Silver coordination-induced n-doping of PCBM for stable and efficient inverted perovskite solar cells.

The bidirectional migration of halides and silver causes irreversible chemical corrosion to the electrodes and perovskite layer, affecting long-term operation stability of perovskite solar cells. Here we propose a silver coordination-induced n-doping of [6,6]-phenyl-C61-butyric acid methyl ester strategy to safeguard Ag electrode against corrosion and impede the migration of iodine within the PSCs. Meanwhile, the coordination between DCBP and silver induces n-doping in the PCBM layer, accelerating electron extraction from the perovskite layer. The resultant PSCs demonstrate an efficiency of 26.03% (certified 25.51%) with a minimal non-radiative voltage loss of 126 mV. The PCE of resulting devices retain 95% of their initial value after 2500 h of continuous maximum power point tracking under one-sun irradiation, and > 90% of their initial value even after 1500 h of accelerated aging at 85 °C and 85% relative humidity.

Development of Quasi-Two-Dimensional Perovskites and Their Application in Light-Emitting Diodes.

Quasi-two-dimensional (quasi-2D) perovskites have attracted much attention due to their outstanding properties, such as inherent quantum-well structure, strong dielectric and quantum confinement, large exciton binding energy, and high photoluminescence quantum yield. By virtue of these superior merits, quasi-2D perovskites have shown great potential for next-generation light-emitting diodes (LEDs). Herein, this review presents an overview of the basic properties of quasi-2D perovskites and their photoluminescence modulations by large organic cation engineering, monovalent cation engineering, halogen engineering, defect passivation engineering, and dimensionality engineering. Furthermore, the strategies of charge-transport layer optimization, interfacial engineering, light-outcoupling efficiency improvement, and operating stability improvement are summarized for fabricating high-performance quasi-2D perovskite LEDs (PeLEDs). Finally, the challenges and outlook for the future development of quasi-2D PeLEDs are unambiguously proposed.

Broadband Near-Infrared Emission from 0D Hybrid Copper Halides.

Metal halides have attracted increasing attention owing to their outstanding optoelectronic properties and tunable emission characteristics. Among these, low-dimensional metal halides have emerged as a novel and efficient luminescent material, primarily attributed to their broad spectral emission induced by self-trapped excitons (STEs). However, achieving highly efficient deep red and near-infrared (NIR) emission in metal halides remains a challenge. In this study, we report a novel zero-dimensional (0D) copper-based metal halide [Na2(DMSO)8]Cu4Br6 as the NIR light source, which exhibits a full width at half-maximum (FWHM) of 195 nm peaking at 685 nm, an impressive quantum efficiency of 68% and a large Stokes shift of 299 nm. Through comprehensive spectral analysis and meticulous data calculations, we substantiate that the emission originates from STEs formed within the 0D structure. Furthermore, we demonstrate the potential application of [Na2(DMSO)8]Cu4Br6 as an invisible light source in night vision by combining it with a commercially available 365 nm ultraviolet (UV) chip. This work not only enriches the family of low-dimensional metal halide materials but also inspires the potential of low-dimensional metal halides in night vision applications.

Multidentate Chelation Achieves Bilateral Passivation toward Efficient and Stable Perovskite Solar Cells with Minimized Energy Losses.

Defects in the electron transport layer (ETL), perovskite, and buried interface will result in considerable nonradiative recombination. Here, a bottom-up bilateral modification strategy is proposed by incorporating arsenazo III (AA), a chromogenic agent for metal ions, to regulate SnO2 nanoparticles. AA can complex with uncoordinated Sn4+/Pb2+ in the form of multidentate chelation. Furthermore, by forming a hydrogen bond with formamidinium (FA), AA can suppress FA+ defects and regulate crystallization. Multiple chemical bonds between AA and functional layers are established, synergistically preventing the agglomeration of SnO2 nanoparticles, enhancing carrier transport dynamics, passivating bilateral defects, releasing tensile stress, and promoting the crystallization of perovskite. Ultimately, the AA-optimized power conversion efficiency (PCE) of the methylammonium-free (MA-free) devices (Rb0.02(FA0.95Cs0.05)0.98PbI2.91Br0.03Cl0.06) is boosted from 20.88% to 23.17% with a high open-circuit voltage (VOC) exceeding 1.18 V and ultralow energy losses down to 0.37 eV. In addition, the optimized devices also exhibit superior stability.

Water-Molecule-Induced Reversible Fluorescence in a One-Dimensional Mn-Based Hybrid Halide for Anticounterfeiting and Digital Encryption-Decryption.

Hybrid metal halides with reversible transformation of structure and luminescence properties have attracted significant attention in anticounterfeiting. However, their long transition time and slow response rate may hinder the rapid identification of confidential information. Here, a one-dimensional hybrid manganese-based halide, i.e., (C5H11N3)MnCl2Br2·H2O, is prepared and demonstrates the phenomenon of water-molecule-induced reversible photoluminescence transformation. Heating for <40 s induces a dynamic transfer of red-emissive (C5H11N3)MnCl2Br2·H2O to green-emissive (C5H11N3)MnCl2Br2. In addition, the green emission can gradually revert to red emission during a cooling process in a moist environment, demonstrating excellent reversibility. It is found that the water molecule acts as an external stimulus to realize the reversible transition between red and green emission, which also exhibits remarkable stability during repeated cycles. Furthermore, with the assistance of heating and cooling, a complex digital encryption-decryption and an optical "AND" logical gate are achieved, facilitating the development of anticounterfeiting information security.

Additive Conformational Engineering To Improve the PbI2 Framework for Efficient and Stable Perovskite Solar Cells.

The PbI2 framework is critical for two-step fabricated perovskite solar cells. This study investigates the effects of introducing two functional urea-based molecules, biuret (BU) and dithiobiuret (DTBU), into the PbI2 precursor solution on the absorber layer and overall device performance. BU, which contains C═O, enhanced device performance and stability, whereas DTBU, which contains C═S, had negative effects. Research analysis revealed the differences in the spatial structures of the two urea-based molecules. The introduction of symmetrical BU molecules facilitated the crystallization of PbI2, whereas the introduction of DTBU with a twisted molecular structure led to inferior crystallization performance of PbI2. The perovskite thin film, obtained by introducing BU into the PbI2 precursor solution, demonstrated superior performance, characterized by a decreased defect density and an extended carrier lifetime. The device performance and stability were enhanced, resulting in higher open-circuit voltage and fill factor. The highest achieved power conversion efficiency was 23.50%. After 1300 h of storage under unpackaged conditions at 30-40% humidity, the devices maintained 93% of their initial efficiency. Conversely, the devices prepared with DTBU doping exhibited inferior performance and stability, displaying power conversion efficiency below 10% and faster degradation under the same humidity conditions.

Low-Temperature Solution Synthesis of Stable Cs3Cu2Br5 Single Crystals for Visible Light Communications.

Inorganic perovskites CsPbX3 (X = Cl, Br, I) have shown great potential as luminescent materials for a wide range of photoelectric devices. However, the practical use of these materials is limited due to the toxicity of lead and poor stability. Here, we present a facile low-temperature, solution-based method to synthesize lead-free and highly stable Cs3Cu2Br5 single crystals (SCs) without the use of organic solvents. Owing to the self-trapped exciton emissions, Cs3Cu2Br5 SCs exhibit a strong broadband blue emission with a high photoluminescence quantum yield (PLQY) upon 254 nm ultraviolet light excitation. In addition, the Cs3Cu2Br5 SCs show a high stability against heat, humidity, and UV light. Therefore, the Cs3Cu2Br5 SCs are utilized as emitters in white light emitting diodes (WLEDs), demonstrating a high color rendering index of 81 and a decent commission internationale de l'Eclairage coordinate of (0.30, 0.34). Furthermore, the prepared WLEDs are used in wireless visible light communications, showing a -3 dB bandwidth of 6.7 MHz and an achievable data rate of 45 Mbps. Our study provides a novel organic-solvent-free, low-temperature method to synthesize Cs3Cu2Br5 SCs and could promote the development of Cu-based metal halides in visible light communications.

Suppressing Phase Segregation in CsPbIBr2 Films via Anchoring Halide Ions toward Underwater Solar Cells.

Inorganic CsPbIBr2 perovskite solar cells (PSCs) have accomplished many milestones, yet their progress has been constrained by ion migration and phase separation. This study explores the modulation of perovskite crystallization kinetics and halide ion migration through chlorobenzene (CB) antisolvent with bis(pentafluorophenyl)zinc (Zn(C6F5)2) additive. The photoluminescence and absorption spectra reveal the significantly reduced phase segregaton in CsPbIBr2 film treated by CB with Zn(C6F5)2. Moreover, this research analyzes the CsPbIBr2 film's free carrier lifetime, diffusion length, and mobility using time-resolved microwave conductivity and transient absorption spectroscopy after Zn(C6F5)2 modification. Consequently, the modified CsPbIBr2 PSCs offer a 12.57% power conversion efficiency (PCE), the highest value among CsPbIBr2 PSCs with negligible hysteresis and prolonged stability. Furthermore, under 1-m-deep water, CsPbIBr2 PSCs display a PCE of 14.18%. These findings provide an understanding of the development of phase-segregation-free CsPbIBr2 films and showcase the prospective applications of CsPbIBr2 PSCs in underwater power systems.

Flexible perovskite scintillators and detectors for X-ray detection.

X-ray detection and imaging technology has been rapidly developed for various fields since 1895, offering great opportunities to scientific and industrial communities. Particularly, flexible X-ray detectors have drawn numerous attention in medical-related applications, solving the uniform issues of traditional rigid X-ray detectors. Out of all the potential materials, metal halide perovskites (MHPs) have been emerged as excellent candidates as flexible X-ray scintillators and detectors owing to the advantages including low temperature solution processable, strong X-ray absorption coefficient, large mobility lifetime product and tunable bandgap. In this review, the recent advances of MHP-based flexible X-ray detectors are comprehensively summarized, focusing on the scalable synthesis technologies of materials and diverse device architectures, and covering both direct and indirect X-ray detection. A brief outlook that highlights the current challenges impeding the commercialization of flexible MHP-based X-ray detectors is also included with possible solutions to those problem being provided.

Significant performance enhancement of UV-Vis self-powered CsPbBr3 quantum dot-based photodetectors induced by ligand modification and P3HT embedding.

In this work, we report a novel, to the best of our knowledge, strategy to improve the performance of UV-Vis self-powered CsPbBr3 quantum dot (QD) based photodetectors (PDs) by ligand modification and poly(3-hexylthiophene) (P3HT) embedding. Compared with those based on pure QDs, modified PDs show a shortened response time by nearly ten times, and increases of maximum responsivity and specific detectivity by nearly 45 and 97 times, respectively. Such PDs also show a high stability with 90% of the initial photocurrent being maintained even after storage in ambient air without any encapsulation for 30 days.

All-Inorganic Lead-Free Perovskite(-Like) Single Crystals: Synthesis, Properties, and Applications.

Due to their nontoxicity, stability, and unique optoelectronic properties, all-inorganic lead-free halide semiconductors with perovskite and perovskite-like structures have successfully emerged as promising optoelectronic materials for various applications, such as solar cells, light-emitting diodes (LEDs), photodetectors, and X-ray detectors. To further explore their practical potentials, researchers have paid more attention in all-inorganic lead-free perovskite (-like) (ILFP) single crystals. For these single crystals, the advantages of large sizes, uniform surface morphology, and few defects can facilitate their excellent performances and practical applications. Besides, compared with the low dimensional and polycrystalline ILFP materials, the ILFP single crystals feature enhanced performances, including a longer carrier diffusion length and a larger light absorption coefficient, which attract a great deal of attention. Therefore, focus is on the researching progress of ILFP single crystals and the development of their preparation methods, as well as the novel properties of ILFP single crystals. In addition, the reported applications of ILFP single crystals are proposed to highlight their practical importance. With the perspective of the evolution and challenges, the current limitations of the materials and devices are discussed, followed by an inspirational outlook on their future development directions.

Photoluminescent Semiconducting Graphene Nanoribbons via Longitudinally Unzipping Single-Walled Carbon Nanotubes.

The lack of a sizeable band gap has so far prevented graphene from building effective electronic and optoelectronic devices despite its numerous exceptional properties. Intensive theoretical research reveals that a band gap larger than 1 eV can only be achieved in sub-3 nm wide graphene nanoribbons (GNRs), but real fabrication of such ultranarrow GNRs still remains a critical challenge. Herein, we demonstrate an approach for the synthesis of ultranarrow and photoluminescent semiconducting GNRs by longitudinally unzipping single-walled carbon nanotubes. Atomic force microscopy reveals the unzipping process, and the resulting 2.2 nm wide GNRs are found to emit strong and sharp photoluminescence at ∼685 nm, demonstrating a very desirable semiconducting nature. This band gap of 1.8 eV is further confirmed by follow-up photoconductivity measurements, where a considerable photocurrent is generated, as the excitation wavelength becomes shorter than 700 nm. More importantly, our fabricated GNR field-effect transistors (FETs), by employing the hexagonal boron nitride-encapsulated heterostructure to achieve edge-bonded contacts, demonstrate a high current on/off ratio beyond 105 and carrier mobility of 840 cm2/V s, approaching the theoretical scattering limit in semiconducting GNRs at room temperature. Especially, highly aligned GNR bundles with lengths up to a millimeter are also achieved by prepatterning a template, and the fabricated GNR bundle FETs show a high on/off ratio reaching 105, well-defined saturation currents, and strong light-emitting properties. Therefore, GNRs produced by this method open a door for promising applications in graphene-based electronics and optoelectronics.

Room temperature synthesis of Sn2+ doped highly luminescent CsPbBr3 quantum dots for high CRI white light-emitting diodes.

With a high photoluminescence quantum yield (PLQY) being able to exceed 90% for those prepared by the hot injection method, CsPbBr3 quantum dots (QDs) have attracted intensive attention for white light-emitting diodes (WLEDs). However, the whole process is carried out in a 3-neck flask via air isolation and at a relatively high temperature. In addition, CsPbBr3 QDs suffer from poor stability under ambient atmosphere. In this work, an effective strategy through doping of Sn2+ ions at room-temperature is proposed to improve the emission efficiency and stability of CsPbBr3 QDs. Compared with pure CsPbBr3 QDs, a higher PLQY and a better stability are obtained. The detailed physical mechanism for this performance enhancement is discussed and described. An optimum result is found at an Sn2+ doping amount of 20%, which shows a high PLQY of 82.77%. WLEDs based on these 20% Sn2+ doped CsPbBr3 QDs are also studied, exhibiting a high color rendering index of 89 and a correlated color temperature (CCT) of 3954. The method proposed here provides an effective strategy to enhance the fluorescence and stability of CsPbBr3 QDs, which might have promising potential in the lighting fields.

Challenges and strategies relating to device function layers and their integration toward high-performance inorganic perovskite solar cells.

Parallel to the flourishing of inorganic-organic hybrid perovskite solar cells (PSCs), the development of inorganic cesium-based metal halide PSCs (CsPbX3) is accelerating, with power conversion efficiency (PCE) values of over 20% being obtained. Although CsPbX3 possesses numerous merits, such as superior thermal stability and great potential for use in tandem solar cells, severe challenges remain, such as its phase instability, trap state density, and absorption range limitations, hindering further performance improvements and commercialization. This review summarizes challenges and strategies relating to each device functional layer and their integration for the purposes of performance improvement and commercialization, utilizing the fundamental configuration of a perovskite photo-absorption layer, electron transport layer (ETL), and hole transport layer (HTL ). In detail, we first analyze comprehensively strategies for designing high-quality CsPbX3 perovskite films, including precursor engineering, element doping, and post-treatment, followed by discussing the precise control of the CsPbX3 film fabrication process. Then, we introduce and analyze the carrier dynamics and interfacial modifications of inorganic ETLs, such as TiO2, SnO2, ZnO, and other typical organic ETLs with p-i-n configuration. The pros and cons of inorganic and organic HTLs are then discussed from the viewpoints of stability and band structure. Subsequently, promising candidates, i.e., HTL-free carbon-electrode-based inorganic CsPbX3 PSCs, that meet the "golden triangle" criteria used by the PSC community are reviewed, followed by discussion of other obstacles, such as hysteresis and large-scale fabrication, that lie on the road toward PSC commercialization. Finally, some perspectives relating to solutions to development bottlenecks are proposed, with the attempt to gain insight into CsPbX3 PSCs and inspire future research prospects.

Transparent Thin-Film Transistors Based on Sputtered Electric Double Layer.

Electric-double-layer (EDL) thin-film transistors (TFTs) have attracted much attention due to their low operation voltages. Recently, EDL TFTs gated with radio frequency (RF) magnetron sputtered SiO2 have been developed which is compatible to large-area electronics fabrication. In this work, fully transparent Indium-Gallium-Zinc-Oxide-based EDL TFTs on glass substrates have been fabricated at room temperature for the first time. A maximum transmittance of about 80% has been achieved in the visible light range. The transparent TFTs show a low operation voltage of 1.5 V due to the large EDL capacitance (0.3 µF/cm² at 20 Hz). The devices exhibit a good performance with a low subthreshold swing of 130 mV/dec and a high on-off ratio > 105. Several tests have also been done to investigate the influences of light irradiation and bias stress. Our results suggest that such transistors might have potential applications in battery-powered transparent electron devices.

A Sputtered Silicon Oxide Electrolyte for High-Performance Thin-Film Transistors.

Low operating voltages have been long desired for thin-film transistors (TFTs). However, it is still challenging to realise 1-V operation by using conventional dielectrics due to their low gate capacitances and low breakdown voltages. Recently, electric double layers (EDLs) have been regarded as a promising candidate for low-power electronics due to their high capacitance. In this work, we present the first sputtered SiO2 solid-state electrolyte. In order to demonstrate EDL behaviour, a sputtered 200 nm-thick SiO2 electrolyte was incorporated into InGaZnO TFTs as the gate dielectric. The devices exhibited an operating voltage of 1 V, a threshold voltage of 0.06 V, a subthreshold swing of 83 mV dec-1 and an on/off ratio higher than 105. The specific capacitance was 0.45 µF cm-2 at 20 Hz, which is around 26 times higher than the value obtained from thermally oxidised SiO2 films with the same thickness. Analysis of the microstructure and mass density of the sputtered SiO2 films under different deposition conditions indicates that such high capacitance might be attributed to mobile protons donated by atmospheric water. The InGaZnO TFTs with the optimised SiO2 electrolyte also showed good air stability. This work provides a new pathway to the realisation of high-yield low-power electronics.