In-Sensor Tactile Fusion and Logic for Accurate Intention Recognition.

Touch control intention recognition is an important direction for the future development of human-machine interactions (HMIs). However, the implementation of parallel-sensing functional modules generally requires a combination of different logical blocks and control circuits, which results in regional redundancy, redundant data, and low efficiency. Here, a location-and-pressure intelligent tactile sensor (LPI tactile sensor) unprecedentedly combined with sensing, computing, and logic is proposed, enabling efficient and ultrahigh-resolution action-intention interaction. The LPI tactile sensor eliminates the need for data transfer among the functional units through the core integration design of the layered structure. It actuates in-sensor perception through feature transmission, fusion, and differentiation, thereby revolutionizing the traditional von Neumann architecture. While greatly simplifying the data dimensionality, the LPI tactile sensor achieves outstanding resolution sensing in both location (<400 µm) and pressure (75 Pa). Synchronous feature fusion and decoding support the high-fidelity recognition of action and combinatorial logic intentions. Benefiting from location and pressure synergy, the LPI tactile sensor demonstrates robust privacy as an encrypted password device and interaction intelligence through pressure enhancement. It can recognize continuous touch actions in real time, map real intentions to target events, and promote accurate and efficient intention-driven HMIs.

The dynamic surface evolution of halide perovskites induced by external energy stimulation.

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum (UHV) interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3  in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position, hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

Deciphering Vacancy Defect Evolution of 2D MoS2 for Reliable Transistors.

Two-dimensional (2D) MoS2 is an excellent candidate channel material for next-generation integrated circuit (IC) transistors. However, the reliability of MoS2 is of great concern due to the serious threat of vacancy defects, such as sulfur vacancies (VS). Evaluating the impact of vacancy defects on the service reliability of MoS2 transistors is crucial, but it has always been limited by the difficulty in systematically tracking and analyzing the changes and effects of vacancy defects in the service environment. Here, a simulated initiator is established for deciphering the evolution of vacancy defects in MoS2 and their influence on the reliability of transistors. The results indicate that VS below 1.3% are isolated by slow enrichment during initiation. Over 1.3% of VS tend to enrich in pairs and over 3.5% of the enriched VS easily evolve into nanopores. The enriched VS with electron doping in the channel cause the threshold voltage (Vth) negative drift approaching 6 V, while the expanded nanopores initiate the Vth roll-off and punch-through of transistors. Finally, sulfur steam deposition has been proposed to constrain VS enrichment, and reliable MoS2 transistors are constructed. Our research provides a new method for deciphering and identifying the impact of defects.

Conformal Human-Machine Integration Using Highly Bending-Insensitive, Unpixelated, and Waterproof Epidermal Electronics Toward Metaverse.

Efficient and flexible interactions require precisely converting human intentions into computer-recognizable signals, which is critical to the breakthrough development of metaverse. Interactive electronics face common dilemmas, which realize high-precision and stable touch detection but are rigid, bulky, and thick or achieve high flexibility to wear but lose precision. Here, we construct highly bending-insensitive, unpixelated, and waterproof epidermal interfaces (BUW epidermal interfaces) and demonstrate their interactive applications of conformal human-machine integration. The BUW epidermal interface based on the addressable electrical contact structure exhibits high-precision and stable touch detection, high flexibility, rapid response time, excellent stability, and versatile "cut-and-paste" character. Regardless of whether being flat or bent, the BUW epidermal interface can be conformally attached to the human skin for real-time, comfortable, and unrestrained interactions. This research provides promising insight into the functional composite and structural design strategies for developing epidermal electronics, which offers a new technology route and may further broaden human-machine interactions toward metaverse.

Morphotropic Phase Boundary in Polarized Organic Piezoelectric Materials.

Designing the morphotropic phase boundary (MPB) has been the most sought-after approach to achieve high piezoelectric performance of piezoelectric materials. However, MPB has not yet been found in the polarized organic piezoelectric materials. Here, we discover MPB with biphasic competition of ß and 3/1-helical phases in the polarized piezoelectric polymer alloys (PVTC-PVT) and demonstrate a mechanism to induce MPB using the compositionally tailored intermolecular interaction. Consequently, PVTC-PVT exhibits a giant quasistatic piezoelectric coefficient of >32 pC/N while maintaining a low Young's modulus of 182 MPa, with a record-high figure of merit of piezoelectricity modulus of about 176 pC/(N·GPa) among all piezoelectric materials.

Boosting Charge Utilization in Self-Powered Photodetector for Real-Time High-Throughput Ultraviolet Communication.

Ultraviolet (UV) communication is a cutting-edge technology in communication battlefields, and self-powered photodetectors as their optical receivers hold great potential. However, suboptimal charge utilization has largely limited the further performance enhancement of self-powered photodetectors for high-throughput communication application. Herein, a self-powered Ti3 C2 Tx -hybrid poly(3,4 ethylenedioxythiophene):poly-styrene sulfonate (PEDOT:PSS)/ZnO (TPZ) photodetector is designed, which aims to boost charge utilization for desirable applications. The device takes advantage of photothermal effect to intensify pyro-photoelectric effect as well as the increased conductivity of the PEDOT:PSS, which significantly facilitated charge separation, accelerated charge transport, and suppressed interface charge recombination. Consequently, the self-powered TPZ photodetector exhibits superior comprehensive performance with high responsivity of 12.3 mA W-1 and fast response time of 62.2 µs, together with outstanding reversible and stable cyclic operation. Furthermore, the TPZ photodetector has been successfully applied in an integrated UV communication system as the self-powered optical receiver capable of real-time high-throughput information transmission with ASCII code under 9600 baud rate. This work provides the design insight of highly performing self-powered photodetectors to achieve high-efficiency optical communication in the future.

Roles of Low-Dimensional Nanomaterials in Pursuing Human-Machine-Thing Natural Interaction.

A wide variety of low-dimensional nanomaterials with excellent properties can meet almost all the requirements of functional materials for information sensing, processing, and feedback devices. Low-dimensional nanomaterials are becoming the star of hope on the road to pursuing human-machine-thing natural interactions, benefiting from the breakthroughs in precise preparation, performance regulation, structural design, and device construction in recent years. This review summarizes several types of low-dimensional nanomaterials commonly used in human-machine-thing natural interactions and outlines the differences in properties and application areas of different materials. According to the sequence of information flow in the human-machine-thing interaction process, the representative research progress of low-dimensional nanomaterials-based information sensing, processing, and feedback devices is reviewed and the key roles played by low-dimensional nanomaterials are discussed. Finally, the development trends and existing challenges of low-dimensional nanomaterials in the field of human-machine-thing natural interaction technology are discussed.

Comparison of biochemical composition, nutritional quality, and metals concentrations between males and females of three different Crassostrea sp.

Gametogenesis can significantly affect the biochemical composition of oysters, but little research on the difference between sexes. Therefore, we conducted the first in-depth study on the composition differences between males and females of three different Crassostrea sp.. The results showed that females had higher glycogen, lipid, Cu and Zn contents than males, while males had higher protein and taurine contents than females at maturity, which might be related to special meiosis pattern of eggs and less energy was required for female gametogenesis. In addition, both males and females had well-balanced essential amino acid compositions. The omega-3: omega-6 (n-3: n-6) ratio of males was significantly higher than that of females, indicating that the nutritional quality of males was higher. These results provide a reliable and refined theoretical and research basis for revealing the nutritional quality, extracting beneficial ingredients, and developing functional food of Crassostrea sp., and provide data support for the sex-regulated breeding of oysters.

Identifying and Interpreting Geometric Configuration-Dependent Activity of Spinel Catalysts for Water Reduction.

The catalytic activity of transition metal-based catalysts is overwhelmingly dependent on the geometric configuration. Identification and interpretation of different geometric configurations' contributions to catalytic activity plays a pivotal role in catalytic performance elevation. Spinel structured AB2X4, consisting of tetrahedral (A2+-X)Td and octahedral (B3+-X)Oh geometric configurations, is a prototypical category of multi-geometric-configuration featured catalysts. However, it is still under debate about the predominant geometric configuration responsible for spinel catalyst activity, and the mechanistic origin of specific activity discrepancy among varied geometric configurations also remains ambiguous. Herein, CoTd2+ and CoOh3+ in Co3O4 are replaced by catalytically inert Zn2+ and Al3+ to yield ZnCo2O4 and CoAl2O4, respectively, thus ensuring the manipulable exposure of monotypic active configurations. By means of pulse voltammetry and in situ extended X-ray absorption fine structure, (Co3+-O)Oh is identified to be dominant for alkaline HER. In-depth theoretical investigation in combination with X-ray absorption spectroscopy further interprets the synergistic effect between Co and O sites in (Co3+-O)Oh configuration on water reduction kinetics upon both water dissociation and hydrogen desorption steps. Furthermore, specific facet dependence of catalytic activity is also deciphered based on precise facet exposure identification and serial theoretical analysis. This work unambiguously figures out the subtle geometric configuration dependence of spinel catalyst activity for water reduction and highlights the synergistic relationship among different components confined in geometric configuration, thereby shedding new light on the rational design of advanced catalysts from the atomic level of geometric configuration optimization.

Synthesis of Large-Area MXenes with High Yields through Power-Focused Delamination Utilizing Vortex Kinetic Energy.

Evaluating the delamination process in the synthesis of MXenes (2D transition metal carbides and nitrides) is critical for their development and applications. However, the preparation of large defect-free MXene flakes with high yields is challenging. Here, a power-focused delamination (PFD) strategy is demonstrated that can enhance both the delamination efficiency and yield of large Ti3 C2 Tx MXene nanosheets through repetitive precipitation and vortex shaking processes. Following this protocol, a colloidal concentration of 20.4 mg mL-1 of the Ti3 C2 Tx MXene can be achieved after five PFD cycles, and the yield of the basal-plane-defect-free Ti3 C2 Tx nanosheets reaches 61.2%, which is 6.4-fold higher than that obtained using the sonication-exfoliation method. Both nanometer-thin devices and self-supporting films exhibit excellent electrical conductivities (≈25 000 and 8260 S cm-1 for a 1.8 nm thick monolayer and 11 µm thick film, respectively). Hydrodynamic simulations reveal that the PFD method can efficiently concentrate the shear stress on the surface of the unexfoliated material, leading to the exfoliation of the nanosheets. The PFD-synthesized large MXene nanosheets exhibit superior electrical conductivities and electromagnetic shielding (shielding effectiveness per unit volume: 35 419 dB cm2 g-1 ). Therefore, the PFD strategy provides an efficient route for the preparation of high-performance single-layer MXene nanosheets with large areas and high yields.

A van der Waals Ferroelectric Tunnel Junction for Ultrahigh-Temperature Operation Memory.

Facing the constant scaling down and thus increasingly severe self-heating effect, developing ultrathin and heat-insensitive ferroelectric devices is essential for future electronics. However, conventional ultrathin ferroelectrics and most 2D ferroelectric materials (2DFMs) are not suitable for high-temperature operation due to their low Curie temperature. Here, by using few-layer α-In2 Se3 , a special 2DFM with high Curie temperature, van der Waals (vdW) ferroelectric tunnel junction (FTJ) memories that deliver outstanding and reliable performance at both room and high temperatures are constructed. The vdW FTJs offer a large on/off ratio of 104 at room temperature and still reveal excellent on/off ratio at an ultrahigh temperature of 470 K, which will fail down other 2DFMs. Moreover, long retention and reliable cyclic endurance at high temperature are achieved, showing robust thermal stability of the vdW FTJ memory. The observations of this work demonstrate an exciting promise of α-In2 Se3 for reliable service in high temperature either from self-heating or harsh environments.

Omnibearing Interpretation of External Ions Passivated Ion Migration in Mixed Halide Perovskites.

Fundamental understanding of ion migration inside perovskites is of vital importance for commercial advancements of photovoltaics. However, the mechanism for external ions incorporation and its effect on ion migration remains elusive. Herein, taking K+ and Cs+ co-incorporated mixed halide perovskites as a model, the impact of external ions on ion migration behavior has been interpreted via multiple dimensional characterization aspects. The space-effect on phase segregation inhibition has been revealed by the photoluminescence evolution and in situ dynamic cathodoluminescence behaviors. The plane-effect on current suppression along grain boundary has been evidenced via visualized surface current mapping, local current hysteresis, and time-resolved current decay. And the point-effect on activation energy incremental for individual ions has been also probed by cryogenic electronic quantification. All these results sufficiently demonstrate the passivated ion migration results in the eventually improved phase stability of perovskite, of which the origin lies in various ion migration energy barriers.

Interpretation of Rubidium-Based Perovskite Recipes toward Electronic Passivation and Ion-Diffusion Mitigation.

Rubidium cation (Rb+ ) addition is witnessed to play a pivotal role in boosting the comprehensive performance of organic-inorganic hybrid perovskite solar cells. However, the origin of such success derived from irreplaceable superiorities brought by Rb+ remains ambiguous. Herein, grain-boundary-including atomic models are adopted for the accurate theoretical analysis of practical Rb+ distribution in perovskite structures. The spatial distribution, covering both the grain interiors and boundaries, is thoroughly identified by virtue of synchrotron-based grazing-incidence X-ray diffraction. On this basis, the prominent elevation of the halogen vacancy formation energy, improved charge-carrier dynamics, and the electronic passivation mechanism in the grain interior are expounded. As evidenced by the increased energy barrier and suppressed microcurrent, the critical role of Rb+ addition in blocking the diffusion pathway along grain boundaries, inhibiting halide phase segregation, and eventually enhancing intrinsic stability is elucidated. Hence, the linkage avalanche effect of occupied location dominated by subtle changes in Rb+ concentration on electronic defects, ion migration, and phase stability is completely investigated in detail, shedding a new light on the advancement of high-efficiency cascade-incorporating strategies and perovskite compositional engineering.

All-van-der-Waals Barrier-Free Contacts for High-Mobility Transistors.

Ultrathin 2D semiconductor devices are considered to have beyond-silicon potential but are severely troubled by the high Schottky barriers of the metal-semiconductor contacts, especially for p-type semiconductors. Due to the severe Fermi-level pinning effect and the lack of conventional semimetals with high work functions, their Schottky hole barriers are hardly removed. Here, an all-van-der-Waals barrier-free hole contact between p-type tellurene semiconductor and layered 1T'-WS2 semimetal is reported, which achieves a zero Schottky barrier height of 3 ± 9 meV and a high field-effect mobility of ≈1304 cm2 V-1 s-1 . The formation of such contacts can be attributed to the higher work function of ≈4.95 eV of the 1T'-WS2 semimetal, which is in sharp contrast with low work function (4.1-4.7 eV) of conventional semimetals. The study defines an available strategy for eliminating the Schottky barrier of metal-semiconductor contacts, facilitating 2D-semiconductor-based electronics and optoelectronics to extend Moore's law.

Architecture Design and Interface Engineering of Self-assembly VS4/rGO Heterostructures for Ultrathin Absorbent.

The employment of microwave absorbents is highly desirable to address the increasing threats of electromagnetic pollution. Importantly, developing ultrathin absorbent is acknowledged as a linchpin in the design of lightweight and flexible electronic devices, but there are remaining unprecedented challenges. Herein, the self-assembly VS4/rGO heterostructure is constructed to be engineered as ultrathin microwave absorbent through the strategies of architecture design and interface engineering. The microarchitecture and heterointerface of VS4/rGO heterostructure can be regulated by the generation of VS4 nanorods anchored on rGO, which can effectively modulate the impedance matching and attenuation constant. The maximum reflection loss of 2VS4/rGO40 heterostructure can reach - 43.5 dB at 14 GHz with the impedance matching and attenuation constant approaching 0.98 and 187, respectively. The effective absorption bandwidth of 4.8 GHz can be achieved with an ultrathin thickness of 1.4 mm. The far-reaching comprehension of the heterointerface on microwave absorption performance is explicitly unveiled by experimental results and theoretical calculations. Microarchitecture and heterointerface synergistically inspire multi-dimensional advantages to enhance dipole polarization, interfacial polarization, and multiple reflections and scatterings of microwaves. Overall, the strategies of architecture design and interface engineering pave the way for achieving ultrathin and enhanced microwave absorption materials.

Gold Catalyst Anchored to Pre-Reduced Co3O4 Nanorods for the Hydrodeoxygenation of Vanillin Using Alcohols as Hydrogen Donors.

The preparation of highly dispersed metal catalysts with strong electronic metal-support interactions (EMSIs) is of great significance. In this study, oxygen vacancies (OVs) were generated on the surfaces of Co3O4 nanorods (NRs) through NaBH4 treatment, and then the generated surface OVs were used to anchor gold clusters. The resulting catalyst was used for the hydrodeoxygenation (HDO) of vanillin based on transfer hydrogenation with alcohol donors. The conversion of vanillin and the selectivity to 2-methoxy-4-methylphenol (MMP) both reached 99% under the optimized reaction conditions, and these values were significantly higher than those obtained for the gold catalyst supported on the untreated Co3O4 NRs. The obtained results were verified by theoretical calculations and experimental data and confirmed the existence of strong EMSIs between the OV-enriched Co3O4 NRs (Co3O4 NRs-OVs) and the gold clusters, which allows electron transfer from the Co3O4 NRs to gold. Increasing the number of electrons on the gold surface can promote the catalytic hydrogen transfer of alcohol, in addition to selectively adsorbing the C═O group in vanillin to improve the selectivity toward MMP. This strategy based on the OV-anchoring of metals onto the surface of a support can be extended to other metals, thereby providing a promising method for the design of advanced and highly efficient metal catalysts.

Single-Atom Engineering to Ignite 2D Transition Metal Dichalcogenide Based Catalysis: Fundamentals, Progress, and Beyond.

Single-atom catalysis has been recognized as a pivotal milestone in the development history of heterogeneous catalysis by virtue of its superior catalytic performance, ultrahigh atomic utilization, and well-defined structure. Beyond single-atom protrusions, two more motifs of single-atom substitutions and single-atom vacancies along with synergistic single-atom motif assemblies have been progressively developed to enrich the single-atom family. On the other hand, besides traditional carbon material based substrates, a wide variety of 2D transitional metal dichalcogenides (TMDs) have been emerging as a promising platform for single-atom catalysis owing to their diverse elemental compositions, variable crystal structures, flexible electronic structures, and intrinsic activities toward many catalytic reactions. Such substantial expansion of both single-atom motifs and substrates provides an enriched toolbox to further optimize the geometric and electronic structures for pushing the performance limit. Concomitantly, higher requirements have been put forward for synthetic and characterization techniques with related technical bottlenecks being continuously conquered. Furthermore, this burgeoning single-atom catalyst (SAC) system has triggered serial scientific issues about their changeable single atom-2D substrate interaction, ambiguous synergistic effects of various atomic assemblies, as well as dynamic structure-performance correlations, all of which necessitate further clarification and comprehensive summary. In this context, this Review aims to summarize and critically discuss the single-atom engineering development in the whole field of 2D TMD based catalysis covering their evolution history, synthetic methodologies, characterization techniques, catalytic applications, and dynamic structure-performance correlations. In situ characterization techniques are highlighted regarding their critical roles in real-time detection of SAC reconstruction and reaction pathway evolution, thus shedding light on lifetime dynamic structure-performance correlations which lay a solid theoretical foundation for the whole catalytic field, especially for SACs.