interfacial compatibility. The PDINN‐F based OSCs with PM6: BTP‐eC9 as active layer exhibit an enhanced fill factor and larger short‐circuit current density, leading to a high power conversion efficiency (PCE) exceeding 18%. The devices with PDINN‐F CIL retained more than 80% of its initial PCE after operating at the maximum power point under continuous illumination for 750 hours. This work prescribes a facile, cost‐effective and scalable method for the preparation of stable, high‐performance fluorinated CILs, and instilling promise for the NIR‐SMAs‐based OSCs moving forward. This article is protected by copyright. All rights reserved