Lignin, a byproduct from the pulp industry, is one of the redox active biopolymers being investigated as a component in the electrodes for sustainable energy storage applications. Due to its insulating nature, it needs to be combined with a conductor such as carbon or conducting polymer for efficient charge storage. Here, the lignin/carbon composite electrodes manufactured via mechanical milling (ball milling) are reported. The composite formation, correlation between performance and morphology is studied by comparison with manual mixing and jet milling. Superior charge storage capacity with approximate to 70% of the total contribution from the Faradaic process involving the redox functionality of lignin is observed in a mechanically milled composite. In comparison, manual mix shows only approximate to 30% from the lignin storage participation while the rest is due to the electric double layer at the carbon-electrolyte interface. The significant participation of lignin in the ball milled composite is attributed to the homogeneous, intimate mixing of the carbon and the lignin leading the electronic carrier transported in the carbon phase to reach most of the redox group of lignin. A maximum capacity of 49 mAh g(-1) is obtained at charge/discharge rate of 0.25 A g(-1) for the sample milled for 60 min.

The key figure-of-merit for materials in stationary energy storage applications, such as large-scale energy storage for buildings and grids, is the cost per kilo per electrochemical cycle, rather than the energy density. In this regard, forest-based biopolymers such as lignin, are attractive, as they are abundant on Earth. Here, we explored lignin as an electroactive battery material, able to store two electrons per hydroquinone aromatic ring, with the targeted operation in aqueous electrolytes. The impact of the sulfonation level of lignin on the performance of its composite electrode with carbon was investigated by considering three lignin derivatives: lignosulfonate (LS), partially desulfonated lignosulfonate (DSLS), and fully desulfonated lignin (KL, lignin produced by the kraft process). Partial desulfonation helped in better stability of the composite in aqueous media, simultaneously favoring its water processability. In this way, a route to promote ionic conductivity within the lignin/carbon composite electrodes was developed, facilitating the access to the entire bulk of the volumetric electrodes. Electrochemical performance of DSLS/C showed highly dominant Faradaic contribution (66%) towards the total capacity, indicating an efficient mixed ionic-electronic transport within the lignin-carbon phase, displaying a capacity of 38 mAh/g at 0.25 A/g and 69% of capacity retention after 2200 cycles at a rate of 1 A/g.

A trihybrid bioelectrode composed of lignin, poly(3,4-ethylenedioxythiophene) (PEDOT), and poly(aminoanthraquinone) (PAAQ) is prepared by a two-step galvanostatic electropolymerization, and characterized for supercapacitor applications. Using PEDOT/Lignin as a base layer, followed by the consecutive deposition of PAAQ, the hybrid electrode PEDOT/Lignin/PAAQ shows a high specific capacitance of 418 F g(-1) with small self-discharge. This trihybrid electrode material can be assembled into symmetric and asymmetric super-capacitors. The asymmetric supercapacitor uses PEDOT + Lignin/PAAQ as positive electrode and PEDOT/PAAQ as negative electrode, and exhibits superior electrochemical performance due to the synergistic effect of the two electrodes, which leads to a specific capacitance of 74 F g(-1). It can be reversibly cycled in the voltage range of 0-0.7 V. More than 80% capacitance is retained after 10 000 cycles. These remarkable features reveal the exciting potential of a full organic energy storage device with long cycle life.

Perovskite solar cells (per-SCs) with high performance and cost-effective solution processing have been the center of interest for researchers in the past decade. Power conversion efficiencies (PCEs) have been gradually improved up to 25.2% with relatively improved stability, which is an unparalleled progress in all generations of solar cell (SC) technology. However, there are still some prevailing challenges regarding the stability and upscaling of these promising devices. Recently, 2D layered materials (LMs) have been extensively explored to overcome the prevailing challenges of poor stability (under moisture, light soaking and high temperature), halide segregation, hysteresis, involvement of toxic materials (i.e., lead), and upscaling of devices. A critical review addressing the recent developments in the use of 2D materials, especially transition metal dichalcogenides (TMDCs), is hence necessary. The development of novel synthesis and deposition techniques including liquid-metal synthesis and ultrasonic assisted spray pyrolysis has offered more efficient fabrication of 2D-LMs with controlled thickness and morphology. Effective functionalization approaches to increase the dispersability of 2D-LMs in non-polar solvents has boosted their potential application in solar cell technology as well. Moreover, compositing 2D TMDCs with suitable organic/inorganic compounds has enabled superior charge kinetics in all functional parts of per-SCs. In addition, newly developed materials such as graphyne and graphdyine along with 2D metal organic frameworks (MOFs) and covalent organic frameworks (COFs) have been employed in per-SCs to achieve PCEs up to 20%. This review summarizes the recent progress and challenges in the application of 2D-LMs in per-SCs and outlines the future pathways to further extend the PCE of per-SCs beyond 25%. This review particularly focuses on 2D-LMs as electrode materials and additives, the underlying charge (electron-hole) transport phenomenon in the functional layers, and their chemical and structural stability.

Three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0 % benzene (P-0), to 50 % (P-50), and 75 % (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S cm and Power factors of 13.2 mu Wm(-1) K-2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.

Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO2 substrate. Na+ was employed as the crucial cement to direct Au single atoms onto TiO2, while the light-induced electron transfer from excited TiO2 to Au(Na+) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO2. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h(-1) that exceeded other Au/TiO2-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.

In virtually all solar cells, including optimized ones that operate close to the Shockley-Queisser (SQ) limit, thermalization losses are a major, efficiency-limiting factor. In typical bulk heterojunction organic solar cells, the loss of the excess energy of photocreated charge carriers in the disorder-broadened density of states is a relatively slow process that for commonly encountered disorder values takes longer than the charge extraction time. Herein, it is demonstrated by numerical modeling that this slow relaxation can be rectified by means of a linear gradient in the donor:acceptor ratio between anode and cathode. For experimentally relevant parameters, open-circuit voltage (VOC) enhancements up to approximate to 0.2 V in combination with significant enhancements in fill factor as compared to devices without gradient are found. The VOC enhancement can be understood in terms of a simple nonequilibrium effective temperature model. Implications for existing and future organic photovoltaics (OPV) devices are discussed.

True random number generation is not thought to be possible using a classical approach but by instead exploiting quantum mechanics genuine randomness can be achieved. Here, the authors demonstrate a certified quantum random number generation using a metal-halide perovskite light emitting diode as a source of weak coherent polarisation states randomly producing an output of either 0 or 1. The recent development of perovskite light emitting diodes (PeLEDs) has the potential to revolutionize the fields of optical communication and lighting devices, due to their simplicity of fabrication and outstanding optical properties. Here we demonstrate that PeLEDs can also be used in the field of quantum technologies by implementing a highly-secure quantum random number generator (QRNG). Modern QRNGs that certify their privacy are posed to replace classical random number generators in applications such as encryption and gambling, and therefore need to be cheap, fast and with integration capabilities. Using a compact metal-halide PeLED source, we generate random numbers, which are certified to be secure against an eavesdropper, following the quantum measurement-device-independent scenario. The obtained generation rate of more than 10 Mbit s(-1), which is already comparable to commercial devices, shows that PeLEDs can work as high-quality light sources for quantum information tasks, thus opening up future applications in quantum technologies.

With the power conversion efficiency of binary polymer solar cells dramatically improved, the thermal stability of the small-molecule acceptors raised the main concerns on the device operating stability. Here, to address this issue, thiophene-dicarboxylate spacer tethered small-molecule acceptors are designed, and their molecular geometries are further regulated via the thiophene-core isomerism engineering, affording dimeric TDY-alpha with a 2, 5-substitution and TDY-beta with 3, 4-substitution on the core. It shows that TDY-alpha processes a higher glass transition temperature, better crystallinity relative to its individual small-molecule acceptor segment and isomeric counterpart of TDY-beta, and amore stablemorphology with the polymer donor. As a result, the TDY-alpha based device delivers a higher device efficiency of 18.1%, and most important, achieves an extrapolated lifetime of about 35000 hours that retaining 80% of their initial efficiency. Our result suggests that with proper geometry design, the tethered small-molecule acceptors can achieve both high device efficiency and operating stability.

Metal halide perovskites are widely used in optoelectronic devices, including solar cells, photodetectors, and light-emitting diodes. Defects in this class of low-temperature solution-processed semiconductors play significant roles in the optoelectronic properties and performance of devices based on these semiconductors. Investigating the defect properties provides not only insight into the origin of the outstanding performance of perovskite optoelectronic devices but also guidance for further improvement of performance. Defects in perovskites have been intensely studied. Here, we review the progress in defect-related physics and techniques for perovskites. We survey the theoretical and computational results of the origin and properties of defects in perovskites. The underlying mechanisms, functions, advantages, and limitations of trap state characterization techniques are discussed. We introduce the effect of defects on the performance of perovskite optoelectronic devices, followed by a discussion of the mechanism of defect treatment. Finally, we summarize and present key challenges and opportunities of defects and their role in the further development of perovskite optoelectronic devices.

Harvesting indoor light to power electronic devices for the Internet of Things has become an application scenario for emerging photovoltaics, especially utilizing organic photovoltaics (OPVs). Combined liquid- and solid-state processing, such as printing and lamination used in industry for developing indoor OPVs, also provides a new opportunity to investigate the device structure, which is otherwise hardly possible based on the conventional approach due to solvent orthogonality. This study investigates the impact of fullerene-based acceptor interlayer on the performance of conjugated polymer-fullerene-based laminated OPVs for indoor applications. We observe open-circuit voltage (V-OC) loss across the interface despite this arrangement being presumed to be ideal for optimal device performance. Incorporating insulating organic components such as polyethyleneimine (PEI) or polystyrene (PS) into fullerene interlayers decreases the work function of the cathode, leading to better energy level alignment with the active layer (AL) and reducing the V-OC loss across the interface. Neutron reflectivity studies further uncover two different mechanisms behind the V-OC increase upon the incorporation of these insulating organic components. The self-organized PEI layer could hinder the transfer of holes from the AL to the acceptor interlayer, while the gradient distribution of the PS-incorporated fullerene interlayer eliminates the thermalization losses. This work highlights the importance of structural dynamics near the extraction interfaces in OPVs and provides experimental demonstrations of interface investigation between solution-processed cathodic fullerene layer and bulk heterojunction AL.

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This chapter analyses the impacts of alloying with nitrogen on structural properties and recombination processes in GaNAs nanowires (NW). It discusses possible innovative applications of these structures in advanced nano-emitters, where the incorporation of nitrogen induces the formation of self-assembled quantum dot-like states embedded in the NWs. The structural properties of these NWs were investigated by transmission electron microcopy. An important material parameter that affects performance of the NW-based devices is carrier lifetime. The non-radiative lifetime is largely affected by the material quality both in bulk and within near-surface regions. The contribution of the surface-related recombination is known to be especially severe in GaAs-based NW structures due to a large surface-to-volume ratio and the presence of surface states participating in the non-radiative recombination processes. The revealed optical properties of the GaNAs-based NW structures may be attractive for future optoelectronic applications in advanced nano-sized light emitters which could be integrated with silicon technology.

This chapter discusses structural and optical properties of novel GaNP nanowires (NW), as well as their potential for future applications in optoelectronics and photonics. It reviews efforts devoted to the optimization of GaNP-based NWs for future applications in light-emitting devices and discusses the impacts of structural polymorphism on the radiative efficiency and band structure of the material. The chapter shows that GaNP NWs can be utilized as a source of linearly polarized light with the polarization direction that is not determined by dielectric mismatch between the NW and its surrounding. GaNP alloys are novel III–V semiconductors, which have a great potential for applications in amber-red light-emitting diodes and also as an active material in innovative intermediate the band solar cells. NWs grown under the non-optimized conditions usually suffer from various point and structural defects, which degrade the radiative efficiency.

Perovskites are a class of compounds with the general formula ABX₃ and becoming increasingly attractive recently. Because this kind of material possesses various advantages such as abundant raw materials, easy synthesis, excellent photoelectric properties, and short production process. As one of the applications for lead-based perovskites, the perovskite solar cells have quickly enhanced their PCE from 3.8% in 2009 to over 25% within a short period. However, the problems, such as instability of the ionic crystal nature and toxicity of lead, largely hinder the lead-based perovskites towards commercialization. Therefore, it is necessary to develop new lead-free materials as alternative to lead-based perovskites, where similar structures can be formed to inherit the excellent optoelectronic properties. Moreover, new properties can be achieved due to more abundant metal candidates in lead-free materials. Based on this, we develop different kinds of perovskite-structure-like lead-free materials such as organic inorganic hybrid materials, chiral materials and double perovskites. In addition to physical and chemical properties like photoluminescence, absorption, structure, etc., we further demonstrate their potential applications according to their unique properties such as multicolor light emission.

We incorporate chiral MBA (methylbenzylamine) in inorganic metal system to obtain chiral lead-free organic inorganic hybrid materials, where significant crystallization difference is observed between rac and chiral halide compounds for the first time. Such difference is confirmed by spectrum and structural results. What’s more, we find that moisture can cause the structural transfer in chiral compounds, attributed to the asymmetric hydrogen bonding of chiral compounds. Our achievements open up new chance to improve our material property and provide new horizon for synthesis of chiral materials in the future.

Then, we obtained blue emission center in Mn-based organic and inorganic compounds by choosing organic molecule MBA. The method has basic difference with the emissions in Mn based compounds. The coexisting two emission centers of our Mn based samples is verified by spectral results. Because two emission centers can induce different PL excitation responses, so that the excitation wavelengths are capable of manipulating the emission color. Specifically, we achieve CIE coordinates of (0.33, 0.35) with a white emission. The potential of our materials in anti-counterfeiting and multicolor lighting technology are further demonstrated. Our accomplishments explore a new approach for multicolor emission in Mn based materials.

We finally obtained Sb³⁺/Cu⁺ co-doped Cs₂NaInCl₆ (CNIC) double perovskite by hydrothermal reaction which exhibits tunable dual emissions with PL quantum efficiency (PLQE) of 78%. Depending on different photoluminescence excitation (PLE) spectra between two emissions, multiple emission colors can be got by manipulating excitation wavelength. Interestingly, emission color gamut can be further tuned through manipulating the feeding ratio of Cu^I dopant, where warm color and cool color can be achieved separately. We further illustrated the application potential of our co-doped materials in the fileds of multicolor lighting devices and anti-counterfeiting. Our achievements open up a brand-new strategy for wider spectral luminescence of double perovskites and pace up the road for a series of new applications.

Manganese-based organic-inorganic metal halide composites have been considered as promising candidates for lead-free emitters. However, in spite of their excellent luminescence properties in green and red regions, blue emission-a critical component for white light generation-from pristine manganese-based composites is currently missing. In this work, we successfully achieve blue luminescence center in manganese-based composites through selecting specific organic component methylbenzylamine (MBA). Our approach is fundamentally different from green and red emission in manganese-based composites, which result from manganese-halide frameworks. The coexistence of different luminescence centers in our manganese-based composites is confirmed by photoluminescence (PL) and photoluminescence excitation (PLE) results. As a result of different photoluminescence excitation responses of different emission centers, the resulting emission color can be tuned with selecting different excitation wavelengths. Specifically, a white light emission can be obtained with Commission Internationale de leclairage coordinates of (0.33, 0.35) upon the 330 nm excitation. We further demonstrate the promise of our manganese-based composites in the anti-counterfeiting technology and multicolor lighting. Our results provide a novel strategy for full-spectral emission in manganese-based organic-inorganic metal halide composites and lay a solid foundation for a range of new applications. (C) 2022 Author(s).

Incorporating chiral organic compounds into metal halide frames is a common and useful method to introduce chirality in metal halide composites. The structures of resulting racemic and chiral composites are usually considered to be nearly identical owing to similar chemical bonding. In this work, by incorporating chiral MBABr (bromide methylbenzylamine) into an inorganic frame, a significant crystallization difference between the resulting racemic and chiral metal halide composites is observed, as confirmed by both structural and spectroscopic measurements. In addition, the structural transformation in the chiral composites can also be induced by moisture, ascribed to the asymmetric hydrogen bonding in chiral materials. These results provide new insights for the future synthesis of chiral materials and open up new possibilities to advance the materials functionalities.

The photovoltaic performance of perovskite solar cell is determined by multiple interrelated factors, such as perovskite compositions, electronic properties of each transport layer and fabrication parameters, which makes it rather challenging for optimization of device performances and discovery of underlying mechanisms. Here, we propose and realize a novel machine learning approach based on forward-reverse framework to establish the relationship between key parameters and photovoltaic performance in high-profile MASn(x)Pb(1-x)I(3) perovskite materials. The proposed method establishes the asymmetrically bowing relationship between band gap and Sn composition, which is precisely verified by our experiments. Based on the analysis of structural evolution and SHAP library, the rapid-change region and low-bandgap plateau region for small and large Sn composition are explained, respectively. By establishing the models for photovoltaic parameters of working photovoltaic devices, the deviation of short-circuit current and opencircuit voltage with band gap in defective-zone and low-bandgap-plateau regions from Shockley-Queisser theory is captured by our models, and the former is due to the deep-level traps formed by crystallographic distortion and the latter is due to the enhanced susceptibility by increased Sn (4+ )content. The more difficulty for hole extraction than electron is also concluded in the models and the prediction curve of power conversion efficiency is in a good agreement with Shockley-Queisser limit. With the help of search and optimization algorithms, an optimized Sn:Pb composition ratio near 0.6 is finally obtained for high-performance perovskite solar cells, then verified by our experiments. Our constructive method could also be applicable to other material optimization and efficient device development.

The field of organic solar cells has experienced paradigm-shifting changes in recent years because of the emergence of nonfullerene acceptors (NFAs). It is critically important to gain more insight into the structure-property relationship of the emerging A-DAD-A-type NFAs. In this Letter, a family of NFAs named BPF-4F, BPT-4F, and BPS-4F incorporating various chalcogen-containing heterocycles, i.e., furan, thiophene, and selenophene, respectively, was designed and synthesized. These NFAs exhibited dramatic differences in their photovoltaic performances with device efficiencies of 16.8% achieved by the thiophene-based cells, which was much higher than the furan-based ones (12.6%). In addition, the selenophene-based NFA showed a red-shifted absorption relative to the furan- and thiophene-based ones and obtained a decent efficiency of 16.3% owing to an improved J(SC). The reasons why these NFAs performed differently are systematically studied by comparing their optoelectronic properties and film morphology, which provides new understandings of the molecular design of high-performance NFAs.

The power conversion efficiencies (PCEs) of laboratory-sized organic solar cells (OSCs), usually processed from low-boiling-point and toxic solvents, have reached high values of over 18%. However, there is usually a notable drop of the PCEs when green solvents are used, limiting practical development of OSCs. Herein, we obtain certificated PCEs over 17% in OSCs processed from a green solvent paraxylene (PX) by a guest-assisted assembly strategy, where a third component (guest) is employed to manipulate the molecular interaction of the binary blend. In addition, the high-boiling-point green solvent PX also enables us to deposit a uniform large-area module (36 cm(2)) with a high efficiency of over 14%. The strong molecular interaction between the host and guest molecules also enhances the operational stability of the devices. Our guest-assisted assembly strategy provides a unique approach to develop large-area and high-efficiency OSCs processed from green solvents, paving the way for industrial development of OSCs. Organic solar cells processed from green solvents are easier to implement in manufacturing yet their efficiency is low. Chen et al. devise a guest molecule to improve the molecular packing, enabling devices with over 17% efficiency.

Sequential Cs incorporation strategy is developed to decouple crystallization of FACs perovskite with reduced electron-phonon coupling, resulting in highly stable FACs tri-iodide perovskite photovoltaics with record efficiency. Although pure formamidinium iodide perovskite (FAPbI(3)) possesses an optimal gap for photovoltaics, their poor phase stability limits the long-term operational stability of the devices. A promising approach to enhance their phase stability is to incorporate cesium into FAPbI(3). However, state-of-the-art formamidinium-cesium (FA-Cs) iodide perovskites demonstrate much worse efficiency compared with FAPbI(3), limited by the different crystallization dynamics of formamidinium and cesium, which result in poor composition homogeneity and high trap densities. We develop a novel strategy of crystallization decoupling processes of formamidinium and cesium via a sequential cesium incorporation approach. As such, we obtain highly reproducible, highly efficient and stable solar cells based on FA(1)(-)(x)Cs(x)PbI(3) (x = 0.05-0.16) films with uniform composition distribution in the nanoscale and low defect densities. We also revealed a new stabilization mechanism for Cs doping to stabilize FAPbI(3), i.e. the incorporation of Cs into FAPbI(3) significantly reduces the electron-phonon coupling strength to suppress ionic migration, thereby improving the stability of FA-Cs-based devices.

The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) forms a promising alternative to conventional inorganic conductors, where deposition of thin films via vapour phase polymerization (VPP) has gained particular interest owing to high electrical conductivity within the plane of the film. The conductivity perpendicular to the film is typically much lower, which may be related not only to preferential alignment of PEDOT crystallites but also to vertical stratification across the film. In this study, we reveal non-linear vertical microstructural variations across VPP PEDOT:Tos thin films, as well as significant differences in doping level between the top and bottom surfaces. The results are consistent with a VPP mechanism based on diffusion-limited transport of polymerization precursors. Conducting polymer films with vertical inhomogeneity may find applications in gradient-index optics, functionally graded thermoelectrics, and optoelectronic devices requiring gradient doping.

Organic solar cells based on non-fullerene acceptors have enabled high efficiencies yet their charge dynamics and its impact on the photovoltaic parameters are not fully understood. Now, Chen et al. provide a general description of non-radiative voltage losses in both fullerene and non-fullerene solar cells. Recent advances in organic solar cells based on non-fullerene acceptors (NFAs) come with reduced non-radiative voltage losses (Delta V-nr). Here we show that, in contrast to the energy-gap-law dependence observed in conventional donor:fullerene blends, the Delta V-nr values in state-of-the-art donor:NFA organic solar cells show no correlation with the energies of charge-transfer electronic states at donor:acceptor interfaces. By combining temperature-dependent electroluminescence experiments and dynamic vibronic simulations, we provide a unified description of Delta V-nr for both fullerene- and NFA-based devices. We highlight the critical role that the thermal population of local exciton states plays in low-Delta V-nr systems. An important finding is that the photoluminescence yield of the pristine materials defines the lower limit of Delta V-nr. We also demonstrate that the reduction in Delta V-nr (for example, <0.2 V) can be obtained without sacrificing charge generation efficiency. Our work suggests designing donor and acceptor materials with high luminescence efficiency and complementary optical absorption bands extending into the near-infrared region.

Lead halide perovskites have been considered promising semicon-ducting materials for next-generation optoelectronic devices due to their solution processability and excellent optoelectronic proper-ties. Device performance of perovskite light-emitting diodes (PeLEDs) and perovskite solar cells (PSCs) has been rapidly devel-oped during the past decade. Very recently, organic molecules containing phosphine oxide groups have emerged as promising ad-ditives and passivators to improve the device performance and sta-bility of both PeLEDs and PSCs. In this perspective, we summarize recent progress in the development of new phosphine-oxide-based additives for PeLEDs and PSCs. The passivation mechanism, molecule design principle, and structure-property relationship of phosphine oxide molecules for PeLEDs and PSCs are systematically discussed and analyzed. Finally, we provide an outlook on the mo-lecular design of novel phosphine oxide compounds for efficient and stable PeLEDs and PSCs in the future.

Circularly polarized light sources with free-space directional emission play a key role in chiroptics(1), spintronics(2), valleytronics(3) and asymmetric photocatalysis(4). However, conventional approaches fail to simultaneously realize pure circular polarization, high directionality and large emission angles in a compact emitter. Metal-halide perovskite semiconductors are promising light emitters(5-8), but the absence of an intrinsic spin-locking mechanism results in poor emission chirality. Further, device integration has undermined the efficiency and directionality of perovskite chiral emitters. Here we realize compact spin-valley-locked perovskite emitting metasurfaces where spin-dependent geometric phases are imparted into bound states in the continuum via Brillouin zone folding, and thus, photons with different spins are selectively addressed to opposite valleys. Employing this approach, chiral purity of 0.91 and emission angle of 41.0 degrees are simultaneously achieved, with a beam divergence angle of 1.6 degrees. With this approach, we envisage the realization of chiral light- emitting diodes, as well as the on-chip generation of entangled photon pairs.

The development of highly efficient blue perovskite light-emitting diodes (PeLEDs) remains a big challenge, requiring more fundamental investigations. In this work, significant photoluminescence enhancement in mixed halide blue perovskite films is demonstrated by using a molecule, benzylphosphonic acid, which eventually doubles the external quantum efficiency to 6.3% in sky-blue PeLEDs. The photoluminescence enhancement is achieved by forming an oxide-bonded perovskite surface at grain boundaries and suppressing electron-phonon interaction, which enhances the radiative recombination rate and reduces the nonradiative recombination rate, respectively. Moreover, severe thermal quenching is observed in the blue perovskite films, which can be explained by a two-step mechanism involving exciton dissociation and electron-phonon interaction. The results suggest that enhancing the radiative recombination rate and reducing the electron-phonon interaction-induced nonradiative recombination rate are crucial for achieving blue perovskite films with strong emission at or above room temperature.

To deal with the invalidation of commonly employed series model and parallel model in capacitance-voltage (C-V) characterization of organic thin films when current injection is significant, a three-element equivalent circuit model is proposed. On this basis, the expression of real capacitance in consideration of current injection is theoretically derived by small-signal analysis method. The validity of the proposed equivalent circuit and theoretical expression are verified by a simulating circuit consisting of a capacitor, a diode, and a resistor. Moreover, the accurate C-V characteristic of an organic thin film device is obtained via theoretical correction of the experimental measuring result, and the real capacitance is 35.7% higher than the directly measured capacitance at 5-V bias in the parallel mode. This work strongly demonstrates the necessity to consider current injection in C-V measurement and provides a strategy for accurate C-V characterization experimentally.

The development of non-fullerene acceptors (NFAs) has facilitated the realization of efficient organic solar cells (OSCs) with minimal burn-in losses and excellent long-term stability. However, the role of NFA molecular structures on device stability remains unclear, limiting commercialization of NFA-based OSCs. Herein, the photostability of 10 OSC devices, fabricated with various NFAs (O-IDTBR, EH-IDTBR, ITIC, and ITIC-M) blended with donor polymers (PTB7-Th, PffBT4T-2OD, and PBDB-T), is investigated. O-IDTBR and EH-IDTBR form highly stable devices with all three polymers, whereas ITIC and ITIC-M devices suffer from burn-in losses and long-term degradation. Conformational instability is found to be responsible for the poor photostability of ITIC and ITIC-M, resulting in poor device stability. Twisting and potential breakage of the chemical bond that links the end group to the main backbone of ITIC and ITIC-M molecules causes undesirable conformational changes. Potential strategies to overcome such detrimental photo-induced conformational changes in NFAs are proposed.

The hybrid metal halide perovskites have shown enormous promise for optoelectronic devices, including efficient photovoltaics, however their insensitivity to defects has remained puzzling. Polaron correlations have been cited as a possible means to protect charge carriers from defect scattering. In this paper, we show time-resolved THz spectroscopy measurements are capable of directly probing polaron correlations via an intra-band coherent beat arising from center-of-mass quasi-particle motion and the internal motion of charge within its self-induced potential. We describe these measurements indicating that charge carriers do indeed exist as polarons, which are coherent for several hundred femtoseconds following photon absorption.

Photovoltaic (PV) cells offer a convenient energy source to drive micropower electronic devices for indoor applications. However, it is challenging to measure the power conversion efficiency (PCE) of PV cells under indoor lighting and the PV community lacks a feasible and accurate measurement protocol. Here, we start with the fundamental parameters which determine the PCE, and carefully design a series of experiments to examine the origins which might cause measurement errors for organic PV measurements under indoor lighting. We demonstrate the critical importance of: 1, temporal stability and spatial homogeneity of the light sources, 2, calibration of the spectral irradiance and illuminations of the light sources, 3, the area of the cells (1 cm2 or large cells are preferred), 4, the aperture of the mask (an aperture slightly smaller than the cell area is preferred), and 5, stray lights from the measurement environment. Based on these careful investigations, we suggest a feasible measurement method, by which accurate measurement of the indoor PV efficiency is made possible. Our study will promote the healthy development of indoor PV technology for practical applications.

Comprehensive design ideas on the fused-ring donor-core in state-of-the-art acceptor-donor-acceptor (A-D-A) nonfullerene acceptors (NFAs) are still of great importance for regulating the electron push-pull effect for the sake of optimal light-harvesting, frontier molecular orbital levels, and finally their photovoltaic properties. Herein, thieno[3,2-b]thiophenes were fused in bay-area of naphthalene via six-member-ring connection, resulting in the formation of dihydropyrenobisthieno[3,2-b]thiophene based octacyclic ladder-type donor core, which was flanked by two 1,1-dicyanomethylene-3-indanone (IC) acceptor motifs with and without 5,6-diflourination, namely PTT-IC and PTT-2FIC, respectively, as novel efficient A-D-A fused-ring electron acceptors (FREAs). Compared with PTT-IC, fluorinated PTT-2FIC possesses narrower optical bandgap of 1.48 eV, better pi-pi stacking, and its PBDB-T:PTT-2FIC blend film exhibited better morphology, and better hole and electron mobility. As a result, nonfullerene solar cells using PBDB-T:PTT-2FIC as the active layer achieved a decent PCE of 10.40%, with an open-circuit voltage (V-OC) of 0.87 V, a fill factor (FF) of 0.65, and a much higher short-circuit current (J(SC)) of 18.26 mA/cm(2). Meanwhile, the PBDB-T:PTT-IC cells delivered a lower J(SC) of 12.58 mA/cm(2) but a higher V-OC of 0.99 V, thus resulting in a PCE of 7.39% due to its wider optical bandgap of 1.58 eV and higher LUMO energy level. These results demonstrated that NFAs based on fused-ring donor core from fusing thieno [3,2-b]thiophenes with naphthalene via six-member-ring connection are promising for organic photovoltaic applications.

Exact and perturbation methods were employed in simulations of powder ENDOR spectra to obtain the anisotropic hyperfine (hfc) and nuclear quadrupole (nqc) coupling constants of certain organic radicals of interest in fundamental research and in applications in radiation research, surface chemistry and biophysics. The principal hfc values of the ring protons and methyl substituents for several aromatic cations trapped in disordered matrices might be more accurate than those previously reported using regular EPR. Only one of the earlier assignments of the naphthalene cation spectrum was in acceptable agreement with the simulations. The proton couplings at the beta-position of alkyl radicals were deduced by simulations while the spectrum due to alpha-couplings with appreciable anisotropy was weak. Accurate simulation of the 14N (I = 1) spectra in bio-radicals was obtained by adjustment of the relative orientation of the principal hfc and nuclear quadrupole coupling (nqc) tensors as well as the principal values. Adjustment of the excitation width parameter employed in the software was also required in a few cases to improve the agreement with the experimental spectra. The hfc patterns due to matrix nuclei (1H and 7Li) around the radicals of X-irradiated samples were simulated to elucidate the nature of the trapping sites in materials used for EPR dosimetry. ENDOR simulation programs known to us are presented in an Appendix. The performance of the ENDORF2 program used in previous works was examined by comparison with exact treatment. Input and output examples, source and executable codes used in this work can be downloaded at https://github.com/EndorF2/Simulation.

Organic photovoltaics (OPVs) have achieved great progress in recent years due to delicately designed non-fullerene acceptors (NFAs). Compared with tailoring of the aromatic heterocycles on the NFA backbone, the incorporation of conjugated side-groups is a cost-effective way to improve the photoelectrical properties of NFAs. However, the modifications of side-groups also need to consider their effects on device stability since the molecular planarity changes induced by side-groups are related to the NFA aggregation and the evolution of the blend morphology under stresses. Herein, a new class of NFAs with localisomerized conjugated side-groups are developed and the impact of local isomerization on their geometries and device performance/stability are systematically investigated. The device based on one of the isomers with balanced side- and terminal-group torsion angles can deliver an impressive power conversion efficiency (PCE) of 18.5%, with a low energy loss (0.528 V) and an excellent photo- and thermal stability. A similar approach can also be applied to another polymer donor to achieve an even higher PCE of 18.8%, which is among the highest efficiencies obtained for binary OPVs. This work demonstrates the effectiveness of applying local isomerization to fine-tune the side-group steric effect and non-covalent interactions between side-group and backbone, therefore improving both photovoltaic performance and stability of fused ring NFA-based OPVs.

Organic photovoltaics (OPV) are one of the most effective ways to harvest renewable solar energy, with the power conversion efficiency (PCE) of the devices soaring above 19% when processed with halogenated solvents. The superior photocurrent of OPV over other emerging photovoltaics offers more opportunities to further improve the efficiency. Tailoring the absorption band of photoactive materials is an effective way to further enhance OPV photocurrent. However, the field has mostly been focusing on improving the near-infrared region photo-response, with the absorption shoulders in short-wavelength region (SWR) usually being neglected. Herein, by developing a series of non-fullerene acceptors (NFAs) with varied side-group conjugations, we observe an enhanced SWR absorption band with increased side-group conjugation length. The underpinning factors of how molecular structures and geometries improve SWR absorption are clearly elucidated through theoretical modelling and crystallography. Moreover, a clear relationship between the enhanced SWR absorption and reduced singlet-triplet energy gap is established, both of which are favorable for the OPV performance and can be tailored by rational structure design of NFAs. Finally, the rationally designed NFA, BO-TTBr, affords a decent PCE of 18.5% when processed with a non-halogenated green solvent.

Obtaining both high open-circuit voltage (V-oc) and short-circuit current density (J(sc)) has been a major challenge for efficient all-polymer solar cells (all-PSCs). Herein, we developed a polymer acceptor PF5-Y5 with excellent optical absorption capability (onset extending to similar to 880 nm and maximum absorption coefficient exceeding 105 cm(-1) in a film), high electron mobility (3.18 x 10(3) cm(2) V-1 s(-1)) and high LUMO level (-3.84 eV) to address such a challenge. As a result, the PBDB-T:PF5-Y5-based all-PSCs achieved a high power conversion efficiency of up to 14.45% with both a high Voc (0.946 V) and a high Jsc (20.65 mA cm(-2)), due to the high and broad absorption coverage, small energy loss (0.57 eV) and efficient charge separation and transport in the device, which are among the best values in the all-PSC field. In addition, the all-PSC shows a similar to 15% improvement in PCE compared to its counterpart small molecule acceptor (Y5)-based device. Our results suggest that PF5-Y5 is a very promising polymer acceptor candidate for applications in efficient all-PSCs.

Anon-fully conjugated polymer as a new class of acceptor materials has shown some advantages over its small molecular counterpart when used in photoactive layers for all-polymer solar cells (all-PSCs), despite a low power conversion efficiency (PCE) caused by its narrow absorption spectra. Herein, a novel non-fully conjugated polymer acceptor PFY-2TS with a low bandgap of similar to 1.40 eV was developed, via polymerizing a large pi-fused small molecule acceptor (SMA) building block (namely YBO) with a non-conjugated thioalkyl linkage. Compared with its precursor YBO, PFY-2TS retains a similar low bandgap but a higher LUMO level. Moreover, compared with the structural analog of YBO-based fully conjugated polymer acceptor PFY-DTC, PFY-2TS shows similar absorption spectrum and electron mobility, but significantly different molecular crystallinity and aggregation properties, which results in optimal blend morphology with a polymer donor PBDB-T and better device physical processes in all-PSCs. As a result, PFY-2TS-based all-PSCs achieved a PCE of 12.31% with a small energy loss of 0.56 eV enabled by the reduced non-radiative energy loss (0.24 eV), which is better than that of 11.08% for the PFY-DTC-based ones. Our work clearly demonstrated that non-fully conjugated polymers as a new class of acceptor materials are very promising for the development of high-performance all-PSCs.

Achieving both high open-circuit voltage (V-oc) and short-circuit current density (J(sc)) to boost power-conversion efficiency (PCE) is a major challenge for organic solar cells (OSCs), wherein high energy loss (E-loss) and inefficient charge transfer usually take place. Here, three new Y-series acceptors of mono-asymmetric asy-YC11 and dual-asymmetric bi-asy-YC9 and bi-asy-YC12 are developed. They share the same asymmetric D(1)AD(2) (D-1=thieno[3,2-b]thiophene and D-2=selenopheno[3,2-b]thiophene) fused-core but have different unidirectional sidechain on D-1 side, allowing fine-tuned molecular properties, such as intermolecular interaction, packing pattern, and crystallinity. Among the binary blends, the PM6 : bi-asy-YC12 one has better morphology with appropriate phase separation and higher order packing than the PM6 : asy-YC9 and PM6 : bi-asy-YC11 ones. Therefore, the PM6 : bi-asy-YC12-based OSCs offer a higher PCE of 17.16 % with both high V-oc and J(sc), due to the reduced E-loss and efficient charge transfer properties. Inspired by the high V-oc and strong NIR-absorption, bi-asy-YC12 is introduced into efficient binary PM6 : L8-BO to construct ternary OSCs. Thanks to the broadened absorption, optimized morphology, and furtherly minimized E-loss, the PM6 : L8-BO : bi-asy-YC12-based OSCs achieve a champion PCE of 19.23 %, which is one of the highest efficiencies among these annealing-free devices. Our developed unidirectional sidechain engineering for constructing bi-asymmetric Y-series acceptors provides an approach to boost PCE of OSCs.

Despite the enormous developments in perovskite light-emitting diodes (PeLEDs) recently, obtaining efficient blue PeLEDs is still considered a critical challenge due to the non-radiative recombination and unbalanced charge injection caused by the unmatched carrier mobility and the deep hole-injection barrier between the hole-transport layer (HTL) and the emissive layer (EML). Herein, we incorporate tris(4-trifluoromethylphenyl)phosphine oxide (TMFPPO), obtained through a facile oxidation synthesis process, into poly(9-vinylcarbazole) (PVK). TMFPPO incorporation modulated the energy level and hole mobility of the binary-blend HTLs to eliminate the hole-injection barrier and balance the charge injection within the EML. Consequently, the blue PeLEDs with blended HTL presented an external quantum efficiency (EQE) of 7.23% centred at 477 nm, which was much higher than the EQE of a PVK device (4.95%). Our results demonstrate that modulating the energy level and charge injection of the HTL in the device is a promising method for obtaining efficient blue PeLEDs. TMFPPO is developed and incorporated into PVK to modulate the hole mobility and energy level of the hole-transport layer, giving rise to a barrier-free blue perovskite light-emitting diode and an enhancement of the EQE from 4.95 to 7.23% at 477 nm.

Perovskite quantum-dot-based light-emitting diodes (QLEDs) are highly promising for future solid-state lightings and high-definition displays due to their excellent color purity. However, their device performance is easily affected by charge accumulation induced luminescence quenching due to imbalanced charge injection in the devices. Here we report green perovskite QLEDs with simultaneously improved efficiency and operational lifetime through balancing the charge injection with the employment of a bilayered electron transport structure. The charge-balanced QLEDs exhibit a color-saturated green emission with a full-width at half-maximum (FWHM) of 18 nm and a peak at 520 nm, a low turn-on voltage of 2.0 V and a champion external quantum efficiency (EQE) of 21.63%, representing one of the most efficient perovskite QLEDs so far. In addition, the devices with modulated charge balance demonstrate a nearly 20-fold improvement in the operational lifetime compared to the control device. Our results demonstrate the great potential of further improving the device performance of perovskite QLEDs toward practical applications in lightings and displays via rational device engineering. (C) 2020 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.

Green and scalable materials are essential to fulfill the need of electrification for transitioning into a fossil-fuels free society, and sustainability is a requirement for all new technologies. Rechargeable batteries are one of the most important elements for electrification, enabling the transition to mobile electronics, electrical vehicles and grid storage. We here report synthesis and characterization of polyelectrolyte complexes of alginate and chitosan, both biopolymers deriving from the sea, for transport of zinc ions in hydrogel electrolytes. We have used vibrational spectroscopy, thermal measurements and microscopy, as well as transport measurements with ohmic or blocking contacts. The transference number for zinc ions is close to 1, the conductivity is approximate to 10 mS/cm, with stability at Zn interfaces seen through 7000 cycles in symmetric zinc//zinc cell. A zinc ion aqueous electrolyte was prepared from blends of chitosan and alginate, by using a simple and scalable route. These green zinc ion electrolytes exhibit a stability window up to 2 V, a zinc ion transference number close to 1, and electrochemical cyclability over 7000 cycles at interfaces to zinc. This biologically derived polyelectrolyte complex offers many possibilities for optimizing transport and stability at electrode interfaces.image

Y Despite the significant progresses made in all-polymer solar cells (all-PSCs) recently, the relatively low short-circuit current density (J(sc)) and large energy loss are still quite difficult to overcome for further development. To address these challenges, we developed a new class of narrow-bandgap polymer acceptors incorporating a benzotriazole (BTz)-core fused-ring segment, named the PZT series. Compared to the commonly used benzothiadiazole (BT)-containing polymer PYT, the less electron-deficient BTz renders PZT derivatives with significantly red-shifted optical absorption and up-shifted energy levels, leading to simultaneously improved J(sc) and open-circuit voltage in the resultant all-PSCs. More importantly, a regioregular PZT (PZT-gamma) has been developed to achieve higher regiospecificity for avoiding the formation of isomers during polymerization. Benefiting from the more extended absorption, better backbone ordering, and more optimal blend morphology with donor component, PZT-gamma-based all-PSCs exhibit a record-high power conversion efficiency of 15.8% with a greatly enhanced J(sc) of 24.7 mA/cm(2) and a low energy loss of 0.51 eV.

Organic-inorganic hybrid perovskite solar cells (PSCs) are promising third-generation solar cells. They exhibit high power conversion efficiency (PCE) and, in theory, can be manufactured with less energy than several more established photovoltaic technologies, particularly solution-processed PSCs. Various materials have been widely utilized to modify the buried bottom interface to improve the performance and long-term stability of PSCs. Here, the latest progress in modifying the buried interface to enhance the performance and stability of PSCs is examined from a materials standpoint, which is classified into inorganic salts, the organic molecular and polymer, carbon materials, perovskite-related materials, and 2D materials. This material perspective is useful in determining the tactics for achieving the theoretical PCE value of PSCs. It also serves as a solid reference of interface adjustment for other layered structure heterojunction devices.

It has been a hindering issue in perovskite solar cells that the interfaces between the perovskite and charge transport layers show significantly high concentrations of defects with an amount about 100 times more than inside the bulk perovskite layer. The issue causes substantial reduction in both the efficiency and stability of the devices. Herein, a solid-solid contact approach is demonstrated to realize a multifunctional ion-lock layer with strong chemical interaction to the perovskite layer. The multifunctional ion-lock layer remarkably suppresses the interface defects and tunes the work function, contributing to promoting the carrier extraction, increasing the open-circuit voltage, and enlarging the photocurrent. In addition, the multifunctional ion-lock layer successfully locks ions from movement and thus improves the stability of the devices. Finally, with a multifunctional ion-lock layer, the perovskite solar cells deliver an efficiency of up to 23.13% along with desirable long-term operational, storage, and humidity stability. Consequently, the work offers guidelines for establishing defect-suppressed interfaces between perovskites and hole transport layers.

The use of non-fullerene acceptors (NFAs) in organic solar cells has led to power conversion efficiencies as high as 18%(1). However, organic solar cells are still less efficient than inorganic solar cells, which typically have power conversion efficiencies of more than 20%(2). A key reason for this difference is that organic solar cells have low open-circuit voltages relative to their optical bandgaps(3), owing to non-radiative recombination(4). For organic solar cells to compete with inorganic solar cells in terms of efficiency, non-radiative loss pathways must be identified and suppressed. Here we show that in most organic solar cells that use NFAs, the majority of charge recombination under open-circuit conditions proceeds via the formation of non-emissive NFA triplet excitons; in the benchmark PM6:Y6 blend(5), this fraction reaches 90%, reducing the open-circuit voltage by 60 mV. We prevent recombination via this non-radiative channel by engineering substantial hybridization between the NFA triplet excitons and the spin-triplet charge-transfer excitons. Modelling suggests that the rate of back charge transfer from spin-triplet charge-transfer excitons to molecular triplet excitons may be reduced by an order of magnitude, enabling re-dissociation of the spin-triplet charge-transfer exciton. We demonstrate NFA systems in which the formation of triplet excitons is suppressed. This work thus provides a design pathway for organic solar cells with power conversion efficiencies of 20% or more. A substantial pathway for energy loss in organic solar cells may be suppressed by engineering hybridization between non-fullerene acceptor triplet excitons and spin-triplet charge transfer excitons.

Engineering a low singlet-triplet energy gap (Delta E-ST) is necessary for efficient reverse intersystem crossing (rISC) in delayed fluorescence (DF) organic semiconductors but results in a small radiative rate that limits performance in LEDs. Here, we study a model DF material, BF2, that exhibits a strong optical absorption (absorption coefficient = 3.8 x 10(5) cm(-1)) and a relatively large Delta E-ST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (delayed lifetime = 260 mu s), but in aggregated films, BF2 generates intermolecular charge transfer (inter-CT) states on picosecond timescales. In contrast to the microsecond intramolecular rISC that is promoted by spin-orbit interactions in most isolated DF molecules, photoluminescence-detected magnetic resonance shows that these inter-CT states undergo rISC mediated by hyperfine interactions on a similar to 24 ns timescale and have an average electron-hole separation of >= 1.5 nm. Transfer back to the emissive singlet exciton then enables efficient DF and LED operation. Thus, access to these inter-CT states, which is possible even at low BF2 doping concentrations of 4 wt%, resolves the conflicting requirements of fast radiative emission and low Delta E-ST in organic DF emitters.

The remarkable success of lead halide perovskites (LHPs) in photovoltaics and other optoelectronics is significantly linked to their defect tolerance, although this correlation remains not fully clear. The tendency of LHPs to decompose into toxic lead-containing compounds in the presence of humid air calls for the need of low-toxicity LHP alternatives comprising of cations with stable oxidation states. To this aim, a plethora of low-dimensional and wide-bandgap perovskite-inspired materials (PIMs) are proposed. Unfortunately, the optoelectronic performance of PIMs currently lags behind that of their LHP-based counterparts, with a key limiting factor being the high concentration of defects in PIMs, whose rich and complex chemistry is still inadequately understood. This review discusses the defect chemistry of relevant PIMs belonging to the halide elpasolite, vacancy-ordered double perovskite, pnictogen-based metal halide, Ag-Bi-I, and metal chalcohalide families of materials. The defect-driven optical and charge-carrier transport properties of PIMs and their device performance within and beyond photovoltaics are especially discussed. Finally, a view on potential solutions for advancing the research on wide-bandgap PIMs is provided. The key insights of this review will help to tackle the commercialization challenges of these emerging semiconductors with low toxicity and intrinsic air stability.

Perovskite light emitting diodes suffer from poor operational stability, exhibiting a rapid decay of external quantum efficiency within minutes to hours after turn-on. To address this issue, we explore surface treatment of perovskite films with phenylalkylammonium iodide molecules of varying alkyl chain lengths. Combining experimental characterization and theoretical modelling, we show that these molecules stabilize the perovskite through suppression of iodide ion migration. The stabilization effect is enhanced with increasing chain length due to the stronger binding of the molecules with the perovskite surface, as well as the increased steric hindrance to reconfiguration for accommodating ion migration. The passivation also reduces the surface defects, resulting in a high radiance and delayed roll-off of external quantum efficiency. Using the optimized passivation molecule, phenylpropylammonium iodide, we achieve devices with an efficiency of 17.5%, a radiance of 1282.8 W sr(-1) m(-2) and a record T-50 half-lifetime of 130h under 100mAcm(-2). Perovskite light emitting diodes suffer from operational stability, showing rapid decay of performance within minutes to hours after turn-on. Here, the authors investigate how the steric and Coulomb interaction of ammonium passivation molecules with varying alkyl chain length can improve device stability by suppressing iodide ion migration.

Nanoparticles (NPs) elicit sterile inflammation, but the underlying signaling pathways are poorly understood. Here, we report that human monocytes are particularly vulnerable to amorphous silica NPs, as evidenced by single-cell-based analysis of peripheral blood mononuclear cells using cytometry by time-of-flight (CyToF), while silane modification of the NPs mitigated their toxicity. Using human THP-1 cells as a model, we observed cellular internalization of silica NPs by nanoscale secondary ion mass spectrometry (nanoSIMS) and this was confirmed by transmission electron microscopy. Lipid droplet accumulation was also noted in the exposed cells. Furthermore, time-of-flight secondary ion mass spectrometry (ToF-SIMS) revealed specific changes in plasma membrane lipids, including phosphatidylcholine (PC) in silica NP-exposed cells, and subsequent studies suggested that lysophosphatidylcholine (LPC) acts as a cell autonomous signal for inflammasome activation in the absence of priming with a microbial ligand. Moreover, we found that silica NPs elicited NLRP3 inflammasome activation in monocytes, whereas cell death transpired through a non-apoptotic, lipid peroxidation-dependent mechanism. Together, these data further our understanding of the mechanism of sterile inflammation.