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Se‐functionalized small molecule acceptors (SMAs) exhibit unique advantages in constructing materials with near‐infrared absorption, but their photovoltaic performance lags behind that of S‐containing analogs in organic solar cells (OSCs). Herein, two new Se‐containing SMAs, namely Se‐EH and Se‐EHp, are designed and synthesized by regulating bifurcation site of outer alkyl chain, which enables Se‐EH and Se‐EHp to form different 3D crystal frameworks from CH1007. Se‐EH displays tighter π–π stacking and denser packing framework with smaller‐sized pore structure induced by larger steric hindrance effect of outer alkyl chain branched at 2‐position, and a higher dielectric constant of PM6:Se‐EH active layer can be obtained. OSCs based on PM6:Se‐EH achieved very high PCEs of 18.58% in binary and 19.03% in ternary devices with a high FF approaching 80% for Se‐containing SMAs. A more significant alkyl chain steric hindrance effect in Se‐EH adjusts the molecular crystallization to form a favorable nanofiber interpenetrating network with an appropriate domain size to reduce rate of sub‐ns recombination and promote balanced transport of carriers. This work provides references for further design and development of highly efficient Se‐functionalized SMAs. [ABSTRACT FROM AUTHOR]

Tin‐based perovskite solar cells (TPSCs) have received increasing attention due to their low toxicity, high theoretical efficiency, and potential applications as wearable devices. However, the inherent fast and uncontrollable crystallization process of tin‐based perovskites results in high defect density in the film. Meanwhile, when fabricated into flexible devices, the prepared perovskite film exhibits inevitable brittleness and high Young's modulus, seriously weakening the mechanical stability. In this work, we design and synthesize a cross‐linkable fullerene, thioctic acid functionalized C60 fulleropyrrolidinium iodide (FTAI), which has multiple interactions with perovskite components and can finely regulate the crystallization quality of perovskite film. The obtained perovskite film shows an increased grain size and a more matched energy level with the electron transport material, effectively improving the carrier extraction efficiency. The FTAI‐based rigid device achieves a champion efficiency of 14.91 % with enhanced stability. More importantly, the FTAI located at the perovskite grain boundaries could spontaneously cross‐link during the perovskite annealing process, which effectively improves the conductivity and elasticity of grain boundaries, thereby giving the film excellent bending resistance. Finally, the FTAI‐based wearable device yields a record efficiency of 12.35 % and displays robust bending durability, retaining about 90 % of the initial efficiency after 10,000 bending times. [ABSTRACT FROM AUTHOR]

Recently, lead‐free Sn‐based perovskite light‐emitting diodes (PeLEDs) have attracted wide attention due to their near‐infrared emission and environmental friendliness. However, desired Sn2+ is easily oxidized to Sn4+ in the crystallization process, resulting in defects and intrinsically p‐doped properties in the perovskite films. The uncontrollable oxidation affects the charge injection balance and radiative recombination, leading to poor device performance. Herein, a bi‐functional conductive molecular, 2,7‐bis(diphenylphosphoryl)‐9,9′‐spirobifluorene (SPPO13) with two P═O functional groups, is used to interact with perovskite to passivate defects and suppress the oxidation of Sn2+. Moreover, the SPPO13 modification layer inserted between the perovskite emitter and the electron transport layer can regulate the carrier injection and transport, thus promoting the charge balance. As a result, the high‐performance near‐infrared CsSnI3 PeLEDs with a record external quantum efficiency (EQE) of 6.60% and ultra‐low efficiency roll‐off are achieved. The work provides a novel approach to regulate defect passivation and charge transport for efficient Sn‐based PeLEDs. [ABSTRACT FROM AUTHOR]

Metal halide perovskite light‐emitting diodes (Pero‐LEDs) have gained great attention due to their promising applications in lighting and displays. However, in their conventional three‐layered sandwich structure, some undeserved carrier behaviors, such as imbalanced carrier injection, severe carrier loss, and unstable recombination zone, limit the device's performance. Herein, a four‐layered design by inserting a nickel acetate (Ni(OAc)2) interlayer between the emitter and hole‐transport layer(HTL) to manage carrier behavior and improve radiative recombination efficiency is proposed. Specifically, the Ni(OAc)2 interlayer is poorly conductive and can partially block the hole injection, making the hole‐electron injection more balanced. And the Ni(OAc)2 interlayer avoids the direct contact between the perovskite emitter and hole transporter, reducing the interfacial carrier quenching. Moreover, the Ni(OAc)2 interlayer inhibits the electron‐migrated recombination at the hole transporter interface, confining the carrier recombination zone in the emitter layer. As a result, the corresponding Pero‐LEDs achieve a maximum external quantum efficiency (EQEmax) of 24.6% with good reproducibility, showing an average EQEmax of over 20%. [ABSTRACT FROM AUTHOR]

Perovskite films prepared by the solution process usually result in irregular grain orientation and rich buried interface defects, hindering the further improvement of device performance. Herein, multi‐fluorine‐containing C60‐ and C70 (higher fullerene)‐porphyrin derivatives, F60PD and F70PD, are synthesized and pre‐buried to modify the SnO2/perovskite heterointerface. The F70PD modification layer provides a better perovskite quality and more effective electron transporting capability compared to the corresponding F60PD, with the F70PD being more effective in regulating the perovskite growth, passivating the buried interface defects, and optimizing the interface energy level alignment. Consequently, the F70PD‐based device delivers superior efficiency and stability than the control and F60PD‐based devices. The F70PD‐based device yields a champion efficiency of 24.09% with negligible hysteresis. Meanwhile, due to the increased activation energy of ion migration, the F70PD‐based device maintains 80% of its initial efficiency after operating at the maximum power point for 1620 h. This study highlights the potential of designing higher fullerene materials for buried interface to further improve the perovskite solar cells' performance. [ABSTRACT FROM AUTHOR]

The non‐radiative recombination at the interfaces of perovskite solar cells (PSCs) is a crucial issue that limits the efficiency and stability of the devices. State‐of‐the‐art surface passivation strategies usually utilize alkyl ammonium halides to suppress the non‐radiative recombination of PSCs, but their high surface reactivity leads to the transformation into 2D perovskites under working conditions, limiting the passivation effect and the charge transport of PSCs. Herein, a non‐halide ionic salt 1‐naphthylmethylammonium formate (NMACOOH) is synthesized for surface passivation of perovskite films. In contrast to the traditional 1‐naphthylmethylammonium iodide, NMACOOH treatment hinders the formation of 2D perovskite and forms a thermally stable PbI2‐NMACOOH adduct on the perovskite surface. Surface characterization reveals that NMA+ can passivate the cation vacancies of the 3D perovskite while HCOO− passivates the metallic Pb0 and halide‐vacancy defects. Therefore, the non‐radiative recombination of PSCs is dramatically suppressed and a high open‐circuit voltage of 1.19 V is obtained. Finally, PSCs with high efficiency of 24.75% and improved long‐term stability (98% of the initial efficiency after 1800‐h storage) are obtained. Moreover, the NMACOOH‐passivated devices also show robust operational stability, retaining 83% of the initial efficiency after working for 658 h under continuous one‐sun illumination. [ABSTRACT FROM AUTHOR]

Developing X-ray charged dosimeters with excellent charge carrier storage capacity and stability is challenging. Such energy storage dosimeters have fascinating use in developing novel applications, for instance, in radiation detection, advanced multimode anti-counterfeiting, and flexible X-ray imaging of curved objects. Herein, novel LiTaO 3 :Ln3+,Eu3+ (Ln=Tb or Pr) perovskite dosimeters are developed by combining the vacuum referred binding energy (VRBE) diagram of LiTaO 3 and the optimization of dopant's concentration and compound synthesis condition. [Display omitted] • Eu3+ was evidenced as a good electron trapping centre. • Excellent LiTaO 3 :Ln3+,Eu3+ (Ln = Tb or Pr) dosimeters were rationally developed. • Charge carriers can be stored more than 1000 h. • New and advanced X-ray imaging application for curved objects was realized. • Promising and advanced anti-counterfeiting applications were demonstrated. Developing X-ray charged dosimeters with excellent charge carrier storage capacity and stability is challenging. Such energy storage dosimeters have fascinating use in developing novel applications, for instance, in radiation detection, advanced multimode anti-counterfeiting, and flexible X-ray imaging of curved objects. Herein, novel LiTaO 3 :Ln3+,Eu3+ (Ln = Tb or Pr) perovskite dosimeters are reported by combining the vacuum referred binding energy (VRBE) diagram of LiTaO 3 and the optimization of dopant's concentration and compound synthesis condition. Based on the VRBE diagram prediction, charge carrier capturing and de-trapping processes in Eu3+ and/or Ln3+ (Ln = Tb or Pr) doped LiTaO 3 will be studied to unravel the role of Eu3+ as a good electron trapping centre and to discover a record storage phosphor. The ratios of the thermoluminescence intensity of the optimized LiTaO 3 :0.005Tb3+,0.001Eu3+ to that of the state-of-the-art BaFBr(I):Eu2+, Al 2 O 3 :C, or NaLuF 4 :Tb3+ are 5.2, 8.8, or 2.8, respectively. The charge carriers can be stored more than 1000 h in LiTaO 3 :0.005Tb3+,0.001Eu3+. Proof-of-concept anti-counterfeiting application will be demonstrated by combining the colour-tailorable photoluminescence, afterglow, thermally, or optically stimulated luminescence in LiTaO 3 :0.005Tb3+,xEu3+ and LiTaO 3 :0.005Pr3+,0.001Eu3+. Multimode anti-counterfeiting application will be proposed by combining a high absolute X-ray scintillation light yield of 19000 ± 1800 ph/MeV of LiTaO 3 :0.005Tb3+,0.001Eu3+. Proof-of-concept flexible X-ray imaging application will be demonstrated by using the optimized LiTaO 3 :0.005Tb3+, 0.001Eu3+ dispersed in a silicone gel film. [ABSTRACT FROM AUTHOR]

Highlights: The modification of perovskite precursor by a series of phosphoryl chloride molecules can indeed improve the performance of perovskite LEDs (Pero-LEDs). The bis(2-oxo-3-oxazolidinyl) phosphinic chloride can not only regulate the phase distribution by controlling the crystallization rate but also passivate the defects of the quasi-2D perovskite. Highly efficient and reproducible Pero-LEDs are achieved with an maximum external quantum efficiency (EQEmax) of 20.82% and an average EQE (EQEave) of around 20% on 50 devices. Quasi-2D perovskites have attracted tremendous interest for application as light-emission layers in light-emitting diodes (LEDs). However, the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs (Pero-LEDs). Meanwhile, the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance. Here, we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs. Then, we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl) phosphinic chloride (BOPCl). It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects. As a result, the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency (EQEmax) of 20.82% and an average EQE (EQEave) of around 20% on the optimal 50 devices, proving excellent reproducibility. Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films. [ABSTRACT FROM AUTHOR]

Highlights: Three bulky cation chlorides (PMACl, PEACl and NMACl) are used to modify the perovskite surface and form pure-anion 2D (PMA)2PbCl4, mixed-anion 2D (PEA)2Pb(IxCl4-x), and non-2D NMAI passivation layers, respectively. Intermolecular interactions between the bulky cations and the strength of cation-halide hydrogen bonds are critical to forming the three distinct passivation layers. Semi-transparent wide-bandgap perovskite solar cells (WBG-PSCs) with ITO as the back electrode show hysteresis-free PCE of 18.60% and VOC deficit of 0.49 V. Wide-bandgap (WBG) perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large open-circuit voltage (VOC) deficits, limiting their photovoltaic performance. Here, we address these issues by in-situ forming a well-defined 2D perovskite (PMA)2PbCl4 (phenmethylammonium is referred to as PMA) passivation layer on top of the WBG active layer. The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent. First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase. The (PMA)2PbCl4 forms improved type-I energy level alignment with the WBG perovskite, reducing the electron recombination at the perovskite/hole-transport-layer interface. Applying this strategy in fabricating semi-transparent WBG perovskite solar cells (indium tin oxide as the back electrode), the VOC deficits can be reduced to 0.49 V, comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes. Consequently, we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high VOC of 1.23 V. [ABSTRACT FROM AUTHOR]

Interfacial defects are one of the main origins of the hysteresis effect and limit the efficiency and light stability of perovskite solar cells (PSCs). Herein, the authors propose to grant the hole‐transport materials' (HTMs) improved isotropic coordination and defect passivation through simple halogenation, enabling a robust perovskite/hole‐transport layer interface while avoiding the use of an external passivation layer. First‐principles simulations and experimental results show that the halogenated HTMs offer more isotropic coordination sites for Pb2+ ions than the halogen‐free ones, thus providing the enhanced passivating ability of defects regardless of their molecular orientation at the surface of perovskite films. Consequently, the PSCs based on the chlorinated spiro[fluorene‐9,9′‐xanthene]‐based HTM show suppressed nonradiative recombination, delivering a remarkable open‐circuit voltage (VOC) enhancement (from 1.07 to 1.14 V) and a minimal hysteresis index of as low as 0.07%. The corresponding cells also show much improved light stability, retaining 81% of the initial efficiency after 1000 h of continuous illumination at the maximum power point. This work demonstrates that a solid isotropic coordination capability of HTMs with Pb2+ is critical to forming a robust interface and improving the PSCs' light stability. [ABSTRACT FROM AUTHOR]

Pyrite (FeS 2 ) stands out from other metal sulfides due to its abundance, low toxicity and high specific energy density. However, the low utilization and short cycle life of FeS 2 caused by irreversible side reactions and dramatic structural changes during charge/discharge process seriously hinders its practical application. In this work, we designed FeS 2 nanochains to address these issues because this unique structure not only shortens the ion/electron diffusion distance, increases the electrode/electrolyte contact area, but also accommodates the strain associated with Li ion intercalation and deintercalation reactions. Compared with nanoparticles, the FeS 2 nanochains synthesized by magnetic - field - assisted aerosol pyrolysis could cycle up to 800 cycles at 0.5C, remained a discharge capacity of 342.4 mA h g −1 in the voltage range of 1.0 - 2.6 V and achieved a remarkable capacity fading rate of 0.02% per cycle, which is among the best values demonstrated so far for Li/FeS 2 cells. In - situ Raman experiments revealed that the irreversible side reactions could be suppressed through controlling the voltage window, which can be benefit for further improving the performance of Li/FeS 2 cells. [ABSTRACT FROM AUTHOR]

The under‐coordinated defects within perovskite and its relevant interfaces always attract and trap the free carriers via the electrostatic force, significantly limiting the charge extraction efficiency and the intrinsic stability of perovskite solar cells (PSCs). Herein, self‐diffusion interfacial doping by using ionic potassium L‐aspartate (PL‐A) is first reported to restrain the carrier trap induced recombination via the reconstruction of energy level structure at SnO2/perovskite interface in conventional n‐i‐p structured PSCs. Experiments and theories are consistent with the PL‐A anions that can remain at the SnO2 surface due to strong chemical adsorption. During the spin‐coating of the perovskite film, the cations gradually diffuse into perovskite and endow an n‐doping effect, which provides higher force and a better energy level alignment for the carrier transport. As a result, they obtained 23.74% power conversion efficiency for the PL‐A modified small‐area devices, with dramatically improved open‐circuit voltage of 1.19 V. The corresponding large‐area devices (1.05 cm2) achieved an efficiency of 22.23%. Furthermore, the modified devices exhibited negligible hysteresis and enhanced ambient air stability exceeding 1500 h. [ABSTRACT FROM AUTHOR]

Perovskite light‐emitting diodes (Pero‐LEDs) with external quantum efficiencies (EQEs) of over 20% have been achieved in the last several years. However, the reproducibility of such high‐efficiency Pero‐LEDs is still low. The perovskite film quality, especially for the non‐radiative defects, is crucial in determining the device performance. These defects may lie in bulk grains, grain boundaries, and interfaces of the as‐formed perovskite films. Here, a polymer infiltrative treatment method is developed to realize effective and universal defect passivation. Specifically, poly(vinylidene fluoride) (PVDF) polymer chains are blended into the perovskite films before they are fully crystallizing. This infiltrative treatment method can regulate crystallization and passivate defects through the chemical interactions of perovskite lattices and PVDF. As a result, high‐quality perovskite films with void‐free surfaces and few‐defect crystals are obtianed. The corresponding Pero‐LEDs show a maximum EQE of 22.29% and an average EQE of 20.44 ± 0.73% based on a statistical analysis of 50 devices, exhibiting excellent reproducibility. The work provides better insights into controlling crystal growth and defect passivation via polymer‐assisted methods for efficient Pero‐LEDs. [ABSTRACT FROM AUTHOR]

Perovskite light‐emitting diodes (Pero‐LEDs) have attracted significant attention due to their high color purity and solution processing, presenting potential applications for next‐generation solid‐state lighting and displays. Continued materials development has shown that passivating non‐radiative defects can improve device performance. In theory, CsPbBr3&Cs4PbBr6 should be a model emitter for Pero‐LEDs, as its lattice matching provides ideal passivation and efficient exciton confinement. However, the low charge transport of Cs4PbBr6 has so far hindered device performance. Herein, a dual‐phase regulation method to grow a CsPbBr3&Cs4PbBr6 perovskite layer that enables efficient electrical injection is developed. This leads to the realization that Pero‐LEDs with a maximum EQE of 22.3% with a luminance of 10,050 cd m−2, and the devices show a T50 of 59 h at 130 cd m−2. [ABSTRACT FROM AUTHOR]

Fullerene-based electron-transporting layers (ETLs) significantly influence the defect passivation and device performance of inverted perovskite solar cells (PSCs). However, the π-cage structures of fullerenes lead to a strong tendency to self-aggregate, which affects the long-term stability of the corresponding PSCs. Experimental results revealed that [6,6]-phenyl-C 61 -butyric acid methyl ester (PCBM)-based ETLs exhibit a certain degree of self-aggregation that affects the stability of the device, particularly under continuous irradiation stress. To modulate the aggregation behavior, we replaced a methyl hydrogen of PCBM with a phenyl group to yield [6,6]-phenyl-C 61 -butyric acid benzyl ester (PCBB). As verified through X-ray crystallography, this minor structural modification results in more non-covalent intermolecular interactions, which effectively enhanced the electron-transporting ability of the PCBB-based ETL and led to an efficiency approaching 20%. Notably, the enhanced intermolecular forces of PCBB suppressed its self-aggregation, and the corresponding device showed significantly improved stability, retaining approximately 90% of its initial efficiency after 600 h under one-sun irradiation with maximum power point tracking. These findings provide a viable approach for the design of new fullerene derivatives to tune their intermolecular interactions to suppress self-aggregation within the ETL for high-performance PSCs. [ABSTRACT FROM AUTHOR]

We systematically review the progress of CsPb(I x Br 1− x) 3 solar cells in four aspects: phase stability, crystallization control, low-temperature preparation, and defect passivation. We propose challenges and future directions for developing highly efficient and stable devices. Owing to its nice performance, low cost, and simple solution-processing, organic-inorganic hybrid perovskite solar cell (PSC) becomes a promising candidate for next-generation high-efficiency solar cells. The power conversion efficiency (PCE) has boosted from 3.8% to 25.2% over the past ten years. Despite the rapid progress in PCE, the device stability is a key issue that impedes the commercialization of PSCs. Recently, all-inorganic cesium lead halide perovskites have attracted much attention due to their better stability compared with their organic-inorganic counterpart. In this progress report, we summarize the properties of CsPb(I x Br 1− x) 3 and their applications in solar cells. The current challenges and corresponding solutions are discussed. Finally, we share our perspectives on CsPb(I x Br 1− x) 3 solar cells and outline possible directions to further improve the device performance. [ABSTRACT FROM AUTHOR]

Although it usually involves troublesome and time-consuming synthesis work, molecular structure tailoring has been the mainstream tool to adjust the optical absorption and bandgap of organic semiconductors. Herein, we provided a convenient and feasible method to prepare narrow bandgap small-molecule semiconductors by Lewis acid-base chemistry and the optical absorption was adjusted by the stoichiometry of Lewis acid-base reactions. In this work, three pyridine capped diketopyrrolopyrrole (DPP) molecules, i.e., DPPPy-Ph-F , DPPPy-Ph-3F , and DPPPy-Py-F , with medium bandgap were synthesized to coordinate with Lewis acid of B(C 6 F 5 ) 3 (BCF). By coordinating with BCF, as demonstrated by 1 H, 19 F, and 11 B NMR spectra, the bandgaps of these DPP molecules were depressed largely. For DPPPy-Ph-F , with two pyridine units flanking symmetrically, 2 eq of BCF converted the two pyridine nitrogens stoichiometrically to Lewis acid adducts, along with absorption bands red-shifted and bandgap depressed (1.89 vs . 1.80 eV). For DPPPy-Ph-3F , with two pyridine units flanked and trifluorobenzene capped, adding 2 eq of BCF was unable to convert the two pyridine nitrogens to BCF adducts completely, due to the strong electron-drawing ability of trifluorobenzene substituent on pyridine, reducing its basicity. After adding excess BCF to coordinate with nitrogens, the bandgaps of DPPPy-Ph-3F also decreased from 1.92 eV to 1.84 eV. For DPPPy-Py-F , with four pyridine units flanked, 4 eq of BCF were required to bind the pyridine nitrogens. Accordingly, the red-shift of absorption bands and the depression of optical bandgaps (1.96 vs . 1.75 eV) for DPPPy-Py-F were most striking among the three molecules. [ABSTRACT FROM AUTHOR]

[Display omitted] • VRBEs in the Bi2+ 2P 1/2 ground state in NaYGeO 4 and NaLuGeO 4 were experimentally determined by thermoluminescence study. • Electron liberation from Bi2+ has been evidenced. • Fully control of Bi3+ trapping depth via conduction band engineering. • Rational design of new Bi3+-based afterglow phosphor. It is challenging to rational design persistent luminescence and storage phosphors with high storage capacity of electrons and holes after X-ray charging. Such phosphors have potential applications in anti-counterfeiting and X-ray imaging. Here we have combined vacuum referred binding energy diagram (VRBE) construction, photoluminescence spectroscopy, and thermoluminescence to study the trapping processes of charge carriers in NaYGeO 4. In NaYGeO 4 :0.004Bi3+ and NaYGeO 4 :0.004Bi3+,0.005Ln3+ (Ln = Tb or Pr), Bi3+ appears to act as a shallow electron trap, while Bi3+ and Ln3+ act as deep hole trapping and recombination centres. We will show how to experimentally determine the VRBE in the Bi2+ 2P 1/2 ground state in NaYGeO 4 and NaLuGeO 4 by thermoluminescence study. The electron trap depth produced by Bi3+ codopant in NaLu 1-x Y x GeO 4 :0.003Bi3+,0.008 Tb3+ can be adjusted, by increasing x, resulting in conduction band engineering. By combining Bi3+ as an electron trap and Bi3+ and Tb3+ as the hole traps, excellent X-ray charged afterglow phosphors were developed. The integrated TL intensity of the optimized NaYGeO 4 :0.004Bi3+ and NaYGeO 4 :0.003Bi3+,0.008Tb3+ after exposure to X-rays is about 4.5 and 1.1 times higher than that of the state-of-the-art BaFBr(I):Eu2+ storage phosphor. Intense initial Tb3+ 4f → 4f afterglow appears in NaYGeO 4 :0.003Bi3+,0.008Tb3+ and more than 40 h afterglow is measurable in NaYGeO 4 :0.004Bi3+ and NaYGeO 4 :0.003Bi3+, 0.008 Tb3+ after X-ray charging. We will show proof-of-concept anti-counterfeiting and X-ray imaging applications by using the developed afterglow phosphors and CsPbI 3 quantum dots. This work not only provides experimental evidence on the VRBE in the Bi2+ 2P 1/2 ground state in NaYGeO 4 , but also shows how to design and develop good afterglow phosphors for anti-counterfeiting and X-ray imaging by deeply studying and controlling the trapping processes of charge carriers in bismuth and/or lanthanides doped inorganic compounds. [ABSTRACT FROM AUTHOR]

A stable cyan-emitting perovskite was fabricated through the incorporation of two branched cations into methylamine-based halide perovskite, obtaining a stable and high PLQY of ~87.8%. Such superior optical merits endow the perovskite with high and stable performance in cyan and white LEDs. [Display omitted] • DMAPbBr 3 with hollow PbBr 3 − and high solubility (at least 2.0 M) was pre-synthesized. • Branched DMA+ and TmMA+ were adopted to form 2D/3D perovskites for the first time. • Both the effective blueshift (from 541 nm to 486 nm) and enhanced PLQY (from ~9.9% to ~87.8%) were achieved. • Stable cyan LED with improved durability and white LED with increased CRI (from ~73.1 to ~81.7) were fabricated. As an indispensable part of the visible light region, cyan emission (470 nm–500 nm) is of great importance in lighting, displays, and light communication. Metal halide perovskite materials have made significant progress in the field of luminescent materials and devices. However, the corresponding cyan emission through halide mixing is non-stable due to halogen migration and phase separation. Herein, we developed a steric stabilization approach to tune and stabilize the cyan emission of methylammonium (MA)-based perovskites. Dimethylammonium (DMA+) lead bromide, with the small DMA+ branched cation, was used as intermediate to react with MABr, forming blue-to-green emissive (MA) x (DMA)PbBr 3 +x compounds simular to the low-dimensional perovskites. Furthermore, protonated (trimethylsilyl)methylamine (TmMA), the larger branched cation, was adopted as an interlayer space to further reduce the perovskite dimension, tuning the emission to the cyan region. The combination of the two branched cations enabled us to achieve a champion photoluminescence quantum yield (PLQY) of ~87.8% (peak wavelength ~486 nm). Moreover, the as-synthesized double cations modified perovskites in combination with LED InGaN chip can be used to fabricate stable cyan emission LEDs with improved durability (over 1000 min) and white LEDs with increased color rendering index (from ~73.1 to ~81.7). [ABSTRACT FROM AUTHOR]

Eco-friendly Sn-based perovskites show significant potential for high-performance second near-infrared window light-emitting diodes (900 nm - 1700 nm). Nevertheless, achieving efficient and stable Sn-based perovskite second near-infrared window light-emitting diodes remains challenging due to the propensity of Sn 2+ to oxidize, resulting in detrimental Sn 4+ -induced defects and compromised device performance. Here, we present a targeted strategy to eliminate Sn 4+ -induced defects through moisture-triggered hydrolysis of tin tetrahalide, without degrading Sn 2+ in the CsSnI 3 film. During the moisture treatment, tin tetrahalide is selectively hydrolyzed to Sn(OH) 4 , which provides sustained protection. As a result, we successfully fabricate second near-infrared window light-emitting diodes emitting at 945 nm, achieving a performance breakthrough with an external quantum efficiency of 7.6% and an operational lifetime reaching 82.6 h., Competing Interests: Competing interests The authors declare no competing interests., (© 2024. The Author(s).)

Improving the efficiency of tin-based perovskite solar cells (TPSCs) is significantly hindered by energy level mismatch and weak interactions at the interface between the tin-based perovskite and fullerene-based electron transport layers (ETLs). In this study, four well-defined multidentate fullerene molecules with 3, 4, 5, and 6 diethylmalonate groups, labeled as FM3, FM4, FM5, and FM6 are synthesized, and employed as interfacial layers in TPSCs. It is observed that increasing the number of functional groups in these fullerenes leads to shallower lowest unoccupied molecular orbital (LUMO) energy levels and enhance interfacial chemical interactions. Notably, FM5 exhibits a suitable energy level and robust interaction with the perovskite, effectively enhancing electron extraction and defect passivation. Additionally, the unique molecular structure of FM5 allows the exposed carbon cage to be tightly stacked with the upper fullerene cage after interaction with the perovskite, facilitating efficient charge transfer and protecting the perovskite from moisture and oxygen damage. As a result, the FM5-based device achieves a champion efficiency of 15.05%, significantly surpassing that of the PCBM-based (11.77%), FM3-based (13.54%), FM4-based (14.34%), and FM6-based (13.75%) devices. Moreover, the FM5-based unencapsulated device exhibits excellent stability, maintaining over 90% of its initial efficiency even after 300 h of air exposure., (© 2024 Wiley‐VCH GmbH.)

Perovskite light-emitting diodes (Pero-LEDs) have garnered significant attention due to their exceptional emission characteristics, including narrow full width at half maximum, high color purity, and tunable emission colors. Recent efficiency and operational stability advancements have positioned Pero-LEDs as a promising next-generation display technology. Extensive research and review articles on the compositional engineering and defect passivation of perovskite layers have substantially contributed to the development of multi-color and high-efficiency Pero-LEDs. However, the crucial aspect of charge transport layer (CTL) modulation in Pero-LEDs remains relatively underexplored. CTL modulation not only impacts the charge carrier transport efficiency and injection balance but also plays a critical role in passivating the perovskite surface, blocking ion migration, enhancing perovskite crystallinity, and improving light extraction efficiency. Therefore, optimizing CTLs is pivotal for further enhancing Pero-LED performance. Herein, this review discusses the roles of CTLs in Pero-LEDs and categorizes both reported and potential CTL materials. Then, various CTL optimization strategies are presented, alongside an analysis of the selection criteria for CTLs in high-performance Pero-LEDs. Finally, a summary and outlook on the potential of CTL modulation to further advance Pero-LED performances are provided., (© 2024 Wiley‐VCH GmbH.)

In 2024, tandem perovskite light-emitting diodes (tandem-PLEDs) achieved a breakthrough external quantum efficiency of 43.42%, with an organic electroluminescence (EL) unit stacked atop a perovskite EL unit, surpassing the previous single-junction perovskite LEDs. This innovative design enables a higher brightness at lower currents, enhancing the longevity and efficiency of the tandem-PLEDs. Additionally, the tandem-PLEDs can also be fabricated by combining a perovskite EL unit with a perovskite quantum dot unit. In this perspective, the key advancements in tandem-PLEDs are highlighted, focusing on the development of perovskite-organic materials, perovskite-perovskite quantum dots, and the design principles for obtaining efficient and stable charge generation layers. But more importantly, the challenges and solutions are discussed in fabricating all-perovskite tandem LEDs using strongly polar solvents that have yet to be reported nowadays. This comprehensive guide aims to support researchers in advancing the practical deployment of tandem-PLED technology., (© 2024 Wiley‐VCH GmbH.)

The imperfect charge behavior at the interfaces of perovskite/electron-transport layer (ETL)/transparent conducting oxide (TCO) limits the further performance improvement of perovskite/silicon tandem solar cells. Herein, an indium tin oxide interlayer is deposited between ETL and TCO to address this issue. Specifically, the interlayer is prepared using an all-physical and H 2 O-free method, electron-beam evaporation, which can avoid any potential damage to the underlying perovskite and ETL layers. Moreover, the interlayer's composition can be readily tuned by changing the evaporator component, enabling authors to regulate the contact resistance and energy-level alignment of the ETL/TCO interface. Consequently, the resultant perovskite/silicon tandem solar cells exhibit an impressive power conversion efficiency (PCE) of 30.8% (certified 30.3%). Moreover, the device retains 98% of its initial PCE after continuous operation under ambient conditions for 1078 h, representing one of the most stable and efficient perovskite/silicon tandem solar cells., (© 2024 Wiley‐VCH GmbH.)

Layered metal-halide perovskites, a category of self-assembled quantum wells, are of paramount importance in emerging photonic sources, such as lasers and light-emitting diodes (LEDs). Despite high trap density in two-dimensional (2D) perovskites, efficient non-radiative energy funneling from wide- to narrow-bandgap components, sustained by the Förster resonance energy transfer (FRET) mechanism, contributes to efficient luminescence by light or electrical injection. Herein, it is demonstrated that bandgap extension of layered perovskites to the blue-emitting regime will cause sluggish and inefficient FRET, stemming from the tiny spectral overlap between different phases. Motivated by the importance of blue LEDs and inefficient energy transfer in materials with phase polydispersity, wide-bandgap quasi-2D perovskites with narrow phase distribution, improved crystallinity, and the pure crystal orientation perpendicular to the charge transport layer are developed. Based on this emitter, high-performance blue perovskite LEDs with improved electroluminescence (EL) external quantum efficiency (EQE) of 7.9% at 478 nm, a narrow full width at half-maximum (FWHM) of 22 nm and a more stable EL spectra are achieved. These results provide an important insight into spectrally stable and efficient blue emitters and EL devices based on perovskites., (© 2024 Wiley‐VCH GmbH.)

Surface defect passivation and carrier injection regulation have emerged as effective strategies for enhancing the performance of perovskite light-emitting diodes (Pero-LEDs). It usually requires two functional molecules to realize defect passivation and carrier injection regulation separately. In other words, developing one single molecule possessing these capabilities remains challenging. Herein, we utilized π-conjugated fluorene derivatives as surface treatment materials, 9,9-Spirobi[fluorene] (SBF), 9,9-Spirobifluoren-2-yl-diphenylphosphine oxide (SPPO1), and 2,7-bis(diphenylphosphoryl)-9,9'-spirobifluorene (SPPO13), to investigate the influence of their chemical structure on device optoelectronic performance, especially for defect passivation and carrier injection regulation. Consequently, the passivation capability of double-bonded SPPO13 surpassed single-bonded SPPO1 and nonbonded SBF, which all showed excellent electron transport properties, enhancing electron injection. The maximum external quantum efficiencies (EQE) for Pero-LEDs treated with SBF, SPPO1, and SPPO13 were 8.13, 17.48, and 22.10%, respectively, exceeding that of the derivative-free device (6.55%). Notably, SPPO13-treated devices exhibited exceptional reproducibility, yielding an average EQE of 20.00 ± 1.10% based on 30 devices. This result emphasizes the potential of tailored fluorene derivatives for enhancing the device performance of Pero-LEDs.

Light-induced phase segregation is one of the main issues restricting the efficiency and stability of wide-bandgap perovskite solar cells (WBG PSCs). Small organic molecules with abundant functional groups can passivate various defects, and therefore suppress the ionic migration channels for phase segregation. Herein, a series of pyridine-derivative isomers containing amino and carboxyl are applied to modify the perovskite surface. The amino, carboxyl, and N-terminal of pyridine in all of these molecules can interact with undercoordinated Pb 2+ through coordination bonds and suppress halide ions migration via hydrogen bonding. Among them, the 5-amino-3-pyridine carboxyl acid (APA-3) treated devices win the champion performance, enabling an efficiency of 22.35% (certified 22.17%) using the 1.68 eV perovskite, which represents one of the highest values for WBG-PSCs. This is believed to be due to the more symmetric spatial distribution of the three functional groups of APA-3, which provides a better passivation effect independent of the molecular arrangement orientation. Therefore, the APA-3 passivated perovskite shows the slightest halide segregation, the lowest defect density, and the least nonradiative recombination. Moreover, the APA-3 passivated device retains 90% of the initial efficiency after 985 h of operation at the maximum power point, representing the robust durability of WBG-PSCs under working conditions., (© 2024 Wiley‐VCH GmbH.)

All-small-molecule organic solar cells with good batch-to-batch reproducibility combined with non-halogen solvent processing show great potential for commercialization. However, non-halogen solvent processing of all-small-molecule organic solar cells are rarely reported and its power conversion efficiencies are very difficult to improve. Herein, we designed and synthesized a small molecule donor BM-ClEH that can take advantage of strong aggregation property induced by intramolecular chlorine-sulfur non-covalent interaction to improve molecular pre-aggregation in tetrahydrofuran and corresponding micromorphology after film formation. Tetrahydrofuran-fabricated all-small-molecule organic solar cells based on BM-ClEH:BO-4Cl achieved high power conversion efficiencies of 15.0% in binary device and 16.1% in ternary device under thermal annealing treatment. In contrast, weakly aggregated BM-HEH without chlorine-sulfur non-covalent bond is almost inefficient under same processing conditions due to poor pre-aggregation induced disordered π-π stacking, indistinct phase separation and exciton dissociation. This work promotes the development of non-halogen solvent processing of all-small-molecule organic solar cells and provides further guidance., (© 2024. The Author(s).)

Designing and synthesizing fullerene bisadducts with a higher-lying conduction band minimum is promising to further improve the device performance of tin-based perovskite solar cells (TPSCs). However, the commonly obtained fullerene bisadduct products are isomeric mixtures and require complicated separation. Moreover, the isomeric mixtures are prone to resulting in energy alignment disorders, interfacial charge loss, and limited device performance improvement. Herein, we synthesized single-isomer C 60 - and C 70 -based diethylmalonate functionalized bisadducts (C 60 BB and C 70 BB) by utilizing the steric-hindrance-assisted strategy and determined all molecular structures involved by single crystal diffraction. Meanwhile, we found that the different solvents used for processing the fullerene bisadducts can effectively regulate the molecular packing in their films. The dense and amorphous fullerene bisadduct films prepared by using anisole exhibited the highest electron mobility. Finally, C 60 BB- and C 70 BB-based TPSCs showed impressive efficiencies up to 14.51 and 14.28%, respectively. These devices also exhibited excellent long-term stability. This work highlights the importance of developing strategies to synthesize single-isomer fullerene bisadducts and regulate their molecular packing to improve TPSCs' performance.

Efficient charge injection and radiative recombination are essential to achieving high-performance perovskite light-emitting diodes (Pero-LEDs). However, the perovskite emission layer (EML) and the electron transport layer (ETL) form a poor physically interfacial contact and non-negligible charge injection barrier, limiting the device performance. Herein, we utilize a phosphine oxide, 2,4,6-tris[3-(diphenylphosphinyl)phenyl]-1,3,5-triazine (PO-T2T), to treat the perovskite/ETL interface and form a chemically bonded contact. Specifically, PO-T2T firmly bonds on the perovskite's surface and grain boundaries through a dative bond, effectively passivating the uncoordinated lead defects. Additionally, PO-T2T has high electron mobility and establishes an electron transport highway to bridge the ETL and EML. As a result, a maximum external quantum efficiency (EQE max ) of 22.06% (average EQE max of 20.02 ± 1.00%) and maximum luminance ( L max ) of 103286 cd m -2 have been achieved for the champion device. Our results indicate that EML/ETL interface modifications are crucial for the fabrication of highly efficient Pero-LEDs.

Perovskite solar cells (PSCs) have demonstrated over 25% power conversion efficiency (PCE) via efficient surface passivation. Unfortunately, state-of-the-art perovskite post-treatment strategies can solely heal the top interface defects. Herein, an ion-diffusion management strategy is proposed to concurrently modulate the top interfaces, buried interfaces, and bulk interfaces (i.e., grain boundaries) of perovskite film, enabling all-interface defect passivation. Specifically, this method is enabled by applying double interactive salts of octylammonium iodide (OAI) and guanidinium chloride (GACl) onto the 3D perovskite surface. It is revealed that the hydrogen-bonding interaction between OA + and GA + decelerates the OA + diffusion and therefore forms a dimensionally broadened 2D capping layer. Additionally, the diffusion of GA + and Cl - determines the composition of the bulk and buried interface of PSCs. As a result, n-inter-i-inter-p, i.e., five-layer structured PSCs can be obtained with a champion PCE of 25.43% (certified 24.4%). This approach also enables the substantially improved operational stability of perovskite solar cells., (© 2023 Wiley-VCH GmbH.)

Constructing 2D/3D perovskite heterojunctions is effective for the surface passivation of perovskite solar cells (PSCs). However, previous reports that studying perovskite post-treatment only physically deposits 2D perovskite on the 3D perovskite, and the bulk 3D perovskite remains defective. Herein, we propose Cl 2 -dissolved chloroform as a multifunctional solvent for concurrently constructing 2D/3D perovskite heterojunction and inducing the secondary growth of the bulk grains. The mechanism of how Cl 2 affects the performance of PSCs is clarified. Specifically, the dissolved Cl 2 reacts with the 3D perovskite, leading to Cl/I ionic exchange and Ostwald ripening of the bulk grains. The generated Cl - further diffuses to passivate the bulk crystal and buried interface of PSCs. Hexylammonium bromide dissolved in the solvent reacts with the residual PbI 2 to form 2D/3D heterojunctions on the surface. As a result, we achieved high-performance PSCs with a champion efficiency of 24.21% and substantially improved thermal, ambient, and operational stability., (© 2023. The Author(s).)

Tin-based perovskite solar cells (TPSCs) are attracting intense research interest due to their excellent optoelectric properties and eco-friendly features. To further improve the device performance, developing new fullerene derivatives as electron transporter layers (ETLs) is highly demanded. Four well-defined regioisomers (trans-2, trans-3, trans-4, and e) of diethylmalonate-C 60 bisadduct (DCBA) are isolated and well characterized. The well-defined molecular structure enables us to investigate the real structure-dependent effects on photovoltaic performance. It is found that the chemical structures of the regioisomers not only affect their energy levels, but also lead to significant differences in their molecular packings and interfacial contacts. As a result, the devices with trans-2, trans-3, trans-4, and e as ETLs yield efficiencies of 11.69%, 14.58%, 12.59%, and 10.55%, respectively, which are higher than that of the as-prepared DCBA-based (10.28%) device. Notably, the trans-3-based device also demonstrates a certified efficiency of 14.30%, representing one of the best-performing TPSCs., (© 2023 Wiley-VCH GmbH.)

Metal halide perovskite films are prepared mainly by solution-based methods. However, the preparation process is prone to produce massive defects at the interface between the perovskite emitting layer and the charge transport layers, limiting the perovskite light-emitting diode device performance. Aiming at this problem, researchers have proposed many effective strategies to passivate these interface defects. However, most previous research studies only focus on modifying the perovskite top interface, and very few reports deal with the buried interface. Here, we deposited triphenylphosphine oxide (TPPO) molecules between the perovskite and the hole transport layer (HTL) and realized the buried interface modification. Adding TPPO avoids the contact recombination of the perovskite and HTL and improves the film quality by increasing the substrate wettability. Moreover, the lone pair electrons of P═O can interact with the uncoordinated lead (Pb 2+ ) of the perovskite and passivate halogen vacancy defects, and the insulation property of TPPO helps to balance the injection of holes and electrons. As a result, a maximum external quantum efficiency (EQE ma x ) of 21.01% was obtained with an average of 18.4 ± 0.9% over 30 devices, and the device reproducibility was greatly enhanced.

Understanding the function of moisture on perovskite is challenging since the random environmental moisture strongly disturbs the perovskite structure. Here, we develop various N 2 -protected characterization techniques to comprehensively study the effect of moisture on the efficient cesium, methylammonium, and formamidinium triple-cation perovskite (Cs 0.05 FA 0.75 MA 0.20 )Pb(I 0.96 Br 0.04 ) 3 . In contrast to the secondary measurements, the established air-exposure-free techniques allow us directly monitor the influence of moisture during perovskite crystallization. We find a controllable moisture treatment for the intermediate perovskite can promote the mass transportation of organic salts, and help them enter the buried bottom of the films. This process accelerates the quasi-solid-solid reaction between organic salts and PbI 2 , enables a spatially homogeneous intermediate phase, and translates to high-quality perovskites with much-suppressed defects. Consequently, we obtain a champion device efficiency of approaching 24% with negligible hysteresis. The devices exhibit an average T 80 -lifetime of 852 h (maximum 1210 h) working at the maximum power point., (© 2022. The Author(s).)

Recently, surface passivation has been proved to be an essential approach for obtaining efficient and stable perovskite light-emitting diodes (Pero-LEDs). Phosphine oxides performed well as passivators in many reports. However, the most commonly used phosphine oxides are insulators, which may inhibit carrier transport between the perovskite emitter and charge-transporter layers, limiting the corresponding device performance. Here, 2,7-bis(diphenylphosphoryl)-9,9'-spirobifluorene (SPPO13), a conductive molecule with two phosphine oxide functional groups, is introduced to modify the perovskite emitting layer. The bifunctional SPPO13 can passivate the nonradiative defects of perovskite and promote electron injection at the interface of perovskite emitter and electron-transporter layers. As a result, the corresponding Pero-LEDs obtain a maximum external quantum efficiency (EQE) of 22.3%. In addition, the Pero-LEDs achieve extremely high brightness with a maximum of around 190 000 cd/m 2 .

Metal halide perovskites have received considerable attention in the field of electroluminescence, and the external quantum efficiency of perovskite light-emitting diodes has exceeded 20%. CH 3 NH 3 PbBr 3 has been intensely investigated as an emitting layer in perovskite light-emitting diodes. However, perovskite films comprising CH 3 NH 3 PbBr 3 often exhibit low surface coverage and poor crystallinity, leading to high current leakage, severe nonradiative recombination, and limited device performance. Herein, we demonstrate a rationale for composition engineering to obtain high-quality perovskite films. We first reduce pinholes by adding excess CH 3 NH 3 Br to the actual CH 3 NH 3 PbBr 3 films, and we then add CsBr to improve the crystalline quality and to passivate nonradiative defects. As a result, the (CH 3 NH 3 ) 1-x Cs x PbBr 3 based perovskite light-emitting diodes exhibit significantly improved external quantum and power efficiencies of 6.97% and 25.18 lm/W, respectively, representing an improvement in performance dozens of times greater than that of pristine CH 3 NH 3 PbBr 3 -based perovskite light-emitting diodes. Our study demonstrates that composition engineering is an effective strategy for enhancing the device performance of perovskite light-emitting diodes., (© 2020. Higher Education Press.)

Recently, low-bandgap formamidinium lead iodide FAPbI 3 -based perovskites are of particular interest for high-performance perovskite solar cells (PSCs) due to their broad spectral response and high photocurrent output. However, to inhibit the spontaneous α-to-δ phase transition, 15-17% (molar ratio) of bromide and cesium or methylammonium incorporated into the FAPbI 3 are indispensable to achieve efficient PSCs. In return, the high bromide content will increase bandgap and narrow the spectral response region. If simply reducing the bromide content, the corresponding PSCs exhibit inferior operational stability due to α-to-δ phase transition, interface degradation, and halide migration. Herein, we report a CsPbBr 3 -cluster assisted vertically bottom-up crystallization approach to fabricate low-bromide (1% ∼ 6%), α-phase pure, and MA-free FAPbI 3 -based PSCs. The clusters, in the size of several nanometers, could act as nuclei to facilitate vertical growth of high quality α-FAPbI 3 perovskite crystals. Moreover, these clusters can show further intake by perovskite after thermal annealing, which improves the phase homogeneity of the as-prepared perovskite films. As a result, the corresponding mesoporous PSCs deliver a champion efficiency of 21.78% with photoresponse extended to 830 nm. Moreover, these devices show remarkably improved operational stability, retaining ∼82% of the initial efficiency after 1,000 h of maximum power point tracking under 1 sun condition.

Two-dimensional (2D) Ruddlesden-Popper perovskites with bulky organic cations have attracted extensive attention in light-emitting devices and photovoltaics due to their robust environment stability, tunable luminescent color, strong exciton binding and promising efficiency. A quantum well (QW) structure is spontaneously formed by sandwiching PbBr4 layers into bulky organic cations. However, some intrinsic excitonic mechanisms in these materials still need to be elucidated. In this study, the exciton-phonon interaction of quasi-2D (PEA)2(CsPbBr3)n-1PbBr4 with different PbBr4 layer numbers (n) was analyzed by temperature-varied photoluminescence (PL), scanning electron microscopy (SEM) and powder X-ray diffraction (PXRD). The mechanism of bandgap shifting with temperature was found to be dominated by the thermal expansion effect in the large-n 2D and bulk perovskite, and gradually switched to exciton-phonon interaction in the n = 1 (PEA)2PbBr4 phase, indicating enhanced exciton-phonon interaction in the thinner quantum well structure. Further analysis showed that the enhanced exciton-phonon interaction originated from the longitudinal optical phonon-exciton Fröhlich interaction rather than acoustic phonon-exciton coupling. We believe that our results will benefit the further optimization of light-emitting devices based on 2D perovskites.

Metal halide perovskite materials are an emerging class of solution-processable semiconductors with considerable potential for use in optoelectronic devices 1-3 . For example, light-emitting diodes (LEDs) based on these materials could see application in flat-panel displays and solid-state lighting, owing to their potential to be made at low cost via facile solution processing, and could provide tunable colours and narrow emission line widths at high photoluminescence quantum yields 4-8 . However, the highest reported external quantum efficiencies of green- and red-light-emitting perovskite LEDs are around 14 per cent 7,9 and 12 per cent 8 , respectively-still well behind the performance of organic LEDs 10-12 and inorganic quantum dot LEDs 13 . Here we describe visible-light-emitting perovskite LEDs that surpass the quantum efficiency milestone of 20 per cent. This achievement stems from a new strategy for managing the compositional distribution in the device-an approach that simultaneously provides high luminescence and balanced charge injection. Specifically, we mixed a presynthesized CsPbBr 3 perovskite with a MABr additive (where MA is CH 3 NH 3 ), the differing solubilities of which yield sequential crystallization into a CsPbBr 3 /MABr quasi-core/shell structure. The MABr shell passivates the nonradiative defects that would otherwise be present in CsPbBr 3 crystals, boosting the photoluminescence quantum efficiency, while the MABr capping layer enables balanced charge injection. The resulting 20.3 per cent external quantum efficiency represents a substantial step towards the practical application of perovskite LEDs in lighting and display.

In this work, we have designed a mesoporous TiO2 nanobowl (NB) array with pore size, bowl size and film thickness being easily controllable by the sol-gel process and the polystyrene (PS) template diameter. Based on the TiO2 NB array, we fabricated carbon cathode based perovskite solar cells (C-PSCs) to investigate the impact of TiO2 NB nanostructures on the performance of the as-obtained C-PSCs devices. As expected, the TiO2 NB based devices show a higher power conversion efficiency (PCE) than that of the planar counterpart, mainly due to the enhanced light absorption arising from the NB-assisted light management, the improved pore-filling of high quality perovskite crystals and the increased interface contact for rapid electron extraction and fast charge transport. Leveraging these advantages of the novel TiO2 NB film, the 220 nm-PS templated TiO2 NB based devices performed the best on both light absorption capability and charge extraction, and achieved a PCE up to 12.02% with good stability, which is 37% higher than that of the planar counterpart. These results point to a viable and convenient route toward the fabrication of TiO2 ETL nanostructures for high performance PSCs.

A planar perovskite solar cell that incorporates a nanocarbon hole-extraction layer is demonstrated for the first time by an inkjet printing technique with a precisely controlled pattern and interface. By designing the carbon plus CH3NH3I ink to transform PbI2 in situ to CH3NH3PbI3, an interpenetrating seamless interface between the CH3NH3PbI3 active layer and the carbon hole-extraction electrode was instantly constructed, with a markedly reduced charge recombination compared to that with the carbon ink alone. As a result, a considerably higher power conversion efficiency up to 11.60% was delivered by the corresponding solar cell. This method provides a major step towards the fabrication of low-cost, large-scale, metal-electrode-free but still highly efficient perovskite solar cells., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Hybrid organic/inorganic perovskite solar cells have been rapidly evolving with spectacular successes in both nanostructured and thin-film versions. Herein, we report the use of a simple sol-gel-processed NiO nanocrystal (NC) layer as the hole-transport layer in an inverted perovskite solar cell. The thin NiO NC film with a faceted and corrugated surface enabled the formation of a continuous and compact layer of well-crystallized CH3 NH3 PbI3 in a two-step solution process. The hole-extraction and -transport capabilities of this film interfaced with the CH3 NH3 PbI3 film were higher than those of organic PEDOT:PSS layers. The cell with a NiO NC film with a thickness of 30-40 nm exhibited the best performance, as a thinner layer led to a higher leakage current, whereas a thicker layer resulted in a higher series resistance. With the NiO film, we observed a cell efficiency of 9.11 %, which is by far the highest reported for planar perovskite solar cells based on an inorganic hole-extracting layer., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Hybrid organic/inorganic perovskite solar cells are attracting intense attention and further developments largely hinge on understanding the fundamental issues involved in the cell operation. In this paper, a liquid phase deposition (LPD) method is developed to design and grow a TiO(2) nanolayer at room temperature for carbon-based perovskite solar cells. The TiO(2) nanolayer grown on FTO glass is compact but polycrystalline consisting of tiny anatase TiO(2) nanocrystals intimately stacked together. By directly exploiting this TiO(2) nanolayer in a solar cell of TiO(2) nanolayer/CH(3)NH(3)PbI(3)/nanocarbon, we have achieved a Voc as high as 1.07 V, the highest value reported so far for hole transporter-free CH(3)NH(3)PbI(3) solar cells. This is rationalized by the slower electron injection and longer electron lifetime due to the TiO(2) nanolayer, which enhances the electron accumulation in CH(3)NH(3)PbI(3) and consequently the Voc. By employing a rutile TiO(2) nanorod (NR) array as a base structure for the LPD-TiO(2) nanolayer to support the CH(3)NH(3)PbI(3) layer, the photocurrent density is considerably increased without obviously compromising the Voc (1.01 V). As a result, the power conversion efficiency is boosted from 3.67% to 8.61%. More elaborate engineering of the TiO(2) nanolayer by LPD in conjunction with judicious interfacing with other components has the potential to achieve higher performances for this type of solar cell.