Abstract Breakthroughs brought about by two‐dimensional (2D) materials in the field of photodetection have opened up new possibilities in infrared imaging. However, challenges still exist in fabricating high‐density detector arrays using such materials, which are essential for traditional imaging systems. In this study, we present a state‐of‐the‐art computing imaging system that utilizes a MoTe2/Si self‐powered photodetector coupled with flexible Hadamard modulation algorithms. This system demonstrates remarkable capability to produce high‐quality images in the shortwave infrared (SWIR) band, surpassing the capabilities of devices based on alternative material systems. The exceptional infrared imaging capability primarily stems from the MoTe2/Si photodetector's inherent features, including an ultra‐wide spectral range (265–1550 nm) and extremely high sensitivity (linear dynamic range (LDR) up to 123 dB, responsivity (R) up to 0.33 A W–1, external quantum efficiency (EQE) up to 43% and a specific detectivity (D*) exceeding 2.9 × 1011 Jones). Moreover, the imaging system demonstrates the ability to achieve high‐quality edge imaging of objects in the SWIR band (1550 nm), even in strong scattering environments and under low sampling rate conditions (sampling rate of 25%). We believe that this work will effectively advance the application scope of 2D materials in the field of computational imaging in SWIR bands.image

Abstract Static rechargeable zinc‐iodine (Zn‐I2) batteries are superior in safety, cost‐effectiveness, and sustainability, giving them great potential for large‐scale energy storage applications. However, the shuttle effect of polyiodides on the cathode and the unstable anode/electrolyte interface hinder the development of Zn‐I2 batteries. Herein, a self‐segregated biphasic electrolyte (SSBE) was proposed to synergistically address those issues. The strong interaction between polyiodides and the organic phase was demonstrated to limit the shuttle effect of polyiodides. Meanwhile, the hybridization of polar organic solvent in the inorganic phase modulated the bonding structure, as well as the effective weakening of water activity, optimizing the interface during zinc electroplating. As a result, the Zn‐I2 coin cells performed a capacity retention of nearly 100% after 4000 cycles at 2 mA cm−2. And a discharge capacity of 0.6 Ah with no degradation after 180 cycles was achieved in the pouch cell. A photovoltaic energy storage battery was further achieved and displayed a cumulative capacity of 5.85 Ah. The successfully designed energy storage device exhibits the application potential of Zn‐I2 batteries for stationary energy storage.image

Abstract High‐temperature stable transparent conductive oxides (TCOs) are highly desirable in optoelectronics but are rarely achieved due to the defect generation that is inevitable during high‐temperature air annealing. This work reports unprecedented stability in aluminum and fluorine co‐doped ZnO (AFZO) films prepared by pulse laser deposition. The AFZO can retain a mobility of 60 cm2 V−1 s−1, an electron concentration of 4.5 × 1020 cm−3, and a visible transmittance of 91% after air‐annealing at 600°C. Comprehensive defect characterization and first principles calculations have revealed that the offset of substitutional aluminum by zinc vacancy is responsible for the instability observed in aluminum‐doped ZnO, and the pairing between fluorine substitution and zinc vacancy ensures the high‐temperature stability of AFZO. The utility of AFZO in enabling the epitaxial growth of (AlxGa1−x)2O3 film within a high‐temperature, oxygen‐rich environment is demonstrated, facilitating the development of a self‐powered solar‐blind ultraviolet Schottky photodiode. Furthermore, the high‐mobility AFZO transparent electrode enables perovskite solar cells to achieve improved power conversion efficiency by balancing the electron concentration‐dependent conductivity and transmittance. These findings settle the long‐standing controversy surrounding the instability in TCOs and open up exciting prospects for the advancement of optoelectronics.image

Abstract The relentless pursuit of sustainable and safe energy storage technologies has driven a departure from conventional lithium‐based batteries toward other relevant alternatives. Among these, aqueous batteries have emerged as a promising candidate due to their inherent properties of being cost‐effective, safe, environmentally friendly, and scalable. However, traditional aqueous systems have faced limitations stemming from water's narrow electrochemical stability window (~1.23 V), severely constraining their energy density and viability in high‐demand applications. Recent advancements in decoupling aqueous batteries offer a novel solution to overcome this challenge by separating the anolyte and catholyte, thereby expanding the theoretical operational voltage window to over 3 V. One key component of this innovative system is the ion‐selective membrane (ISM), acting as a barrier to prevent undesired crossover between electrolytes. This review provides a comprehensive overview of recent advancements in decoupling aqueous batteries, emphasizing the application of various types of ISMs. Moreover, we summarize different specially designed ISMs and their performance attributes. By addressing the current challenges ISMs face, the review outlines potential pathways for future enhancement and development of aqueous decoupling batteries.image

Abstract Due to the built‐in electric field induced by spontaneous polarization in hybrid perovskite (HP) ferroelectrics, the devices based on them exhibit excellent performance in self‐powered photodetection. However, most of the self‐powered photodetector are made of lead‐based HP ferroelectrics and have a relatively narrow photoresponse waveband. Although lead‐free HPs solve the problem of lead toxicity, their optoelectronic performance is inferior to that of lead‐based HPs and photoresponse waveband is limited by its optical band gap, which hinders their further application. To solve this problem, herein, a lead‐free HP ferroelectric (HDA)BiI5 (HDA is hexane‐1,6‐diammonium) with large spontaneous polarization shows an enhanced photocurrent and achieves x‐ray‐ultraviolet–visible‐near‐infrared (x‐ray‐UV–Vis–NIR) photoresponse through the ferro‐pyro‐phototronic (FPP) effect. The ferroelectric, pyroelectric, and photovoltaic characteristics coupled together in a single‐phase (HDA)BiI5 ferroelectric is an effective way to improve the performance of the devices. What is particularly attractive is that the FPP effect not only improves the optoelectronic performance of (HDA)BiI5, but also achieves broadband photoresponses beyond its optical absorption range. Especially, the current boosting with an exceptional contrast of ~1100% and 2400% under 520 and 637 nm, respectively, which is associated with FPP effect. Meanwhile, single crystal self‐powered photodetector based on (HDA)BiI5 also exhibit significant FPP effects even under high‐energy x‐ray, which owns an outstanding sensitivity of 170.7 μC Gy−1 cm−2 and a lower detection limit of 266 nGy s−1 at 0 V bias. Therefore, it is of great significance to study the coupling of multiple physical effects and improve device performance based on lead‐free HP ferroelectrics.image

Abstract Halide perovskites with naturally coupled electron‐ion dynamics hold great potential for nonvolatile memory applications. Self‐rectifying memristors are promising as they can avoid sneak currents and simplify device configuration. Here we report a self‐rectifying memristor firstly achieved in a single perovskite (NHCINH3)3PbI5 (abbreviated as (IFA)3PbI5), which is sandwiched by Ag and ITO electrodes as the simplest cell in a crossbar array device configuration. The iodide ions of (IFA)3PbI5 can be easily activated, of which the migration in the bulk contributes to the resistance hysteresis and the reaction with Ag at the interface contributes to the spontaneous formation of AgI. The perfect combination of n‐type AgI and p‐type (IFA)3PbI5 gives rise to the rectification function like a p–n diode. Such a self‐rectifying memristor exhibits the record‐low set power consumption and voltage. This work emphasizes that the multifunction of ions in perovskites can simplify the fabrication procedure, decrease the programming power, and increase the integration density of future memory devices.image

Abstract Two‐dimensional (2D) non‐layered materials, along with their unique surface properties, offer intriguing prospects for sensing applications. Introducing mechanical degrees of freedom is expected to enrich the sensing performances of 2D non‐layered devices, such as high frequency, high tunability, and large dynamic range, which could lead to new types of high performance nanosensors. Here, we demonstrate 2D non‐layered nanomechanical resonant sensors based on β‐In2S3, where the devices exhibit robust nanomechanical vibrations up to the very high frequency (VHF) band. We show that such device can operate as pressure sensor with broad range (from 10−3 Torr to atmospheric pressure), high linearity (with a nonlinearity factor as low as 0.0071), and fast response (with an intrinsic response time less than 1 μs). We further unveil the frequency scaling law in these β‐In2S3 nanomechanical sensors and successfully extract both the Young's modulus and pretension for the crystal. Our work paves the way towards future wafer‐scale design and integrated sensors based on 2D non‐layered materials.image

Abstract Plasmonic hot carrier engineering holds great promise for advanced infrared optoelectronic devices. The process of hot carrier transfer has the potential to surpass the spectral limitations of semiconductors, enabling detection of sub‐bandgap infrared photons. By harvesting hot carriers prior to thermalization, energy dissipation is minimized, leading to highly efficient photoelectric conversion. Distinguished from conventional band‐edge carriers, the ultrafast interfacial transfer and ballistic transport of hot carriers present unprecedented opportunities for high‐speed photoelectric conversion. However, a complete description on the underlying mechanism of hot‐carrier infrared optoelectronic device is still lacking, and the utilization of this strategy for tailoring infrared response is in its early stages. This review aims to provide a comprehensive overview of the generation, transfer and transport dynamics of hot carriers. Basic principles of hot‐carrier conversion in heterostructures are discussed in detail. In addition, progresses of two‐dimensional (2D) infrared hot‐carrier optoelectronic devices are summarized, with a specific emphasis on photodetectors, solar cells, light‐emitting devices and novel functionalities through hot‐carrier engineering. Furthermore, challenges and prospects of hot‐carrier device towards infrared applications are highlighted.image

Abstract Visible light‐based human–machine interactive media is capable of transmitting electrical readouts to machines and providing intuitive feedback to users simultaneously. Currently, many inorganic mechanoluminescent (ML) materials‐based interactive media, typically ZnS‐loaded phosphors (ZLPs), have been successfully demonstrated. However, organic ML materials‐based solutions were rarely exploited despite their huge merits of strong structural modification, abundant luminescence property, low cost, easy preparation, and so on. Here, we propose a novel interactive tactile display (ITD) based on organic ML materials (Cz‐A6‐dye) and triboelectric nanogenerator, with ultra‐brightness (130% enhancement) and ultra‐low threshold pressure (57% reduction) as compared to ZLPs. The proposed ITD achieves the conversion of weak mechanical stimuli into visible light and electrical signals simultaneously, without extra power supplies. Furthermore, the relationship between the luminous performance of organic ML materials and mechanical force is quantified, benefiting from the uniform ML layer prepared. Enabled by convolutional neural networks, the high‐accuracy recognition (97.1%) for handwriting and identity of users is realized at the same time. Thus, the ITD has great potential for intelligent wearable electronics and classified military applications.image