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Organic scintillators are praised for their abundant element reserves, facile preparation procedures, and rich structures. However, the weak X‐ray attenuation ability and low exciton utilization efficiency result in unsatisfactory scintillation performance. Herein, a new family of highly efficient organic phosphonium halide salts with thermally activated delayed fluorescence (TADF) are designed by innovatively adopting quaternary phosphonium as the electron acceptor, while dimethylamine group and halide anions (I−) serve as the electron donor. The prepared butyl(2‐[2‐(dimethylamino)phenyl]phenyl)diphenylphosphonium iodide (C4‐I) exhibits bright blue emission and an ultra‐high photoluminescence quantum yield (PLQY) of 100 %. Efficient charge transfer is realized through the unique n‐π and anion‐π stacking in solid‐state C4‐I. Photophysical studies of C4‐I suggest that the incorporation of I accounts for high intersystem crossing rate (kISC) and reverse intersystem crossing rate (kRISC), suppressing the intrinsic prompt fluorescence and enabling near‐pure TADF emission at room temperature. Benefitting from the large Stokes shift, high PLQY, efficient exciton utilization, and remarkable X‐ray attenuation ability endowed by I, C4‐I delivers an outstanding light yield of 80721 photons/MeV and a low limit of detection (LoD) of 22.79 nGy ⋅ s−1. This work would provide a rational design concept and open up an appealing road for developing efficient organic scintillators with tunable emission, strong X‐ray attenuation ability, and excellent scintillator performance. [ABSTRACT FROM AUTHOR]

Stimuli‐responsive luminescent materials have attracted much research attention due to their wide application potential in various fields. Typically, the family of hydrated double perovskite A2MIIIX5·H2O shows unique emission color transformation between hydrated and dehydrated complexes, highlighting the application potential in advanced anti‐counterfeiting. Herein, two zero‐dimensional perovskites of Cs2YbCl5·H2O and Cs3YbCl6, are reported and broad‐band self‐trapped exciton recombination emission can be realized via external Sb3+ doping. Intriguingly, the Cs2YbCl5·H2O can be transformed to the dehydrated counterpart of Cs3YbCl6 through a facile methanol treatment at room temperature, leading to the emission color transformation from yellow to green. Notably, the green‐emissive Cs3YbCl6:Sb3+ delivers a high photoluminescence quantum yield of 67.3%. Leveraging the advantages of obvious methanol‐induced emission color transformation between Cs2YbCl5·H2O and Cs3YbCl6 at room temperature, Cs2YbCl5·H2O can be used in the field of high‐security‐level anti‐counterfeiting. [ABSTRACT FROM AUTHOR]

The development of large‐area transparent organic‐inorganic hybrid metal halide (OIMH) scintillation screens is restricted by the anisotropic single‐crystal growth, numerous grain boundaries in polycrystalline wafers, and inhomogeneous dispersion in perovskite‐polymer composite films. The crystal‐glass phase transition of OIMH materials may provide a promising solution for the above significant challenges. Herein, a new class of transparent amorphous guanidinium‐based manganese bromide glasses, (DPG)2MnBr4 and (DOTG)2MnBr4 (DPG = 1,3‐diphenylguanidinium, DOTG = 1,3‐di‐o‐tolylguanidinium), are synthesized through a low‐temperature melt‐quenching process. The (DOTG)2MnBr4 shows impressive glass‐forming ability because of large viscosity (η) at the melting temperature (Tm) (η(Tm) = 3426 mPa·s) and small fragility index (m = 52.35), which can be a potential glass scintillator. The large‐area (e.g., 13 cm × 13 cm) transparent amorphous (DOTG)2MnBr4 glass scintillator shows high light transmittance of > 80%, a low detection limit of 237.3 nGy s−1 and high X‐ray imaging spatial resolution of 12 lp mm−1. Interestingly, the glass transition temperature of < 40 °C gives (DOTG)2MnBr4 glass unique thermoplastic properties, allowing it to conform to irregularly shaped objects and reduce the distortion in X‐ray imaging. [ABSTRACT FROM AUTHOR]

The current mainstream planar X‐ray imaging techniques face significant challenges for accurately capturing the internal structure of curved objects, since the variable distances between the curved objects and the flat‐panel scintillation screen cannot eliminate the distortion in X‐ray imaging. Though large‐area and transparent curved scintillation screens are much more desirable. Here, organic–inorganic hybrid Mn‐based single crystals ([CH3Ph3P]2MnX4, X = Cl, Br, I) exhibiting high photoluminescence quantum yield (PLQY) and low melting temperature have been employed to prepare transparent glass for X‐ray scintillation imaging application through a low‐temperature melting strategy. The [CH3Ph3P]2MnBr4‐glass shows high PLQY (47.8%), high‐resolution X‐ray imaging performance (12.3 lp mm−1), low limit of detection (25.33 nGy s−1), and impressive X‐ray irradiation stability (102 Gy). Furthermore, high‐contrast X‐ray imaging at a low dose (6.865 µGy per exposure, 14.5 times lower than the chest radiograph) is achieved. Based on the low glass transition temperature (Tg = 53.6 °C) and easy‐shapeable properties of [CH3Ph3P]2MnBr4‐glass scintillator, the large‐area curved scintillation screen with a series of sizes of Φ 2×4 – Φ 8×4 cm2 can be easily fabricated and show high X‐ray imaging quality. These findings provide a paradigm for future research in shapeable X‐ray scintillators, unlocking new possibilities for curved and 3D X‐ray imaging. [ABSTRACT FROM AUTHOR]

Single‐source white‐light emitters are highlighted with stable color and excellent color rendering ability, which can largely simplify the white‐light‐emitting‐diode (WLED) structure. All‐inorganic and lead‐free double perovskites have attracted extensive research interest and provide versatile doping sites to accommodate the extrinsic multi‐valent ions. Herein, the synthesis and tunable emission of Sb3+–Ln3+‐codoped Cs2NaYCl6 single crystals (SCs) is reported. Particularly, bright white‐light emission with a high photoluminescence quantum yield of 80.5% is yielded in 0.5%Sb3+–2%Tb3+–2%Sm3+‐codoped Cs2NaYCl6 SCs. Steady‐state photoluminescence (PL) and time‐resolved PL spectra are employed to reveal the energy transfer from Sb3+‐induced self‐trapped excitons to Ln3+ ions. Temperature‐dependent PL spectra further demonstrate that the fluorescence intensity ratio of band 657 to band 590 nm is highly dependent on the temperature, and the relative sensitivity reaches a maximum of up to 1.59% K−1 at 260 K. Moreover, the WLED based on 0.5%Sb3+‐2%Tb3+‐2%Sm3+‐codoped Cs2NaYCl6 SCs delivers a higher average color rendering index of 87 than 0.5%Sb3+‐0.8%Tb3+‐2.5%Ho3+‐codoped Cs2NaYCl6 (74.6). The outstanding white‐light‐emission performance together with the high temperature dependence of the fluorescence spectra confers Sb3+–Ln3+‐codoped Cs2NaYCl6 with huge application potential in solid‐state lighting and ratiometric optical thermometry. [ABSTRACT FROM AUTHOR]

Metal halide perovskite materials have emerged as a promising class of semiconductors for high‐performance optoelectronic applications, particularly for light‐emitting diodes (LEDs), due to their high quantum efficiency, facile color tunability, narrow emission line widths, as well as cost‐effectiveness. Despite the great successes on green and red perovskite LEDs (PeLEDs), the external quantum efficiency (EQE) of blue PeLEDs still lags far behind that of green and red counterparts. Here, wavelength tunable pure and deep blue PeLEDs with high EQE are presented, achieving 17.5% and 10.8% for emission wavelengths of 472 and 461 nm, respectively. The wavelength tenability and high EQE are attributed to the unique vertically graded bandgaps and grain boundary organic shells in the perovskite films. The results demonstrate a significant performance improvement in blue PeLEDs, provide a novel route to fabricate high‐performance pure and deep blue PeLEDs that can match the performance of the green and red PeLEDs for future lighting and display applications. [ABSTRACT FROM AUTHOR]

Scintillators, which can convert high‐energy ionizing radiation (e.g., X‐ or γ‐rays) into ultraviolet‐visible light, have been widely applied in medical and industrial fields. Developing new scintillation materials with high performance and low cost is very desirable in order to address the growing application demands. Among them, single‐crystal scintillators of organic‐inorganic hybrid metal halides (OIMHs) have attracted much attention because of their excellent optical transparency, suppressed light scattering, and facile solution preparation methods. Herein, three new centimeter‐sized (2‐DMAP)2MnX4 (2‐DMAP+ = 2‐dimethylaminopyridinium, X = Cl, Br, I) single crystals with high crystal quality are synthesized via the solvent evaporation method. Benefiting from the high optical transparency and remarkable luminescence property, (2‐DMAP)2MnBr4 delivers a high X‐ray light yield of 22 000 photons MeV−1, a low limit of detection of 9.50 nGy s−1, and an excellent X‐ray imaging spatial resolution of 20–25 lp mm−1. Moreover, the regulation of single‐crystal thickness from 0.31 mm to 3.03 mm can be easily achieved via a simple solution post‐treatment method, which has a significant influence on the transmittance, spatial imaging resolution, and detection limit. This work demonstrates a promising single‐crystal scintillator for the application of high‐resolution X‐ray imaging with low preparation cost and tunable thickness. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) behaviors in metal halide perovskite and perovskite derivatives are rarely reported due to the absence of suitable TADF molecules that can serve as the A‐site cations. Herein, a series of novel donor‐π‐acceptor type of molecules are developed by adopting substituted phosphine and phosphonium as the electron donor and acceptor linked by the polarized π‐spacer. The prepared ((diphenylphosphaneyl)phenyl)diphenylphosphonium‐X (BzDPP‐X, X = counterions: Cl−, Br−, I−, NO3−, CH3COO− etc.) salts show bright emission in the visible range with TADF characteristics due to the strong intramolecular charge transfer (ICT). Benefiting from the spatially separated highest occupied molecular orbital and lowest unoccupied molecular orbital, small singlet‐triplet energy splitting (ΔEST) is obtained, facilitating the reverse intersystem crossing process. It turns out that the emission of BzDPP‐X is dependent on the counter anions, and the counterions help to stabilize the ICT state. Intriguingly, the emission can be tuned by integrating metal‐halide units into the above phosphonium salt. Remarkably, the zinc‐based halide exhibits a higher photoluminescence quantum yield (36.2%) than the pure benzyl(2‐(diphenylphosphaneyl)phenyl)diphenylphosphonium bromide (26.9%). This work exemplifies an easy design concept and a facile synthetic method toward ionic luminescent materials. [ABSTRACT FROM AUTHOR]

Glass is a group of materials with appealing qualities, including simplicity in fabrication, durability, and high transparency, and they play a crucial role in the optics field. In this paper, a new organic–inorganic metal halide luminescent glass exhibiting >78 % transmittance at 506–800 nm range together with a high photoluminescence quantum yield (PLQY) of 28.5 % is reported through a low‐temperature melt‐quenching approach of pre‐synthesized (HTPP)2MnBr4 (HTPP=hexyltriphenylphosphonium) single crystal. Temperature‐dependent X‐ray diffraction, polarizing microscopy, and molecular dynamics simulations were combined to investigate the glass‐crystal interconversion process, revealing the disordered nature of the glassy state. Benefiting from the transparent nature, (HTPP)2MnBr4 glass yields an outstanding spatial resolution of 10 lp mm−1 for X‐ray imaging. The superb optical properties and facility of large‐scale fabrication distinguish the organic–inorganic metal halide glass as a highly promising class of materials for optical devices. [ABSTRACT FROM AUTHOR]

Anti‐counterfeiting has become a serious issue around the global world; fluorescence‐based tags are praised for the low‐cost and facile decryption process. However, the high‐level anti‐counterfeiting application requires incorporating multifunctional luminescent materials with response to different excitation sources. Herein, a dimeric Cu(I)‐halide‐clusters‐assembled single‐crystal (AEP)2Cu2I6·2I·2H2O (AEP = N‐aminoethylpiperazinium) concerning a high down‐conversion photoluminescence quantum yield (PLQY) value of near unity is reported (λex = 305 nm), which can also be activated by the near‐infrared light and X‐ray. The ultrafast spectroscopy and density functional theory calculations reveal that the broad‐band emission originates from the recombination of self‐trapped excitons. Remarkably, the high PLQY and excellent attenuation capability for X‐ray confers an outstanding light yield of 55 650 photons MeV−1 to (AEP)2Cu2I6·2I·2H2O, which is 5.25 times higher than the standard bismuth germaniumoxide scintillator. Such multi‐light‐stimulus response endows (AEP)2Cu2I6·2I·2H2O with great application potential in anti‐counterfeiting, solid‐state lighting devices, and digital radiography. [ABSTRACT FROM AUTHOR]

Though fluorescence‐tag‐based anti‐counterfeiting technology has distinguished itself with cost‐effective features and huge information loading capacity, the clonable decryption process of spatial‐resolved anti‐counterfeiting cannot meet the requirements for high‐security‐level anti‐counterfeiting. Herein, we demonstrate a spatial‐time‐dual‐resolved anti‐counterfeiting system based on new organic–inorganic hybrid halides BAPPZn2(ClyBr1−y)8 (BAPP=1,4‐bis(3‐ammoniopropyl)piperazinium, y=0–1) with ultra‐long room‐temperature phosphorescence (RTP). Remarkably, the afterglow lifetime can be facilely tuned by regulating the halide‐induced heavy‐atom effect and can be identified by the naked eyes or with the help of a simple machine vision system. Therefore, the short‐lived unicolor fluorescence and lasting‐time‐tunable RTP provide the prerequisites for unicolor‐time‐resolved anti‐counterfeiting, which lowers the decryption‐device requirements and further provides the design strategy of advanced portable anti‐counterfeiting technology. [ABSTRACT FROM AUTHOR]

Due to the large distance or weak electronic conjugation between adjacent Bi‐I octahedrons, the charge transport in the low‐dimensional bismuth‐based hybrid perovskites is impeded and thus hinders their future developments. In this work, A‐site cation engineering by monoamine BZA (benzylamine) and diamine 3‐AMP (3‐(aminomethyl)pyridine) has been demonstrated as an efficient strategy to regulate the corresponding activation energy of ionic migration and carrier transport capacity. Given the higher polarity of 3‐AMP than BZA, producing a more efficient dielectric screening effect, it gives rise to obtaining the small exciton binding energy (50 meV) and low defect states (3.53×109 cm−3). The reduced distance of adjacent Bi‐I octahedrons by the bilateral anchoring of the 3‐AMP2+ diamine cation enhances both electronic conjugation and charge transport performance. Therefore, the photodetector for (3‐AMP)BiI5 SC shows a 243‐fold increase in on/off ratio compared with the (BZA)3BiI6 SC. [ABSTRACT FROM AUTHOR]

Room temperature‐processed electron transport layers (RT‐ETLs) demonstrate vast potential to be used in fabricating high‐performance flexible perovskite solar cells (PSCs) in an energy‐saving manner. However, the RT‐ETL normally suffers from inferior crystallinity, mismatched energy level, and high surface trap‐state density, which would result in under‐optimized interfacial electron extraction and undesirable interfacial charge recombination at ETL/perovskite interface, thus limiting the device performance. Herein, a novel strategy is demonstrated to prepare annealing‐free RT‐ETL based on precrystalline metal ion‐modified SnO2 nanocrystals, which perfectly optimizes the interfacial energy level alignment between ETL and perovskite layer, achieving nearly zero‐barrier charge transfer at the interface. As a result, the charge extraction has been remarkably accelerated and the interfacial charge recombination has been largely suppressed, leading to a ≈26% enhancement in device efficiency. The best‐performing flexible PSCs achieve efficiencies up to 19.3%, accompanied by outstanding mechanical strength under repeated bending cycle tests, which, to the best of the knowledge, is one of the highest reported values for the flexible perovskite photovoltaics fabricated with RT‐ETLs. [ABSTRACT FROM AUTHOR]

0D‐2D p–n type CsPbBr3/BiOCl heterojunction photocatalyst is successfully fabricated via the electrostatic self‐assembly process. On the basis of the photoluminescence and photocurrent density results, the CsPbBr3/BiOCl composite exhibits a higher charge separation rate than pure BiOCl and CsPbBr3. The degradation of Rhodamine B (RhB) result shows that the CsPbBr3/BiOCl composite obtains the highest degradation rate of close to 100% within 60 min, which is significantly higher than those of pure CsPbBr3 (84.21%) and BiOCl (73.57%) because the p–n type heterojunction photocatalyst can promote the separation of photogenerated charge carriers. The free radical capture experiment demonstrates that •O2− plays a major role in the photodegradation of RhB. This study may provide insights into designing advanced photocatalysts for the clean‐ups of environmental pollutants. [ABSTRACT FROM AUTHOR]

Although multiple emissive materials are of great research interest due to their great potential in a variety of applications, it is still challenging to prepare highly luminescent color‐tunable phosphors. Herein, the authors report a series of Pb−Sn alloyed single crystals, (C10NH22)2Pb1−xSnxBr4 (x = 0 to 1), that are equipped with two independent self‐trapped excitons (STEs) emitters. Multicolor luminescent output from blue to red and white light can be obtained by tailoring the composition, excitation wavelength, temperature, or time gating. More importantly, the synergistic effect between PbBr42− and SnBr42− enables (C10NH22)2Pb1−xSnxBr4 to have an extremely high luminescent efficiency up to near unity and remarkably extends stability in ambient air, significantly outperforming the monometallic (C10NH22)2PbBr4 and (C10NH22)2SnBr4. As an encouraging result of the richly endowed emission property and robust stability, (C10NH22)2Pb1−xSnxBr4 is further employed in multifunctional applications including the luminescent radiometric thermometer, white light emitter, and high‐security anti‐counterfeit materials. [ABSTRACT FROM AUTHOR]

Utilizing halide perovskites for photocatalytic aromatic C(sp3)H bond activation remains a great challenge due to the serious recombination of photogenerated charge carriers and slow reaction dynamics of the materials themselves. Herein, a lead‐free perovskite‐based hybrid of Cs3Sb2Br9/g‐C3N4 nanosheet is constructed and applied for photocatalytic aromatic C(sp3)H bond activation, which shows enhanced photocatalytic performance. By introducing ultrathin g‐C3N4 nanosheets as the heterogeneous nucleation sites, size‐reduced and well‐dispersed Cs3Sb2Br9 nanocrystals can be obtained. The as‐formed close contact and high‐quality heterointerface between Cs3Sb2Br9 and g‐C3N4 provides pathways for fast charge transfer which is beneficial to improve the separation efficiency of photogenerated electron−hole pairs. Under visible light irradiation, the Cs3Sb2Br9/g‐C3N4 hybrid photocatalyst can effectively oxidize toluene toward benzaldehyde and benzyl alcohol with a total conversion rate of 8346.8 μmol g−1 h−1, which is 26.6‐ and 6.0‐fold that of pure g‐C3N4 and Cs3Sb2Br9, respectively. This work demonstrates the potential of all‐inorganic lead‐free halide perovskite‐based heterostructures for photocatalytic organic reactions. [ABSTRACT FROM AUTHOR]

The high‐profile candidacy of low‐dimensional metal‐halide single crystals as promising light emitters originates from the intriguing emission properties (e.g., extremely broad luminescence spectra, large Stokes shift, high color rendition), which have enabled the recent great achievements on their application in lighting, artificial illumination, and scintillators. Among the family of low‐dimensional metal‐halide single crystals, zero‐dimensional (0D) materials have been featured in the lowest dimensionality, and as a consequence, strongest quantum confinement, softest lattice, and strongest electron–phonon coupling have been further translated into near‐unity photoluminescence (PL) efficiency with broadband emission. However, as far as it is known, 0D structures are significantly underexplored. Herein, an overview is provided on recent advances of 0D metal‐halide single crystals, with a focus on comprehensive understanding and insightful perspectives behind the photophysical mechanism. Additionally, the challenges and future opportunities currently faced by 0D bulk metal halides are discussed in order to provide a roadmap for the future development of novel materials with versatile optical properties suited for practical applications. [ABSTRACT FROM AUTHOR]

All‐inorganic bismuth‐halide perovskites are promising alternatives for lead halide perovskites due to their admirable chemical stability and optoelectronic properties; however, these materials deliver inferior photoluminescence (PL) properties, severely hindering their prospects in lighting applications. Here, a novel air‐stable but non‐emissive perovskite Rb3BiCl6 is synthesized, and the material is used as a prototype to uncover origin of the poor optical performance in bismuth‐halide perovskite. It is found that the extremely strong exciton–phonon interactions with a large coupling constant up to 693 meV leads to the seriously nonradiative recombination, which, however, can be effectively suppressed to 347 meV by introducing Sb3+ ions. As a result, Sb3+‐doped Rb3BiCl6 exhibits a stable yellow emission with unprecedented PL quantum yield up to 33.6% from self‐trapped excitons. Systematic spectroscopic characterizations and theoretical calculations are carried out to unveil the intriguing photophysical mechanisms. This work reveals the effect of exciton–phonon interaction, that is often underemphasized, on a material's photophysical properties. [ABSTRACT FROM AUTHOR]

In this research highlight, recent significant advances with hot‐assisted blade‐coating or air knife‐assisted blade‐coating of different perovskite compositions with bandgaps ranging from 1.3 eV to 1.9 eV (i.e. wide‐bandgap or small‐bandgap perovskites with mixed cations and anions, 2D/3D perovskites, Pb/Sn binary perovskites, and all‐inorganic perovskites) for single‐junction or tandem PSCs are discussed, with an emphasis on elucidating the distinct ink formulation engineering strategies, crystal growth mechanisms, crystallization kinetics, and optoelectronic properties of the different perovskite compositions. [ABSTRACT FROM AUTHOR]

To make full use of solar energy and achieve effective separation of photogenerated carriers, semiconductor heterojunction engineering is becoming increasingly significant nowadays. Herein, CsxWO3/CsPbBr3 heterojunctions via cosharing the Cs atom are synthesized by a facile acid solution method, which involves the in situ growth of CsPbBr3 nanoparticles on the surface of CsxWO3 nanorods. Transmission electron microscopy (TEM) and X‐ray photoelectron spectroscopy (XPS) tests confirm that a high‐quality interface with strong interaction between CsxWO3 and CsPbBr3 is constructed successfully. Thus, a direct Z‐scheme charge transfer pathway is built in such close‐contact heterojunctions, which can not only effectively prevent the recombination of photogenerated carriers, but also preserve the carriers with higher redox abilities, as confirmed by electron spin resonance (ESR) as well as Kelvin probe force microscopy (KPFM). As a proof of concept, the photocatalytic hydrogen production performance of CsxWO3/CsPbBr3 is evaluated in ethyl acetate, and a 17‐fold enhancement in hydrogen production rate as compared with pristine CsxWO3 is obtained, verifying the effective charge separation in such heterojunctions. Herein, a new idea for in situ synthesis of high‐quality perovskite‐based heterojunctions is provided, which will broaden their optoelectrical applications. [ABSTRACT FROM AUTHOR]

Heterojunction engineering, especially 2D/2D heterojunctions, is regarded as a quite promising strategy to manipulate the photocatalytic performance of semiconductor catalysts. In this manuscript, a direct Z‐scheme 2D/2D heterojunction of CsPbBr3/Bi2WO6 is designed and fabricated by a simple electrostatic self‐assembly process. By using ultrathin nanosheets with several atomic layers as the building blocks, a close CsPbBr3/Bi2WO6 heterointerface over large area with quite a short charge transport distance is obtained, which enables a valid Z‐scheme interfacial charge transfer between Bi2WO6 and CsPbBr3 and thus boosts charge separation. The CsPbBr3/Bi2WO6 heterojunction exhibits a superior photocatalytic performance toward CO2 reduction. By incorporating Pt nanoparticles as the cocatalyst, a high photoelectron consumption rate of 324.0 µmol g−1 h−1 under AM 1.5G irradiation (150 mW cm−2) is obtained, which is 12.2 fold higher than that of CsPbBr3 nanosheets. Moreover, a stable product yield of up to 1582.0 µmol g−1 and electron consumption yield of 8603.0 µmol g−1 for photocatalytic CO2 reduction to CO (11.4%) and CH4 (84.3%) can be achieved after 30 h of continuous catalytic reaction. The accelerated photogenerated charge transfer and spatial charge separation are investigated in detail by ultrafast spectra, photoelectrochemical test, and Kelvin probe force microscopy. [ABSTRACT FROM AUTHOR]

Halide perovskite like methylammonium lead iodide perovskite (MAPbI3) with its prominent optoelectronic properties has triggered substantial concerns in photocatalytic H2 evolution. In this work, to attain preferable photocatalytic performance, a MAPbI3/cobalt phosphide (CoP) hybrid heterojunction is constructed by a facile in situ photosynthesis approach. Systematic investigations reveal that the CoP nanoparticle can work as co‐catalyst to not only extract photogenerated electrons effectively from MAPbI3 to improve the photoinduced charge separation, but also facilitate the interfacial catalytic reaction. As a result, the as‐achieved MAPbI3/CoP hybrid displays a superior H2 evolution rate of 785.9 µmol h−1 g−1 in hydroiodic acid solution within 3 h, which is ≈8.0 times higher than that of pristine MAPbI3. Furthermore, the H2 evolution rate of MAPbI3/CoP hybrid can reach 2087.5 µmol h−1 g−1 when the photocatalytic reaction time reaches 27 h. This study employs a facile in situ photosynthesis strategy to deposit the metal phosphide co‐catalyst on halide perovskite nanocrystals to conduct photocatalytic H2 evolution reaction, which may stimulate the intensive investigation of perovskite/co‐catalyst hybrid systems for future photocatalytic applications. [ABSTRACT FROM AUTHOR]

Multiple‐cation lead mixed‐halide perovskites (MLMPs) have been recognized as ideal candidates in perovskite solar cells in terms of high efficiency and stability due to decreased open‐circuit voltage loss and suppressed yellow phase formation. However, they still suffer from an unsatisfactory long‐term moisture stability. In this study, phosphorus‐containing Lewis acid and base molecules are employed to improve device efficiency and stability based on their multifunction including recombination reduction, phase segregation suppression, and moisture resistance. The strong fluorine‐containing Lewis acid treatment can achieve a champion PCE of 22.02%. Unencapsulated and encapsulated devices retain 63% and 80% of the initial efficiency after 14 days of aging under 75% and 85% relative humidity, respectively. The better passivation of Lewis acid implies more halide defects than Pb defects at the MLMP surface. This unbalanced defect type results from phase segregation that is the synergistic effect of Cs and halide ion migrations. Identifying defect type based on different passivation effects is beneficial to not only choose suitable passivators to boost the efficiency and slow down the moisture degradation of MLMP solar cells, but also to understand the mechanism of defect‐assisted moisture degradation. [ABSTRACT FROM AUTHOR]

Hybrid organic–inorganic lead halide perovskite single crystal thin film (SCTF) recently has attracted enormous interest in the field of optoelectronic devices, since it efficiently resolves the trade‐off between thickness and carrier diffusion length. However, the toxicity of lead element and the instability induced by organic component still hinder its future developments. In this work, lead‐free all‐inorganic Cs3Bi2I9 SCTF with a high orientation along (00h) has been in situ grown on indium tin oxide (ITO) glass via a space‐limited solvent evaporation crystallization method. The trap density of Cs3Bi2I9 SCTF (5.7 × 1012 cm−3) is 263 folds lower than that of the polycrystalline thin film (PCTF) counterpart, together with a 5‐order‐of‐magnitude higher carrier mobility. These superior charge transfer properties enable a photoresponse on–off ratio as high as 11 000, which far surpasses that of the PCTF device by 460 folds, comparable to the lead halide perovskite. Furthermore, the Cs3Bi2I9 SCTF photodetector exhibits outstanding stability even without any encapsulation, whose initial performance is well maintained after aging 1000 h in humid air of 50% RH or continuous on–off light illumination for 20 h. This work will pave the way to produce new families of high‐performance, stable, and nontoxic perovskite SCTF for future optoelectronic applications. [ABSTRACT FROM AUTHOR]

Halide perovskite materials have achieved overwhelming success in various optoelectronic applications, especially perovskite solar cells and perovskite‐based light‐emitting diodes (P‐LEDs), owing to their outstanding optical and electric properties. It is widely believed that flat and mirror‐like perovskite films are imperative for achieving high device performance, while the potential of other perovskite morphologies, such as the emerging textured perovskite, is overlooked, which leaves plenty of room for further breakthroughs. Compared to flat and mirror‐like perovskites, textured perovskites with unique structures, e.g., coral‐like, maze‐like, column‐like or quasi‐core@shell assemblies, are more efficient at light harvesting and charge extraction, thus revolutionizing the pathways toward ultrahigh performance in perovskite‐based optoelectronic devices. Employing a textured perovskite morphology, the record of external quantum efficiency for P‐LEDs is demonstrated as 21.6%. In this research news, recent progress in the utilization of textured perovskite is summarized, with the emphasis on the preparation strategies and prominent optoelectronic properties. The impact of the textured morphology on light harvesting, carrier dynamic management, and device performance is highlighted. Finally, the challenges and great potential of employing these innovative morphologies in fabricating more efficient optoelectronic devices, or creating a new energy harvesting and conversion regime are also provided. [ABSTRACT FROM AUTHOR]

Low‐dimensional lead halide perovskite materials recently have drawn much attention owing to the intriguing broadband emissions; however, the toxicity of lead will hinder their future development. Now, a lead‐free (C4H14N2)2In2Br10 single crystal with a unique zero‐dimensional (0D) structure constituted by [InBr6]3− octahedral and [InBr4]− tetrahedral units is described. The single crystal exhibits broadband photoluminescence (PL) that spans almost the whole visible spectrum with a lifetime of 3.2 μs. Computational and experimental studies unveil that an excited‐state structural distortion in [InBr6]3− octahedral units enables the formation of intrinsic self‐trapped excitons (STEs) and thus contributing the broad emission. Furthermore, femtosecond transient absorption (fs‐TA) measurement reveals that the ultrafast STEs formation together with an efficient intersystem crossing has made a significant contribution to the long‐lived and broad STE‐based emission behavior. [ABSTRACT FROM AUTHOR]

Low‐dimensional luminescent lead halide perovskites have attracted tremendous attention for their fascinating optoelectronic properties, while the toxicity of lead is still considered a drawback. Herein, we report a novel lead‐free zero‐dimensional (0D) indium‐based perovskite (Cs2InBr5⋅H2O) single crystal that is red‐luminescent with a high photoluminescence quantum yield (PLQY) of 33 %. Experimental and computational studies reveal that the strong PL emission might originate from self‐trapping excitons (STEs) that result from an excited‐state structural deformation. More importantly, the in situ transformation between hydrated Cs2InBr5⋅H2O and the dehydrated form is accompanied with a switchable dual emission, which enables it to act as a PL water‐sensor in humidity detection or the detection of traces of water in organic solvents. Unleaded and unleashed: A highly emissive lead‐free indium‐based perovskite single crystal, Cs2InBr5⋅H2O, was successfully prepared. The versatile material is the first reversible metal halide perovskite photoluminescence water sensor and paves the way for the application of metal halide perovskites in water detection. [ABSTRACT FROM AUTHOR]

Engineering non-noble metal-based electrocatalysts with superior water oxidation performance is highly desirable for the production of renewable chemical fuels. Here, an atomically thin low-crystallinity Fe-Mn-O hybrid nanosheet grown on carbon cloth (Fe-Mn-O NS/CC) is successfully synthetized as an efficient oxygen evolution reaction (OER) catalyst. The synthesis strategy involves a facile reflux reaction and subsequent low-temperature calcination process, and the morphology and composition of hybrid nanosheets can be tailored conveniently. The defect-rich Fe-Mn-O ultrathin nanosheet with uniform element distribution enables exposure of more catalytic active sites; moreover, the atomic-scale synergistic action of Mn and Fe oxide contributes to an enhanced intrinsic catalytic activity. Therefore, the optimized Fe-Mn-O hybrid nanosheets, with lateral sizes of about 100-600 nm and ≈1.4 nm in thickness, enable a low onset potential of 1.46 V, low overpotential of 273 mV for current density of 10 mA cm-2, a small Tafel slope of 63.9 mV dec-1, and superior durability, which are superior to that of individual MnO2 and FeOOH electrode, and even outperforming most reported MnO2-based electrocatalysts. [ABSTRACT FROM AUTHOR]

Cupric oxide (CuO), a narrow-bandgap semiconductor, has a band alignment that makes it an ideal photocathode for the renewable production of solar fuels. However, the photoelectrochemical performance of CuO is limited by its poor conductivity and short electron diffusion lengths. Herein, a three-dimensional (3D) architecture consisting of CuO nanosheets supported onto transparent conducting macroporous antimonydoped tin oxide (mpATO@CuONSs) is designed as an excellent photocathode for promoting the hydrogen evolution reaction (HER). Owing to the 3D structure affording superior light-harvesting characteristics, large contact areas with the electrolyte, and highly conductive pathways for separation and transport of charge carriers, the mpATO@CuONSs photocathode produces an impressively high photocurrent density of -4.6 mAcm-2 at 0 V versus the reversible hydrogen electrode (RHE), which is much higher than that of the CuONSs array onto planar FTO glass (-1.9 mAcm-2). [ABSTRACT FROM AUTHOR]

Gentianales consist of Apocynaceae, Gelsemiaceae, Gentianaceae, Loganiaceae, and Rubiaceae, of which the majority are woody plants in tropical and subtropical areas. Despite extensive efforts in reconstructing the phylogeny of Gentianales based on molecular data, some interfamily and intrafamily relationships remain uncertain. We reconstructed the genus-level phylogeny of Gentianales based on the supermatrix of eight plastid markers ( rbcL, matK, atpB, ndhF, rpl16, rps16, the trnL-trnF region, and atpB-rbcL spacer) and one mitochondrial gene ( matR) using maximum likelihood. The major clades and their relationships retrieved in the present study concur with those of previous studies. All of the five families of Gentianales are monophyletic with strong support. We resolved Rubiaceae as sister to the remaining families in Gentianales and showed support for the sister relationship between Loganiaceae and Apocynaceae. Our results provide new insights into relationships among intrafamilial clades. For example, within Rubiaceae we found that Craterispermeae were sister to Morindeae + (Palicoureeae + Psychotrieae) and that Theligoneae were sister to Putorieae. Within Gentianaceae, our phylogeny revealed that Gentianeae were sister to Helieae and Potalieae, and subtribe Lisianthiinae were sister to Potaliinae and Faroinae. Within Loganiaceae, we found Neuburgia as sister to Spigelieae. Within Apocynaceae, our results supported Amsonieae as sister to Melodineae, and Hunterieae as sister to a clade comprising Plumerieae + (Carisseae + APSA). We also confirmed the monophyly of Perplocoideae and the relationships among Baisseeae + (Secamonoideae + Asclepiadoideae). [ABSTRACT FROM AUTHOR]

Photocleavage of H2O into clean and storable H2 fuel by photoelectrochemical (PEC) cell is a vital part of the sustainable hydrogen economy. However, thus far one of the limitations confronted by PEC cell to preferable performance is the insufficient behavior of photoanode for water oxidation half-reaction. One of the strategies to elevate the photoanode performance is integrating with an oxygen evolution catalyst (OEC) to remove the bottleneck of the water oxidation kinetics. Herein, an ultrafine cobalt iron oxide (CIO) nanocrystalline is reported as a novel OEC for photoelectrochemical water splitting. The CIO evenly distributing on the surface of hematite nanorod arrays not only greatly facilitates the surface hole injection, but also promotes the charge separation along with passivating the surface states. Such combined effects of CIO finally lead to an impressive 1.71 fold enhancement on the photocurrent density at 1.23 VRHE and ≈170 mV negative shift of onset potential, even overwhelms the commonly utilized Co-Pi. Along with its excellent long-term stability, the CIO possesses a great potential application in PEC water splitting devices. [ABSTRACT FROM AUTHOR]

Two new electron-rich molecules based on 3,4-phenylenedioxythiophene (PheDOT) were synthesized and successfully adopted as hole-transporting materials (HTMs) in perovskite solar cells (PSCs). X-ray diffraction, absorption spectra, photoluminescence spectra, electrochemical properties, thermal stabilities, hole mobilities, conductivities, and photovoltaic parameters of PSCs based on these two HTMs were compared with each other. By introducing methoxy substituents into the main skeleton, the energy levels of PheDOT-core HTM were tuned to match with the perovskite, and its hole mobility was also improved (1.33×10−4 cm2 V−1 s−1, being higher than that of spiro-OMeTAD, 2.34×10−5 cm2 V−1 s−1). The PSC based on MeO-PheDOT as HTM exhibits a short-circuit current density ( Jsc) of 18.31 mA cm−2, an open-circuit potential ( Voc) of 0.914 V, and a fill factor ( FF) of 0.636, yielding an encouraging power conversion efficiency (PCE) of 10.64 % under AM 1.5G illumination. These results give some insight into how the molecular structures of HTMs affect their performances and pave the way for developing high-efficiency and low-cost HTMs for PSCs. [ABSTRACT FROM AUTHOR]

Great attention to cost-effective high-efficiency solar power conversion of trihalide perovskite solar cells (PSCs) has been hovering at high levels in the recent 5 years. Among PSC devices, admittedly, TiO2 is the most widely used electron transport layer (ETL); however, its low mobility which is even less than that of CH3NH3PbI3 makes it not an ideal material. In principle, SnO2 with higher electron mobility can be regarded as a positive alternative. Herein, a SnO2 nanocolloid sol with ≈3 nm in size synthesized at 60 °C was spin-coated onto the fuorine-doped tin oxide (FTO) glass as the ETL of planar CH3NH3PbI3 perovskite solar cells. TiCl4 treatment of SnO2-coated FTO is found to improve crystallization and increase the surface coverage of perovskites, which plays a pivotal role in improving the power conversion efficiency (PCE). In this report, a champion efficiency of 14.69% (Jsc = 21.19 mA cm−2, Voc = 1023 mV, and FF = 0.678) is obtained with a metal mask at one sun illumination (AM 1.5G, 100 mW cm−2). Compared to the typical TiO2, the SnO2 ETL efficiently facilitates the separation and transportation of photogenerated electrons/holes from the perovskite absorber, which results in a significant enhancement of photocurrent and PCE. [ABSTRACT FROM AUTHOR]

Utilizing photoelectrochemical (PEC) cells to directly collecting solar energy into chemical fuels (e.g., H2 via water splitting) is a promising way to tackle the energy challenge. α‐Fe2O3 has emerged as a desirable photoanode material in a PEC cell due to its wide spectrum absorption range, chemical stability, and earth abundant component. However, the short excited state lifetime, poor minority charge carrier mobility, and long light penetration depth hamper its application. Recently, the elegantly designed hierarchical macroporous composite nanomaterial has emerged as a strong candidate for photoelectrical applications. Here, a novel 3D antimony‐doped SnO2 (ATO) macroporous structure is demonstrated as a transparent conducting scaffold to load 1D hematite nanorod to form a composite material for efficient PEC water splitting. An enormous enhancement in PEC performance is found in the 3D electrode compared to the controlled planar one, due to the outstanding light harvesting and charge transport. A facile and simple TiCl4 treatment further introduces the Ti doping into the hematite while simultaneously forming a passivation layer to eliminate adverse reactions. The results indicate that the structural design and nanoengineering are an effective strategy to boost the PEC performance in order to bring more potential devices into practical use. [ABSTRACT FROM AUTHOR]

Three cone-calix[4]arene-based sensitizers ( Calix-1- Calix-3) with multiple donor-π-acceptor ( D-π-A) moieties are designed, synthesized, and applied in dye-sensitized solar cells (DSSCs). Their photophysical and electrochemical properties are characterized by measuring UV/Vis absorption and emission spectra, cyclic voltammetry, and density functional theory (DFT) calculations. Calix-3 has excellent thermo- and photostability, as illustrated by thermogravimetric analysis (TGA) and dye-aging tests, respectively. Importantly, a DSSC using the Calix-3 dye displays a conversion efficiency of 5.48 % in under standard AM 1.5 Global solar illumination conditions, much better than corresponding DSSCs that use the rod-shaped dye M-3 with a single D-π-A chain (3.56 %). The dyes offer advantages in terms of higher molar extinction coefficients, longer electron lifetimes, better stability, and stronger binding ability to TiO2 film. This is the first example of calixarene-based sensitizers for efficient dye-sensitized solar cells. [ABSTRACT FROM AUTHOR]

Light-harvesting and charge collection have attracted increasing attention in the domain of photovoltaic cells, and can be facilitated dramatically by appropriate design of a photonic nanostructure. However, the applicability of current light-harvesting photoanode materials with single component and/or morphology (such as, particles, spheres, wires, sheets) is still limited by drawbacks such as insufficient electron-hole separation and/or light-trapping. Herein, we introduce a universal method to prepare hierarchical assembly of macroporous material-nanowire coated homogenous or heterogeneous metal oxide composite electrodes (TiO2-TiO2, SnO2-TiO2, and Zn2SnO4-TiO2; homogenous refers to a material in which the nanowire and the macroporous material have the same composition, i.e. both are TiO2. Heterogeneous refers to a material in which the nanowires and the macroporous material have different compositions). The dye-sensitized solar cell based on a TiO2-macroporous material-TiO2-nanowire homogenous composition electrode shows an impressive conversion efficiency of 9.51 %, which is much higher than that of pure macroporous material-based photoelectrodes to date. [ABSTRACT FROM AUTHOR]

Low-cost transparent counter electrodes (CEs) for efficient dye-sensitized solar cells (DSSCs) are prepared by using nanohybrids of carbon nanotube (CNT)-supported platinum nanoparticles as highly active catalysts. The nanohybrids, synthesized by an ionic-liquid-assisted sonochemical method, are directly deposited on either rigid glass or flexible plastic substrates by a facile electrospray method for operation as CEs. Their electrochemical performances are examined by cyclic voltammetry, current density-voltage characteristics, and electrochemical impedance spectroscopy (EIS) measurements. The CNT/Pt hybrid films exhibit high electrocatalytic activity for I−/I3− with a weak dependence on film thickness. A transparent CNT/Pt hybrid CE film about 100 nm thick with a transparency of about 70 % (at 550 nm) can result in a high power conversion efficiency ( η) of over 8.5 %, which is comparable to that of pyrolysis platinum-based DSSCs, but lower cost. Furthermore, DSSC based on flexible CNT/Pt hybrid CE using indium-doped tin oxide-coated polyethylene terephthalate as the substrate also exhibits η=8.43 % with Jsc=16.85 mA cm−2, Voc=780 mV, and FF=0.64, and this shows great potential in developing highly efficient flexible DSSCs. [ABSTRACT FROM AUTHOR]

Heterojunction engineering has been deemed one of the most promising strategies for promoting charge separation and improving solar‐to‐chemicals efficiency. Howbeit, constructing well‐defined nanoheterojunction with superior photocatalytic activity for H2O2 generation and a clear reaction mechanism remains a formidable challenge. Herein, an in situ vulcanization way to synthesize an intriguing 2D/1D Bi3TiNbO9/Bi2S3 heterojunction by growing Bi2S3 nanorods on Bi3TiNbO9 microsheet is used for the first time, where an S‐scheme charge transfer mechanism is formed that facilitates the spatial separation of charge carriers. Moreover, the in situ grown Bi2S3 on Bi3TiNbO9 can optimize the interfacial electronic structure and the reaction energy barriers. As a result, the H2O2 yield rate for Bi3TiNbO9/Bi2S3 can reach 810(2) µmol g−1 h−1 without any sacrificial agents and cocatalysts, ≈6.18 and ≈18.0 times of pristine Bi3TiNbO9 and Bi2S3, respectively. Importantly, the heterojunction unveiled unprecedented stability, remaining ≈95.46(2)% of the initial one after 13 continuous cycles. This work highlights an innovative in situ vulcanization strategy to engineer oxide perovskite/metal sulfide nanocomposite catalysts for artificial photosynthesis of H2O2, opening new opportunities for achieving highly efficient photocatalyst systems. [ABSTRACT FROM AUTHOR]