Multi-Interface Engineering of MXenes for Self-Powered Wearable Devices.

Self-powered wearable devices with integrated energy supply module and sensitive sensors have significantly blossomed for continuous monitoring of human activity and the surrounding environment in healthcare sectors. The emerging of MXene-based materials has brought research upsurge in the fields of energy and electronics, owing to their excellent electrochemical performance, large surface area, superior mechanical performance, and tunable interfacial properties, where their performance can be further boosted via multi-interface engineering. Herein, a comprehensive review of recent progress in MXenes for self-powered wearable devices is discussed from the aspects of multi-interface engineering. The fundamental properties of MXenes including electronic, mechanical, optical, and thermal characteristics are discussed in detail. Different from previous review works on MXenes, multi-interface engineering of MXenes from termination regulation to surface modification and their impact on the performance of materials and energy storage/conversion devices are summarized. Based on the interfacial manipulation strategies, potential applications of MXene-based self-powered wearable devices are outlined. Finally, proposals and perspectives are provided on the current challenges and future directions in MXene-based self-powered wearable devices.

Elastic Properties of Low-Dimensional Single-Crystalline Dielectric Oxides through Controlled Large-Area Wrinkle Generation.

Freestanding single-crystalline SrTiO3 membranes, as high-κ dielectrics, hold significant promise as the gate dielectric in two-dimensional (2D) flexible electronics. Nevertheless, the mechanical properties of the SrTiO3 membranes, such as elasticity, remain a critical piece of the puzzle to adequately address the viability of their applications in flexible devices. Here, we report statistical analysis on plane-strain effective Young's modulus of large-area SrTiO3 membranes (5 × 5 mm2) over a series of thicknesses (from 6.5 to 32.2 nm), taking advantage of a highly efficient buckling-based method, which reveals its evident thickness-dependent behavior ranging from 46.01 to 227.17 GPa. Based on microscopic and theoretical results, we elucidate these thickness-dependent behaviors and statistical data deviation with a bilayer model, which consists of a surface layer and a bulk-like layer. The analytical results show that the ∼3.1 nm surface layer has a significant elastic softening compared to the bulk-like layer, while the extracted modulus of the bulk-like layer shows a variation of ∼40 GPa. This variation is considered as a combined contribution from oxygen deficiency presenting in SrTiO3 membranes, and the alignment between applied strain and the crystal orientation. Upon comparison of the extracted elastic properties and electrostatic control capability to those of other typical gate dielectrics, the superior performance of single-crystalline SrTiO3 membranes has been revealed in the context of flexible gate dielectrics, indicating the significant potential of their application in high-performance flexible 2D electronics.

High-Performance Optoelectronic Gas Sensing Based on All-Inorganic Mixed-Halide Perovskite Nanocrystals with Halide Engineering.

Gas sensors are of great interest to portable and miniaturized sensing technologies with applications ranging from air quality monitoring to explosive detection and medical diagnostics, but the existing chemiresistive NO2 sensors still suffer from issues such as poor sensitivity, high operating temperature, and slow recovery. Herein, a high-performance NO2 sensors based on all-inorganic perovskite nanocrystals (PNCs) is reported, achieving room temperature operation with ultra-fast response and recovery time. After tailoring the halide composition, superior sensitivity of ≈67 at 8 ppm NO2 is obtained in CsPbI2 Br PNC sensors with a detection level down to 2 ppb, which outperforms other nanomaterial-based NO2 sensors. Furthermore, the remarkable optoelectronic properties of such PNCs enable dual-mode operation, i.e., chemiresistive and chemioptical sensing, presenting a new and versatile platform for advancing high-performance, point-of-care NO2 detection technologies.

High-Performance Flexible Graphene Oxide-Based Moisture-Enabled Nanogenerator via Multilayer Heterojunction Engineering and Power Management System.

Recently, there has been a surge of interest in nanogenerators within the scientific community because their immense potential for extracting energy from the surrounding environment. A promising approach involves utilizing ambient moisture as an energy source for portable devices. In this study, moisture-enabled nanogenerators (MENGs) are devised by integrating heterojunctions of graphene oxide (GO) and reduced graphene oxide (rGO). Benefiting from the unique structure, a larger ion concentration gradient is achieved as well as a lower resistance, which leads to enhanced electricity generation. The resulting MENG generates a desirable open-circuit voltage of 0.76 V and a short-circuit current density of 73 µA cm-2 with a maximum power density of 15.8 µW cm-2 . Notably, the designed device exhibits a high voltage retention of more than 90% after 3000 bending cycles, suggesting a high potential for flexible applications. Moreover, a large-scale integrated MENG array is developed by incorporating flexible printed circuit technology and connecting it to a power management system. This integrated system can provide ample energy to operate an electronic ink display and drive a heart rate sensor for health monitoring. The outcomes of this research present a novel framework for advancing next-generation self-powered flexible devices, thereby demonstrating significant promise for future wearable electronics.

Volumetric Nanocrystal Lattice Reconstruction through Dynamic Metal Complex Docking.

Vacancies pose a major challenge in the production of high-quality crystals, particularly at the nanoscale. To address this problem, we report a convenient strategy that involves volumetric lattice reconstruction and dynamic metal complex docking to produce ultrasmall (10 nm) and bright core-shell upconversion nanoparticles (UCNPs). This strategy involves the formation of lanthanide ion-oleic acid complexes during postannealing in solution, which effectively removes vacancies in nanocrystals. The removal of vacancies restricts the diffusion of lanthanide sensitizers and emitters within the core, thus minimizing surface quenching. Our volumetric lattice reconstruction strategy provides fundamental insights into lattice engineering and presents a general strategy for purifying functional nanocrystals for applications in fields such as single-molecule tracking, quantum optics, energy conversion, and others.

Borophene Embedded Cellulose Paper for Enhanced Photothermal Water Evaporation and Prompt Bacterial Killing.

Solar-driven photothermal water evaporation is considered an elegant and sustainable technology for freshwater production. The existing systems, however, often suffer from poor stability and biofouling issues, which severely hamper their prospects in practical applications. Conventionally, photothermal materials are deposited on the membrane supports via vacuum-assisted filtration or dip-coating methods. Nevertheless, the weak inherent material-membrane interactions frequently lead to poor durability, and the photothermal material layer can be easily peeled off from the hosting substrates or partially dissolved when immersed in water. In the present article, the discovery of the incorporation of borophene into cellulose nanofibers (CNF), enabling excellent environmental stability with a high light-to-heat conversion efficiency of 91.5% and water evaporation rate of 1.45 kg m-2 h-1 under simulated sunlight is reported. It is also demonstrated that borophene papers can be employed as an excellent active photothermal material for eliminating almost 100% of both gram-positive and gram-negative bacteria within 20 min under three sun irradiations. The result opens a new direction for the design of borophene-based papers with unique photothermal properties which can be used for the effective treatment of a wide range of wastewaters.

Inorganic Halide Perovskite Quantum Dots: A Versatile Nanomaterial Platform for Electronic Applications.

Metal halide perovskites have generated significant attention in recent years because of their extraordinary physical properties and photovoltaic performance. Among these, inorganic perovskite quantum dots (QDs) stand out for their prominent merits, such as quantum confinement effects, high photoluminescence quantum yield, and defect-tolerant structures. Additionally, ligand engineering and an all-inorganic composition lead to a robust platform for ambient-stable QD devices. This review presents the state-of-the-art research progress on inorganic perovskite QDs, emphasizing their electronic applications. In detail, the physical properties of inorganic perovskite QDs will be introduced first, followed by a discussion of synthesis methods and growth control. Afterwards, the emerging applications of inorganic perovskite QDs in electronics, including transistors and memories, will be presented. Finally, this review will provide an outlook on potential strategies for advancing inorganic perovskite QD technologies.

Low-Dimensional Metal-Halide Perovskites as High-Performance Materials for Memory Applications.

Metal-halide perovskites have drawn profuse attention during the past decade, owing to their excellent electrical and optical properties, facile synthesis, efficient energy conversion, and so on. Meanwhile, the development of information storage technologies and digital communications has fueled the demand for novel semiconductor materials. Low-dimensional perovskites have offered a new force to propel the developments of the memory field due to the excellent physical and electrical properties associated with the reduced dimensionality. In this review, the mechanisms, properties, as well as stability and performance of low-dimensional perovskite memories, involving both molecular-level perovskites and structure-level nanostructures, are comprehensively reviewed. The property-performance correlation is discussed in-depth, aiming to present effective strategies for designing memory devices based on this new class of high-performance materials. Finally, the existing challenges and future opportunities are presented.

High-κ perovskite membranes as insulators for two-dimensional transistors.

The scaling of silicon metal-oxide-semiconductor field-effect transistors has followed Moore's law for decades, but the physical thinning of silicon at sub-ten-nanometre technology nodes introduces issues such as leakage currents1. Two-dimensional (2D) layered semiconductors, with an atomic thickness that allows superior gate-field penetration, are of interest as channel materials for future transistors2,3. However, the integration of high-dielectric-constant (κ) materials with 2D materials, while scaling their capacitance equivalent thickness (CET), has proved challenging. Here we explore transferrable ultrahigh-κ single-crystalline perovskite strontium-titanium-oxide membranes as a gate dielectric for 2D field-effect transistors. Our perovskite membranes exhibit a desirable sub-one-nanometre CET with a low leakage current (less than 10-2 amperes per square centimetre at 2.5 megavolts per centimetre). We find that the van der Waals gap between strontium-titanium-oxide dielectrics and 2D semiconductors mitigates the unfavourable fringing-induced barrier-lowering effect resulting from the use of ultrahigh-κ dielectrics4. Typical short-channel transistors made of scalable molybdenum-disulfide films by chemical vapour deposition and strontium-titanium-oxide dielectrics exhibit steep subthreshold swings down to about 70 millivolts per decade and on/off current ratios up to 107, which matches the low-power specifications suggested by the latest International Roadmap for Devices and Systems5.

Tuning Phase Transition and Thermochromic Properties of Vanadium Dioxide Thin Films via Cobalt Doping.

Vanadium dioxide (VO2) featuring a distinct thermally triggered phase transition is regarded as the most attractive thermochromic material for smart window applications. However, the high transition temperature (∼67 °C) and moderate luminous transmittance (<50%) of the pristine VO2 circumvent room temperature applications. In this work, epitaxial cobalt-doped VO2 thin films were fabricated to tailor the electric and optical properties on a c-plane sapphire substrate. At the highest doping concentration of 10%, the transition temperature of VO2 is reduced to 44 °C, accompanied by a high luminous transmittance of 79% for single-element Co-doped VO2. The roles of cobalt doping and detailed band variation are fully explained experimentally and by modeling (DFT calculation), respectively. Furthermore, the dramatically increased carrier concentration in cobalt-doped VO2 underscores the promising future of cobalt-doped VO2 unveiled by temperature-dependent Hall effect measurement.

Anomalous Structural Evolution and Glassy Lattice in Mixed-Halide Hybrid Perovskites.

Hybrid halide perovskites have emerged as highly promising photovoltaic materials because of their exceptional optoelectronic properties, which are often optimized via compositional engineering like mixing halides. It is well established that hybrid perovskites undergo a series of structural phase transitions as temperature varies. In this work, the authors find that phase transitions are substantially suppressed in mixed-halide hybrid perovskite single crystals of MAPbI3-x Brx (MA = CH3 NH3 + and x = 1 or 2) using a complementary suite of diffraction and spectroscopic techniques. Furthermore, as a general behavior, multiple crystallographic phases coexist in mixed-halide perovskites over a wide temperature range, and a slightly distorted monoclinic phase, hitherto unreported for hybrid perovskites, is dominant at temperatures above 100 K. The anomalous structural evolution is correlated with the glassy behavior of organic cations and optical phonons in mixed-halide perovskites. This work demonstrates the complex interplay between composition engineering and lattice dynamics in hybrid perovskites, shedding new light on their unique properties.

A flexible capacitive photoreceptor for the biomimetic retina.

Neuromorphic vision sensors have been extremely beneficial in developing energy-efficient intelligent systems for robotics and privacy-preserving security applications. There is a dire need for devices to mimic the retina's photoreceptors that encode the light illumination into a sequence of spikes to develop such sensors. Herein, we develop a hybrid perovskite-based flexible photoreceptor whose capacitance changes proportionally to the light intensity mimicking the retina's rod cells, paving the way for developing an efficient artificial retina network. The proposed device constitutes a hybrid nanocomposite of perovskites (methyl-ammonium lead bromide) and the ferroelectric terpolymer (polyvinylidene fluoride trifluoroethylene-chlorofluoroethylene). A metal-insulator-metal type capacitor with the prepared composite exhibits the unique and photosensitive capacitive behavior at various light intensities in the visible light spectrum. The proposed photoreceptor mimics the spectral sensitivity curve of human photopic vision. The hybrid nanocomposite is stable in ambient air for 129 weeks, with no observable degradation of the composite due to the encapsulation of hybrid perovskites in the hydrophobic polymer. The functionality of the proposed photoreceptor to recognize handwritten digits (MNIST) dataset using an unsupervised trained spiking neural network with 72.05% recognition accuracy is demonstrated. This demonstration proves the potential of the proposed sensor for neuromorphic vision applications.

Electrode Engineering in Halide Perovskite Electronics: Plenty of Room at the Interfaces.

Contact engineering is a prerequisite for achieving desirable functionality and performance of semiconductor electronics, which is particularly critical for organic-inorganic hybrid halide perovskites due to their ionic nature and highly reactive interfaces. Although the interfaces between perovskites and charge-transporting layers have attracted lots of attention due to the photovoltaic and light-emitting diode applications, achieving reliable perovskite/electrode contacts for electronic devices, such as transistors and memories, remains as a bottleneck. Herein, a critical review on the elusive nature of perovskite/electrode interfaces with a focus on the interfacial electrochemistry effects is presented. The basic guidelines of electrode selection are given for establishing non-polarized interfaces and optimal energy level alignment for perovskite materials. Furthermore, state-of-the-art strategies on interface-related electrode engineering are reviewed and discussed, which aim at achieving ohmic transport and eliminating hysteresis in perovskite devices. The role and multiple functionalities of self-assembled monolayers that offer a unique approach toward improving perovskite/electrode contacts are also discussed. The insights on electrode engineering pave the way to advancing stable and reliable perovskite devices in diverse electronic applications.

Quantum Dot Passivation of Halide Perovskite Films with Reduced Defects, Suppressed Phase Segregation, and Enhanced Stability.

Structural defects are ubiquitous for polycrystalline perovskite films, compromising device performance and stability. Herein, a universal method is developed to overcome this issue by incorporating halide perovskite quantum dots (QDs) into perovskite polycrystalline films. CsPbBr3 QDs are deposited on four types of halide perovskite films (CsPbBr3 , CsPbIBr2 , CsPbBrI2 , and MAPbI3 ) and the interactions are triggered by annealing. The ions in the CsPbBr3 QDs are released into the thin films to passivate defects, and concurrently the hydrophobic ligands of QDs self-assemble on the film surfaces and grain boundaries to reduce the defect density and enhance the film stability. For all QD-treated films, PL emission intensity and carrier lifetime are significantly improved, and surface morphology and composition uniformity are also optimized. Furthermore, after the QD treatment, light-induced phase segregation and degradation in mixed-halide perovskite films are suppressed, and the efficiency of mixed-halide CsPbIBr2 solar cells is remarkably improved to over 11% from 8.7%. Overall, this work provides a general approach to achieving high-quality halide perovskite films with suppressed phase segregation, reduced defects, and enhanced stability for optoelectronic applications.

Halide Perovskites: A New Era of Solution-Processed Electronics.

Organic-inorganic mixed halide perovskites have emerged as an excellent class of materials with a unique combination of optoelectronic properties, suitable for a plethora of applications ranging from solar cells to light-emitting diodes and photoelectrochemical devices. Recent works have showcased hybrid perovskites for electronic applications through improvements in materials design, processing, and device stability. Herein, a comprehensive up-to-date review is presented on hybrid perovskite electronics with a focus on transistors and memories. These applications are supported by the fundamental material properties of hybrid perovskite semiconductors such as tunable bandgap, ambipolar charge transport, reasonable mobility, defect characteristics, and solution processability, which are highlighted first. Then, recent progresses on perovskite-based transistors are reviewed, covering aspects of fabrication process, patterning techniques, contact engineering, 2D versus 3D material selection, and device performance. Furthermore, applications of perovskites in nonvolatile memories and artificial synaptic devices are presented. The ambient instability of hybrid perovskites and the strategies to tackle this bottleneck are also discussed. Finally, an outlook and opportunities to develop perovskite-based electronics as a competitive and feasible technology are highlighted.

Flexible and efficient perovskite quantum dot solar cells via hybrid interfacial architecture.

All-inorganic CsPbI3 perovskite quantum dots have received substantial research interest for photovoltaic applications because of higher efficiency compared to solar cells using other quantum dots materials and the various exciting properties that perovskites have to offer. These quantum dot devices also exhibit good mechanical stability amongst various thin-film photovoltaic technologies. We demonstrate higher mechanical endurance of quantum dot films compared to bulk thin film and highlight the importance of further research on high-performance and flexible optoelectronic devices using nanoscale grains as an advantage. Specifically, we develop a hybrid interfacial architecture consisting of CsPbI3 quantum dot/PCBM heterojunction, enabling an energy cascade for efficient charge transfer and mechanical adhesion. The champion CsPbI3 quantum dot solar cell has an efficiency of 15.1% (stabilized power output of 14.61%), which is among the highest report to date. Building on this strategy, we further demonstrate a highest efficiency of 12.3% in flexible quantum dot photovoltaics.

An efficient and stable solar flow battery enabled by a single-junction GaAs photoelectrode.

Converting and storing solar energy and releasing it on demand by using solar flow batteries (SFBs) is a promising way to address the challenge of solar intermittency. Although high solar-to-output electricity efficiencies (SOEE) have been recently demonstrated in SFBs, the complex multi-junction photoelectrodes used are not desirable for practical applications. Here, we report an efficient and stable integrated SFB built with back-illuminated single-junction GaAs photoelectrode with an n-p-n sandwiched design. Rational potential matching simulation and operating condition optimization of this GaAs SFB lead to a record SOEE of 15.4% among single-junction SFB devices. Furthermore, the TiO2 protection layer and robust redox couples in neutral pH electrolyte enable the SFB to achieve stable cycling over 408 h (150 cycles). These results advance the utilization of more practical solar cells with higher photocurrent densities but lower photovoltages for high performance SFBs and pave the way for developing practical and efficient SFBs.

Optimizing Surface Chemistry of PbS Colloidal Quantum Dot for Highly Efficient and Stable Solar Cells via Chemical Binding.

The surface chemistry of colloidal quantum dots (CQD) play a crucial role in fabricating highly efficient and stable solar cells. However, as-synthesized PbS CQDs are significantly off-stoichiometric and contain inhomogeneously distributed S and Pb atoms at the surface, which results in undercharged Pb atoms, dangling bonds of S atoms and uncapped sites, thus causing surface trap states. Moreover, conventional ligand exchange processes cannot efficiently eliminate these undesired atom configurations and defect sites. Here, potassium triiodide (KI3) additives are combined with conventional PbX2 matrix ligands to simultaneously eliminate the undercharged Pb species and dangling S sites via reacting with molecular I2 generated from the reversible reaction KI3 â‡Œ I2 + KI. Meanwhile, high surface coverage shells on PbS CQDs are built via PbX2 and KI ligands. The implementation of KI3 additives remarkably suppresses the surface trap states and enhances the device stability due to the surface chemistry optimization. The resultant solar cells achieve the best power convention efficiency of 12.1% and retain 94% of its initial efficiency under 20 h continuous operation in air, while the control devices with KI additive deliver an efficiency of 11.0% and retains 87% of their initial efficiency under the same conditions.

Highly UV Resistant Inch-Scale Hybrid Perovskite Quantum Dot Papers.

Halide perovskite quantum dots (PQDs) are promising materials for diverse applications including displays, light-emitting diodes, and solar cells due to their intriguing properties such as tunable bandgap, high photoluminescence quantum yield, high absorbance, and narrow emission peaks. Despite the prosperous achievements over the past several years, PQDs face severe challenges in terms of stability under different circumstances. Currently, researchers have overcome part of the stability problem, making PQDs sustainable in water, oxygen, and polar solvents for long-term use. However, halide PQDs are easily degraded under continuous irradiation, which significantly limits their potential for conventional applications. In this study, an oleic acid/oleylamine (traditional surface ligands)-free method to fabricate perovskite quantum dot papers (PQDP) is developed by adding cellulose nanocrystals as long-chain binding ligands that stabilize the PQD structure. As a result, the relative photoluminescence intensity of PQDP remains over ≈90% under continuous ultraviolet (UV, 16 W) irradiation for 2 months, showing negligible photodegradation. This proposed method paves the way for the fabrication of ultrastable PQDs and the future development of related applications.

Enhancing the Efficiency and Stability of PbS Quantum Dot Solar Cells through Engineering an Ultrathin NiO Nanocrystalline Interlayer.

Significant progress in PbS quantum dot solar cells has been achieved through designing device architecture, engineering band alignment, and optimizing the surface chemistry of colloidal quantum dots (CQDs). However, developing a highly stable device while maintaining the desirable efficiency is still a challenging issue for these emerging solar cells. In this study, by introducing an ultrathin NiO nanocrystalline interlayer between Au electrodes and the hole-transport layer of the PbS-EDT, the resulting PbS CQD solar cell efficiency is improved from 9.3 to 10.4% because of the improved hole-extraction efficiency. More excitingly, the device stability is significantly enhanced owing to the passivation effect of the robust NiO nanocrystalline interlayer. The solar cells with the NiO nanocrystalline interlayer retain 95 and 97% of the initial efficiency when heated at 80 °C for 120 min and treated with oxygen plasma irradiation for 60 min, respectively. In contrast, the control devices without the NiO nanocrystalline interlayer retain only 75 and 63% of the initial efficiency under the same testing conditions.