Search

The energy transfer processes between polyfluorene and tetraphenyl porphyrin have been investigated through steady state and time resolved measurements. Radiative transfer is found to be negligible and so the results are analyzed in terms of Förster resonance energy transfer. Rate equations are fitted to the experimental data to obtain values for the concentration dependent energy transfer rate. From this, we calculate a value of 38 Å for the energy transfer distance. This compares well with the value for the F&oumlrster radius we calculate from the spectral overlap, even though Förster theory is not strictly valid for this system. [ABSTRACT FROM AUTHOR]

Metal chalcogenide nanocrystals with variable composition and shape can conveniently be produced using cation exchange synthesis; however, the presence of cation‐containing ligands inherited from the starting material often results in contamination of the final product. To address this issue, a two‐step ligand replacement strategy is developed to fabricate CuInSe2/CuInS2 nanorods from CdSe/CdS nanorods via removal of Cd‐phosphonates from an intermediate Cu2‐xSe/Cu2‐xS phase used in the cation exchange conversion. This synthetic approach furnishes CuInSe2/CuInS2 nanorods with cadmium content below 1 at.%, and high photoluminescence quantum yields reaching 40% in the near‐infrared spectral range. Transient absorption studies reveal that the band alignment in the CuInSe2/CuInS2 heterostructure features a quasi‐type II character, with an electron localized in the core and a hole wavefunction spread over the entire nanorod. The efficient passivation of the core and the reduced Cd content leads to excitonic emission with full width at half maximum down to 110 meV, superimposed with a broad emission band from copper‐induced defects. Field‐effect transistors based on cadmium‐free CuInSe2/CuInS2 nanorods show two orders of magnitude lower noise current density compared with the cadmium‐rich devices. The responsivity and specific detectivity of these devices reach 230 mA W−1 and 108 Jones, respectively, under near‐infrared excitation at room temperature. [ABSTRACT FROM AUTHOR]

Bound states in the continuum (BICs) are widely exploited in all‐dielectric metasurfaces to significantly enhance the Q‐factor and second harmonic generation (SHG). However, a higher SHG conversion efficiency is overshadowed by the narrow transparency window of all‐dielectric materials and strict requirement of polarization‐matching. Herein, an augmented SHG assisted is demonstrated by symmetry‐protected quasi‐BICs from z‐cut wurtzite GaN metasurfaces, whose wide transparent range suppresses self‐absorption of second harmonic. Strong resonances emerge under both X‐ and Y‐polarized excitations, where the multipole characters of each eigenmode are quantitatively identified via decomposition simulations. The local field enhancement enabled by the extreme energy confinement of quasi‐BICs contributes to an efficient SHG, recording a conversion efficiency up to 2 × 10−7 at moderately low input peak intensity (≈1 GW cm−2), orders of magnitude larger than bulk GaN. With proper design, the overlapping X‐ and Y‐polarized resonances can support SHG from excitation with arbitrary polarizations. The alleviation of polarization‐matching remarkably enhances the SHG power by 66.2% under unpolarized illumination condition. The results of intense SHG reveal GaN as a promising candidate for high‐performance nanoscale nonlinear photonic devices. The weak polarization sensitivity of the designed structure will chart a novel course for the advancement of next‐generation efficient all‐dielectric metasurfaces. [ABSTRACT FROM AUTHOR]

Cyanation is a common chemical modification strategy to fine‐tune the energy levels and molecular packing of organic semiconductors, especially materials used in organic solar cells (OSCs). Generally, cyanation is used to modify the end groups of high‐performance small‐molecule acceptors (SMAs). However, the cyanation strategy has not been investigated on the central backbone of SMAs, which could introduce stronger intermolecular interaction and enhance the π–π stacking for rapid charge transport. This paper, for the first time, reports a new cyanation strategy on the central benzo‐quinoxaline core and synthesizes two novel A‐DA'D‐A type SMAs, named BQx‐CN and BQx‐2CN, with mono‐ and di‐cyanide groups, respectively. Through tailoring the number of CN groups, the BQx‐CN‐based OSC exhibits the best device performance of 18.8%, which is significantly higher than the non‐cyano BQx‐based one. The reason for the superior performance of BQx‐CN‐based devices can be attributed to the fine‐tuned energy level, stronger packing, and ideal phase segregation, which lead to superior exciton dissociation, faster charge transport, and suppressed recombination, therefore the highest fill factor (FF) and power conversion efficiencies (PCE). The research demonstrates the effectiveness of the cyanation strategy on the central core of SMAs for enhanced molecular packing and better performance of OSCs. [ABSTRACT FROM AUTHOR]

The emission peak shift caused by ion motion, especially under high bias voltage, is an obstacle to the development of blue perovskite light‐emitting diodes (PeLEDs). In this work, 3‐Aminopiperidine dihydrochloride (3AP) to construct heterocyclic dication Dion‐Jacobson (DJ) PeLEDs is introduced, and found that 3AP incorporation can retard the halide segregation and chloride loss, leading to the improvement of the emission spectral stability. By increasing the amount of 3AP (DJ phase), emission centers can be tuned from green to blue but the excitonic peak abnormally disappears, indicative of exciton delocalization. Photoluminescence quantum yield (PLQY) and ultrafast spectroscopy indicated that the introduction of 3AP can passivate defects and control the exciton delocalization to facilitate interlayer charge transfer. The external quantum efficiencies (EQE) of the obtained green (513 nm), sky blue (488 nm), and blue (478 nm) PeLEDs reached 3.0%, 7.1%, and 4.8%, respectively, and the maximum luminance is 10956, 1093 and 782 cd m−2, respectively. Most importantly, under high operating voltages from 3 to 10 V, the PeLEDs delivered outstanding spectral stability free of peak shift. [ABSTRACT FROM AUTHOR]

Despite recent advances, it is still difficult to fabricate deep blue‐emitting perovskite light‐emitting diodes (LEDs) that are immune to the color instability caused by halide mixing. This is largely because it is still challenging to achieve bright, stable, pure bromide perovskite materials with deep blue emission. Here, a novel strategy is reported for synthesizing ultrasmall CsPbBr3 quantum dots (QDs) under ambient conditions. Precise size control is used to tune the peak emission wavelengths, via the confinement effect, from 433 to 501 nm. These ultrasmall QDs, with sizes of 2–6 nm, exhibit ultralow trap density and stable photoluminescence quantum yields up to 94%, particularly in the deep blue spectral region (440–465 nm). QD‐LEDs fabricated with these materials achieve an external quantum efficiency of 1.0% at 459 nm. The exceptional control of the emission properties demonstrated here suggests a new strategy for building stable, efficient blue QD‐LEDs. [ABSTRACT FROM AUTHOR]

Organic solar cell (OSC) development continues to demonstrate impressive device efficiency improvements. However, the materials synthetic simplicity essential to industrialization remains seriously lacking attention, imparting inferior performance records in low‐cost devices. Hence, low bandgap and completely non‐fused electron acceptors (CNFEAs) having simple molecular structures are investigated herein. In contrast to typically explored fused‐ring acceptors with smaller backbone conformational variations, minimizing the interface recombination sites through a greater extent of localized domains is identified as more critical in CNFEAs, leading to remarkable fill factors (FFs) approaching 75%, among the highest currently realized for low‐cost systems. However, this comes with diminishing charge generation efficiency. The general ternary blend optimization strategy modifying the morphology of host components is limited in preserving such remarkably high FFs. To suppress the trade‐off while keeping notable FFs, a new perspective of constructing functionally bridged components based on optical, electronic, and thermodynamic properties is introduced here. Specifically, charge generation is unrestrained from the host acceptor localized domains through the introduction of a "bridge" component while also taking advantage of the configuration to channel polarons toward the efficient transport moieties of the host components. Accordingly, this work incubates understanding‐guided optimizations toward the advancement of more practical devices. [ABSTRACT FROM AUTHOR]

Hetero‐epitaxy for integration of efficient III‐V lasers on silicon can enable wafer‐scale silicon photonic integrated circuits, which can unleash the full advantages of silicon photonics in production on large silicon wafers with low cost, high throughput, and large bandwidth and large‐scale integration. In this work, efficient III‐V distributed feedback (DFB) lasers selectively grown on (001) silicon‐on‐insulator (SOI) wafers are presented. The selective hetero‐epitaxy of sufficiently large areas of III‐V segments allows the demonstration of DFB lasers on the SOI wafer. The fabricated DFB lasers feature a co‐planar configuration with the Si layer, allowing for efficient coupling between III‐V lasers and Si waveguides. The unique III‐V‐on‐insulator structure also provides strong optical confinement for the lasers. Gratings are designed and fabricated with minimal non‐radiative recombination and a simple process with good tolerance. The optically pumped DFB laser has a low lasing threshold of around 17.5 µJ cm−2, stable single‐mode lasing at 1.5 µm, a side‐mode‐suppression‐ratio of over 35 dB, and a spontaneous emission factor of 0.7. The results here demonstrate a step forward towards wafer‐scale integration with monolithically grown lasers, thus outlining the prospect of fully integrated Si photonics. [ABSTRACT FROM AUTHOR]

We demonstrate a novel approach for the easy fabrication of photonic crystals (PCs) with arbitrary optical lattice using two-photon holographic lithography (HL). The quadratic dependence of the two-photon absorption process dramatically increases the contrast of the pattern and the low absorption coefficient of the photoresist at 720 nm lead to a high aspect ratio and low fluctuation of the pattern. By applying such a technique, defect-free and highly uniform one-dimensional gratings, two-dimensional quasicrystals, and three-dimensional (3D) face center cube-type PCs of high aspect ratio and small filling factor are obtained. This two-photon based HL technique is particularly suitable for making 3D PCs and quasicrystals with complex and fine structural details. [ABSTRACT FROM AUTHOR]

In order to advance the development of quantum emitter‐based devices, it is essential to enhance light‐matter interactions through coupling between semiconductor quantum dots with high quality factor resonators. Here, efficient tuning of the emission properties of HgTe quantum dots in the infrared spectral region is demonstrated by coupling them to a plasmonic metasurface that supports bound states in the continuum. The plasmonic metasurface, composed of an array of gold nanobumps, is fabricated using single‐step direct laser printing, opening up new opportunities for creating exclusive 3D plasmonic nanostructures and advanced photonic devices in the infrared region. A 12‐fold enhancement of the photoluminescence in the 900–1700 nm range is observed under optimal coupling conditions. By tuning the geometry of the plasmonic arrays, controllable shaping of the emission spectra is achieved, selectively enhancing specific wavelength ranges across the emission spectrum. The observed enhancement and shaping of the emission are attributed to the Purcell effect, as corroborated by systematic measurements of radiative lifetimes and optical simulations based on the numerical solution of Maxwell's equations. Moreover, coupling of the HgTe photoluminescence to high quality factor modes of the metasurface improves emission directivity, concentrating output within an ≈20° angle. [ABSTRACT FROM AUTHOR]

Producing efficient blue and deep blue perovskite LEDs (PeLEDs) still represents a significant challenge in optoelectronics. Blue PeLEDs still have problems relating to color, luminance, and structural and electrical stability so new materials are needed to achieve better performance. Recent reports suggest using low n states (n = 1, 2, 3) to achieve blue electroluminescence in Ruddlesden–Popper (RP) perovskite films. However, there are fewer reports on the other quasi‐2D structure, Dion–Jacobson (DJ) perovksites, despite their highly desirable optical properties, due to the difficulty in achieving charge injection. To resolve this issue, herein, w e have mixed DJ phase precursors, propane‐1,3‐diammonium (PDA) bromide into RP phase perovskites and fabricated low‐dimensional PeLEDs. It is found that these specific precursors aid in suppressing both the low n (n = 1) and high n (n ≥ 4) quasi‐2D RP phases and is an effective strategy in blue‐shifting sky‐blue RP perovskites into the sub‐470 nm region. With optimization of the PDA concentration and device layers, it is achieved an external quantum efficiency of 1.5% at 469 nm and stable electroluminescence for the first deep blue PeLED to be reported using DJ perovskites. [ABSTRACT FROM AUTHOR]

Although the electroluminescent performances of perovskite light‐emitting diodes (PeLEDs) are continuously improved through defect management strategies, the complicated design of passivation ligands brings great challenges to the rational defect‐annihilation process. Herein, considering the bonding strength with uncoordinated Pb2+, the methoxy group with strong electron donating ability is introduced to commonly used phenethylammonium ligand as an efficient additive, namely 4‐methoxy‐phenethylammonium iodide (4‐MeO‐PEAI), to facilitate passivation process in perovskite light‐emitting materials. It is demonstrated that the 4‐MeO‐PEAI agent substantially increases the crystal orientation, enlarges the crystalline grain size, and mitigates the deep‐level trap centers through strong bonding between the methoxy group with unpaired Pb2+ ions. The external quantum efficiencyvalue of the PeLEDs with optimized passivation reaches a maximum of 21.6%, with an emission peak of 790 nm. In addition, a nearly threefold increase of the operational half‐lifetime T50 of the 4‐MeO‐PEAI‐mediated devices is observed as compared to the reference sample. Further theoretical calculation results suggest that the adhesion of the ligands on perovskite surface via vacancies leads to an increased dissociation barrier of perovskite; thus, ameliorating the degradation of the PeLEDs under electric field. The findings provide an effective design strategy of the passivation agents to produce high‐performance perovskite‐based optoelectronics devices. [ABSTRACT FROM AUTHOR]

Chiral perovskite nanocrystals have emerged as an interesting chiral excitonic platform that combines both structural flexibility and superior optoelectronic properties. Despite several recent demonstrations of optical activity in various chiral perovskite nanocrystals, efficient circularly polarized luminescence (CPL) with tunable energies remains a challenge. The chirality imprinting mechanism as a function of perovskite nanocrystal dimensionality remains elusive. Here, atomically thin inorganic perovskite nanoplatelets (NPLs) are synthesized with precise control of layer thickness and are functionalized by chiral surface ligands, serving as a unique platform to probe the chirality transfer mechanism at the organic/perovskite interface. It is found that chirality is successfully imprinted into mono‐, bi‐, and tri‐layer inorganic perovskite NPLs, exhibiting tunable circular dichroism (CD) and CPL responses. However, chirality transfer decreases in thicker NPLs, resulting in decreased CD and CPL dissymmetry factors for thicker NPLs. Aided by large‐scale first‐principles calculations, it is proposed that chirality transfer is mainly mediated through a surface distortion rather than a hybridization of electronic states, giving rise to symmetry breaking in the perovskite lattice and spin‐split conduction bands. The findings described here provide an in‐depth understanding of chirality transfer and design principles for distorted‐surface perovskites for chiral photonic applications. [ABSTRACT FROM AUTHOR]

Tuning the properties of non‐fullerene acceptors (NFAs) through halogenation, including fluorination and chlorination, represents one of the most promising strategies to boost the performance of organic solar cells (OSCs). However, it remains unclear how the F and Cl choice influences the molecular packing and performance between small‐molecule and polymeric acceptors. Here, a series of small‐molecule and polymeric acceptors with different amounts and types of halogenation is synthesized, and the effects of fluorination and chlorination between small‐molecule and polymeric acceptors are investigated. It is found that chlorinated small‐molecule acceptors lead to longer exciton diffusion length and better performance compared to the corresponding fluorinated ones, which attributes to their stronger intermolecular packing mode. For polymer acceptors, in contrast, the fluorinated polymers achieve a denser packing mode and better performance, because chlorinated polymers exhibit reduced intrachain conjugation between end group moieties and linker units. This study demonstrates different halogenation effects on the packing modes and performances for small‐molecule and polymeric acceptors, which provides important guidance for the molecule design of high‐performance acceptors for OSCs. [ABSTRACT FROM AUTHOR]

Highlights: Synergistic effect triggers the Ostwald ripening for the downward recrystallization of perovskite to form buried submicrocavities as light output coupler. The simulation suggests the buried submicrocavities can improve the light out-coupling efficiency from 26.8% to 36.2% for near-infrared light. Light-emitting diodes yields peak external quantum efficiency increasing from 17.3% at current density of 114 mA cm−2 to 25.5% at current density of 109 mA cm−2 and a radiance increasing from 109 to 487 W sr−1 m−2 with low rolling-off. Embedding submicrocavities is an effective approach to improve the light out-coupling efficiency (LOCE) for planar perovskite light-emitting diodes (PeLEDs). In this work, we employ phenethylammonium iodide (PEAI) to trigger the Ostwald ripening for the downward recrystallization of perovskite, resulting in spontaneous formation of buried submicrocavities as light output coupler. The simulation suggests the buried submicrocavities can improve the LOCE from 26.8 to 36.2% for near-infrared light. Therefore, PeLED yields peak external quantum efficiency (EQE) increasing from 17.3% at current density of 114 mA cm−2 to 25.5% at current density of 109 mA cm−2 and a radiance increasing from 109 to 487 W sr−1 m−2 with low rolling-off. The turn-on voltage decreased from 1.25 to 1.15 V at 0.1 W sr−1 m−2. Besides, downward recrystallization process slightly reduces the trap density from 8.90 × 1015 to 7.27 × 1015 cm−3. This work provides a self-assembly method to integrate buried output coupler for boosting the performance of PeLEDs. [ABSTRACT FROM AUTHOR]

Organic solar cells (OSC) feature a hierarchical structure with the electron donor/acceptor layer sandwiched by anode and cathode, which raises the importance of controlling the molecular crystal orientation, domain size, and vertical distribution to facilitate the charge collection at electrodes. However, the similar conjugated backbone of donor/acceptor material and fast film‐formation kinetics have led to spinodal‐decomposition‐orientated phase separation that result in the film presenting an intimately mixed morphology and random molecular orientation. To solve the issue, the mixing Gibbs free energy‐triggered solid–liquid phase separation during the film formation process is enhanced by solidifying one component and solvating the other based on a liquid additive. Following the liquid evaporation process, a favorable vertical distribution is obtained. Meanwhile, the prolonged solvation process enlarges the domain size and assists the molecules to diffuse and orient properly, enabling better exciton/charge dynamics during the power conversion processes. As a result, the fabricated devices exhibit a fill factor over 80% and an efficiency of 18.72%, which is one of the top efficiencies for binary OSCs. Insights and a methodology is provided here to manipulate the organic donor/acceptor phase separation in terms of mixing Gibbs free energy. [ABSTRACT FROM AUTHOR]

Due to the fast dynamics and re‐equilibration of supramolecular self‐assembly, bottom‐up molecular strategies to fabricate well‐defined and controllable multiblock structures are rare. Herein, we propose a new concept for fabrication of fluorescent multiblock microcolumns containing 1 to 7 blocks via hierarchical supramolecular self‐assembly based on cucurbit[8]uril (CB[8]), NaBr and an AIEgen guest. Through the complexation between CB[8] and different numbers of AIEgen guests (2, 1, 0), the competitive displacement caused by the binding of the sodium cation to the CB[8] portal, and the reversible assembly of positively charged guests in salt solutions, one‐pot hierarchical supramolecular self‐assembly is realized. The molecular structure of each block is analyzed by single‐crystal X‐ray diffraction. The AIEgen enables the self‐assembly of multiblocks to be visualized, understood, and regulated. [ABSTRACT FROM AUTHOR]

Due to the fast dynamics and re‐equilibration of supramolecular self‐assembly, bottom‐up molecular strategies to fabricate well‐defined and controllable multiblock structures are rare. Herein, we propose a new concept for fabrication of fluorescent multiblock microcolumns containing 1 to 7 blocks via hierarchical supramolecular self‐assembly based on cucurbit[8]uril (CB[8]), NaBr and an AIEgen guest. Through the complexation between CB[8] and different numbers of AIEgen guests (2, 1, 0), the competitive displacement caused by the binding of the sodium cation to the CB[8] portal, and the reversible assembly of positively charged guests in salt solutions, one‐pot hierarchical supramolecular self‐assembly is realized. The molecular structure of each block is analyzed by single‐crystal X‐ray diffraction. The AIEgen enables the self‐assembly of multiblocks to be visualized, understood, and regulated. [ABSTRACT FROM AUTHOR]

Central π‐core engineering of non‐fullerene small molecule acceptors (NF‐SMAs) is effective in boosting the performance of organic solar cells (OSCs). Especially, selenium (Se) functionalization of NF‐SMAs is considered a promising strategy but the structure‐performance relationship remains unclear. Here, we synthesize two isomeric alkylphenyl‐substituted selenopheno[3,2‐b]thiophene‐based NF‐SMAs named mPh4F‐TS and mPh4F‐ST with different substitution positions, and contrast them with the thieno[3,2‐b]thiophene‐based analogue, mPh4F‐TT. When placing Se atoms at the outer positions of the π‐core, mPh4F‐TS shows the most red‐shifted absorption and compact molecular stacking. The PM6 : mPh4F‐TS devices exhibit excellent absorption, high charge carrier mobility, and reduced energy loss. Consequently, PM6 : mPh4F‐TS achieves more balanced photovoltaic parameters and yields an efficiency of 18.05 %, which highlights that precisely manipulating selenium functionalization is a practicable way toward high‐efficiency OSCs. [ABSTRACT FROM AUTHOR]

Central π‐core engineering of non‐fullerene small molecule acceptors (NF‐SMAs) is effective in boosting the performance of organic solar cells (OSCs). Especially, selenium (Se) functionalization of NF‐SMAs is considered a promising strategy but the structure‐performance relationship remains unclear. Here, we synthesize two isomeric alkylphenyl‐substituted selenopheno[3,2‐b]thiophene‐based NF‐SMAs named mPh4F‐TS and mPh4F‐ST with different substitution positions, and contrast them with the thieno[3,2‐b]thiophene‐based analogue, mPh4F‐TT. When placing Se atoms at the outer positions of the π‐core, mPh4F‐TS shows the most red‐shifted absorption and compact molecular stacking. The PM6 : mPh4F‐TS devices exhibit excellent absorption, high charge carrier mobility, and reduced energy loss. Consequently, PM6 : mPh4F‐TS achieves more balanced photovoltaic parameters and yields an efficiency of 18.05 %, which highlights that precisely manipulating selenium functionalization is a practicable way toward high‐efficiency OSCs. [ABSTRACT FROM AUTHOR]

Low‐dimensional copper halides having nontoxic elements are attracting increasing attention for their peculiar emission properties. Self‐trapped excitons (STEs) account for their high photoluminescence quantum yields (PLQYs) with emission that can stretch across the entire visible spectrum. However, intrinsic factors that influence the formation or loss of the emissive species in low‐dimensional copper halides remain elusive. Here, a comprehensive study on the STE formation dynamics of one‐dimensional CsCu2I3 and zero‐dimensional Cs3Cu2I5 is presented. It is found from STE kinetic analysis that a slower STE formation demonstrated by the 1D structure is not hindered by a potential barrier, but instead related to the number of phonons released in the self‐trapping process. It is further revealed that in 1D CsCu2I3, the non‐radiative recombination of STEs mainly occurs via the intersection between the STE state and the ground state in the configuration coordinate diagram, placing an intrinsic limit on the PLQY at room temperature. These findings show that the STE formation is affected by both the self‐trapping depth and the phonon energy as opposed to a potential barrier in low‐dimensional copper halides. The better understanding of STE formation and recombination processes provide basis for improving design and performance for broadband light emitting devices. [ABSTRACT FROM AUTHOR]

Electron donors and acceptors in organic solar cells (OSCs) shall strike a favorable vertical phase separation that acceptors and donors have sufficient contact and gradient accumulation near the cathodes and anodes, respectively. Random mixing of donors/acceptors at surface will result in charge accumulation and severe recombination for low carrier‐mobility organic materials. However, it is challenging to tune the vertical distribution in bulk‐heterojunction films as they are usually made from a well‐mixed donor/acceptor solution. Here, for the first time, it presents with solid evidence that the commonly used 1‐chloronaphthalene (CN) additive can tune the donor/acceptor vertical distribution and establish the mechanism. Different from the previous understanding that ascribed the efficiency enhancement brought by CN to the improved molecular stacking/crystallization, it is revealed that the induced vertical distribution is the dominant factor leading to the significantly increased performance. Importantly, the vertical distribution tunability is effective in various hot nonfullerene OSC systems and creates more channels for the collection of dissociated carriers at corresponding organic/electrode interfaces, which contributes the high efficiency of 18.29%. This study of the material vertical distribution and its correlation with molecular stacking offers methods for additives selection and provides insights for the understanding and construction of high‐performance OSCs. [ABSTRACT FROM AUTHOR]

A ternary materials system, which comprises two-photon initiator, oligomer and poly(methyl methacrylate), was prepared. A polymeric waveguide film was manufactured by spinning the materials on ITO, and the two-photon initiated photopolymerization (TPIP) was carried out successfully in the waveguide film. Consequently, an approach using TPIP is demonstrated for fabrication of coupling grating in a thin polymeric film possessing waveguide properties. The results show that the incident laser can be coupled into the polymeric film by this coupling grating obtained from TPIP. The microstructure feature of coupling grating is illustrated, and waveguide mode and transmission loss of the polymeric film are investigated. [Copyright &y& Elsevier]

Transient optical spectroscopy is used to quantify the temperature‐dependence of charge separation and recombination dynamics in P3TEA:SF‐PDI2 and PM6:Y6, two non‐fullerene organic photovoltaic (OPV) systems with a negligible driving force and high photocurrent quantum yields. By tracking the intensity of the transient electroabsorption response that arises upon interfacial charge separation in P3TEA:SF‐PDI2, a free charge generation rate constant of ≈2.4 × 1010 s−1 is observed at room temperature, with an average energy of ≈230 meV stored between the interfacial charge pairs. Thermally activated charge separation is also observed in PM6:Y6, and a faster charge separation rate of ≈5.5 × 1010 s−1 is estimated at room temperature, which is consistent with the higher device efficiency. When both blends are cooled down to cryogenic temperature, the reduced charge separation rate leads to increasing charge recombination either directly at the donor‐acceptor interface or via the emissive singlet exciton state. A kinetic model is used to rationalize the results, showing that although photogenerated charges have to overcome a significant Coulomb potential to generate free carriers, OPV blends can achieve high photocurrent generation yields given that the thermal dissociation rate of charges outcompetes the recombination rate. [ABSTRACT FROM AUTHOR]

The performance of quasi‐2D perovskite light emitting diodes (LEDs) with mixed small cations, cesium and formamidinium (FA), is significantly affected by their ratio. The best devices obtained for Cs:FA ratio of 1:1 exhibit a maximum external quantum efficiency (EQE) of 12.1%, maximum luminance of 15 070 cd m−2 and maximum current efficiency of 46.1 cd A−1, which is significantly higher (about 3 times) compared to devices with FA only (maximum EQE of 4.1%, maximum luminance of 4521 cd m−2) and Cs‐only (maximum EQE of 4.0%, maximum luminance of 4886 cd m−2). The photoluminescence quantum yield of the Cs:FA 1:1 sample is similarly enhanced, 21.3% compared 5.4% and 6%, for FA‐only and Cs‐only samples, respectively. It can be observed that the Cs:FA ratio significantly affects the crystallization of the perovskite, with the optimal 1:1 ratio resulting in the formation of tetragonal Cs0.5FA0.5PbBr3 phase (different from cubic FAPbBr3 and orthorhombic CsPbBr3) with pronounced preferential orientation as well as a significant reduction in the trap density, which leads to a substantial improvement in the light‐emitting performance. [ABSTRACT FROM AUTHOR]

The electroluminescence efficiency of perovskite light‐emitting diodes (PeLEDs) has gained notable achievements, but the poor stability under electric stress severely impedes future practical use. Here, an alkyldiammonium 1,4‐butanediamine (BDA) is incorporated into perovskite emitting layer, which substantially optimizes electrochemical stability and minimizes interfacial deep traps under large external bias. The BDA‐PeLED shows a record operational half‐lifetime T50 of 189.4 h at a high current density of 100 mA cm−2 and 681 h under 50 mA cm−2. Additionally, the device maintains its original performance upon 2500 cycles of voltage scan and withstands 10 000 times of ON–OFF under a pulsed voltage of 2.5 V. Further degradation mechanism study reveals that the main origins of the instability property of PeLEDs without BDA are the generation of deep traps at the interfaces and the infiltration of anions into adjacent layers under long‐term electric stress. The significantly enhanced electrochemical stability suggests that alkyldiammonium cation incorporation can provide a direction to solve the instability issue of PeLEDs. [ABSTRACT FROM AUTHOR]

Chemical modifications of non‐fullerene acceptors (NFAs) play vital roles in the development of high efficiency organic solar cells (OSCs). In this work, on the basis of the previously reported molecule named Y6‐1O, chlorination and inner side‐chain engineering are adopted to endow the corresponding devices with higher open‐circuit voltage (VOC) and short‐circuit current density (JSC) as well as good morphology for high fill factor (FF). As a result, the molecule named BTP1O‐4Cl‐C12 can help achieve a higher power conversion efficiency (PCE) of 17.1% than that of Y6‐1O (16.1%). Furthermore, the following comparisons between BTP1O‐4Cl‐C12 and the two symmetric acceptors named BTP2O‐4Cl‐C12 and BTP‐4Cl‐C12 demonstrate the effect of asymmetric alkoxy substitution on the outer side chains, which not only achieves a balance between VOC and JSC, but also help obtain appropriate morphology for efficient charge dissociation and suppressed charge recombination. Therefore, the asymmetric BTP1O‐4Cl‐C12 can achieve a higher PCE compared to the symmetric BTP2O‐4Cl‐C12 and BTP‐4Cl‐C12. The work not only reports an excellent NFA for high‐performance OSCs, but also puts forward a series of methods for consecutive chemical modifications on Y‐series acceptors, which can be further applied to boost the PCE of OSCs to a higher level. [ABSTRACT FROM AUTHOR]

A solution‐processed top electrode is critical to unlock the full potential of all‐solution‐processed organic solar cells (OSCs) for practical applications. However, the enabled devices suffer from low efficiency (<12%) mainly because of the irreversible damages induced by the top‐electrode deposition process. Herein, a strategy of dry and nonimmersive sintering is demonstrated by introducing a hydrogen‐intercalated molybdenum oxide layer to sinter isolated Ag nanoparticles into the top electrode (all from solution process) with little influences/issues on underlying device structures. Fundamentally, it is unveiled that the intercalated hydrogen will bond with the amino group of the ligands around Ag nanoparticles, which promotes the exposed nanoparticles to merge along a certain crystal orientation (≈45°) and form a conductive electrode (8.6 Ω sq−1). Importantly, the sintered electrode offers 70% optical reflection in the 700–1050 nm wavelength region, which is essential to enhance the light absorption of high‐performance nonfullerene acceptors. Consequently, a record efficiency of 15% is achieved, driving all‐solution processed OSCs toward commercial applications. [ABSTRACT FROM AUTHOR]

The article titled "In-Plane 1.5 µm Distributed Feedback Lasers Selectively Grown on (001) SOI" discusses the development of efficient and in-plane III-V distributed feedback (DFB) lasers grown on (001) silicon-on-insulator (SOI) wafers. This method allows for precise placement of lasers in photonic integrated circuits, offering a scalable and cost-effective solution. The findings of this study have significant implications for achieving efficient coupling between lasers and waveguides, advancing the field of photonic integration. The authors of the article are Ying Xue, Jie Li, Yi Wang, Ke Xu, Zengshan Xing, Kam Sing Wong, Hon Ki Tsang, and Kei May Lau. [Extracted from the article]

The discovery of slow hot carrier cooling in hybrid organic–inorganic lead halide perovskites (HOIPs) has provided exciting prospects for efficient solar cells that can overcome the Shockley–Queisser limit. Questions still loom over how electron‐phonon interactions differ from traditional polar semiconductors. Herein, the electron‐phonon coupling (EPC) strength of common perovskite films (MAPbBr3, MAPbI3, CsPbI3, and FAPbBr3) is obtained using transient absorption spectroscopy by analyzing the hot carrier cooling thermodynamics via a simplified two‐temperature model. Density function theory calculations are numerically performed at relevant electron‐temperatures to confirm experiments. Further, the variation of carrier‐temperature over a large range of carrier‐densities in HOIPs is analyzed, and an "S‐shaped" dependence of the initial carrier‐temperature to carrier‐density is reported. The phenomenon is attributed to the dominance of the large polaron screening and the destabilization effect which causes an increasing‐decreasing fluctuation in temperature at low excitation powers; and a hot‐phonon bottleneck which effectively increases the carrier temperature at higher carrier‐densities. The turning point in the relationship is indicative of the critical Mott density related to the nonmetal‐metal transition. The EPC analysis provides a novel perspective to quantify the energy transfer in HOIPs, electron‐lattice subsystem, and the complicated screening‐bottleneck interplay is comprehensively described, resolving the existing experimental contradictions. [ABSTRACT FROM AUTHOR]

The traditional design strategies for highly bright solid‐state luminescent materials rely on weakening the intermolecular π–π interactions, which may limit diversity when developing new materials. Herein, we propose a strategy of tuning the molecular packing mode by regioisomerization to regulate the solid‐state fluorescence. TBP‐e‐TPA with a molecular rotor in the end position of a planar core adopts a long‐range cofacial packing mode, which in the solid state is almost non‐emissive. By shifting molecular rotors to the bay position, the resultant TBP‐b‐TPA possesses a discrete cross packing mode, giving a quantum yield of 15.6±0.2 %. These results demonstrate the relationship between the solid‐state fluorescence efficiency and the molecule's packing mode. Thanks to the good photophysical properties, TBP‐b‐TPA nanoparticles were used for two‐photon deep brain imaging. This molecular design philosophy provides a new way of designing highly bright solid‐state fluorophores. [ABSTRACT FROM AUTHOR]

The direct growth of III–V lasers on the industry-standard Si-platforms is the key for fully integrated Si-photonics. Conventional III–V hetero-epitaxy on Si substrates is plagued by crystalline defects generated at the mismatched interface, and thick buffers are often used to mitigate the issues. Here, we report the direct deposition of room temperature III–V micro- and nano-lasers on amorphous SiO2 layers. Without the requirement of crystalline substrates nor having to cope with the long-lasting lattice-mismatch problem, we demonstrate the direct hetero-epitaxy of dislocation-free III–V nanopillars and micro-islands on amorphous SiO2 layers. As the epitaxial InP crystals are embedded inside a low-index environment, we observed strong room temperature lasing from the as-grown InP crystallites under optical excitation. [ABSTRACT FROM AUTHOR]

Cell staining is a fascinating research area where monitoring and visualizing different cell organelles can be done using fluorescence techniques. However, the design and synthesis of organelle‐targeting fluorophores is still a challenge for several specific organelles. Herein, a platform for synthesizing efficient red‐emitting aggregation‐induced emission luminogens (AIEgens) with donor–acceptor characteristics is reported. The core molecule can be easily functionalized in order to modulate organelle targeting. The three synthesized AIEgens exhibit quantum yields of up to 39.3% and two‐photon absorption cross‐section values of up to 162 GM. The two zwitterionic AIEgens, CDPP‐3SO3 and CDPP‐4SO3, with the sulfonate function group, are successfully utilized for specific one‐photon and two‐photon imaging of the endoplasmic reticulum (ER) in live human cells. Substituting the zwitterionic nature with a singly positive charge group, one‐photon and two‐photon imaging of CDPP‐BzBr shows mitochondrial specificity, indicating the importance of the zwitterionic group for ER‐targeting. Owing to the good in vitro photostability, cell viability, and high efficiency, these red dyes serve as a good potential candidate for specific organelle targeting, as well as illustrate how such a platform can easily aid in the study of structure–property relationships for designing such probes. [ABSTRACT FROM AUTHOR]

Ruddlesden–Popper halide perovskite (RPP) materials are of significant interest for light‐emitting devices since their emission wavelength can be controlled by tuning the number of layers n, resulting in improved spectral stability compared to mixed halide devices. However, RPP films typically contain phases with different n, and the low n phases tend to be unstable upon exposure to humidity, irradiation, and/or elevated temperature which hinders the achievement of pure blue emission from n = 2 films. In this work, two spacer cations are used to form an RPP film with mixed cation bilayer and high n = 2 phase purity, improved stability, and brighter light emission compared to a single spacer cation RPP. The stabilization of n = 2 phase is attributed to favorable formation energy, reduced strain, and reduced electron–phonon coupling compared to the RPP films with only one type of spacer cation. Using this approach, pure blue light‐emitting diodes (LEDs) with Commission Internationale de l'éclairage (CIE) coordinates of (0.156, 0.088) and excellent spectral stability are achieved. [ABSTRACT FROM AUTHOR]

Photostability is a particularly important parameter for fluorescence imaging especially long-term dynamic tracking in live samples. However, many organic fluorophores show poor photostability under one-photon and two-photon continuous irradiation. In addition, these traditional fluorophores also suffer from aggregation-caused quenching (ACQ) in aggregate state in insolvable water environment. Therefore, it remains challenging to develop photostable and ACQ-free fluorophores for biological imaging. In this work, we developed two highly photostable aggregation-induced emission luminogens (AIEgens) based on the cyanostilbene core for in vitro and ex vivo bioimaging. These AIEgens named CS-Py+SO 3 − and CS-Py+ exhibit near-infrared solid-state emission, large Stokes shift (>180 nm), high fluorescence quantum yield (12.8%–13.7%) and good two-photon absorption cross section (up to 88 GM). CS-Py+SO 3 − and CS-Py+ show specific organelle staining with high biocompatibility in membrane and mitochondria in live cells, respectively. In addition, selective two-photon mitochondria visualization in live rat skeletal muscle tissues with deep-tissue penetration (about 100 μm) is successfully realized by using CS-Py+. Furthermore, these AIEgens especially CS-Py+ exhibit remarkably high resistance to photobleaching under one-photon and two-photon continuous irradiation. These highly photostable AIEgens could be potentially utilized in visualizing and tracking specific organelle-associated dynamic changes in live systems. Image 1 [ABSTRACT FROM AUTHOR]

Abstract: Solution‐processed and low‐temperature Sn‐rich perovskites show their low bandgap of about 1.2 eV, enabling potential applications in next‐generation cost‐effective ultraviolet (UV)–visible (vis)–near infrared (NIR) photodetection. Particularly, the crystallization (crystallinity and orientation) and film (smooth and dense film) properties of Sn‐rich perovskites are critical for efficient photodetectors, but are limitedly studied. Here, controllable crystallization for growing high‐quality films with the improvements of increased crystallinity and strengthened preferred orientation through a introducing rubidium cation into the methylammonium Sn‐Pb perovskite system (65% Sn) is achieved. Fundamentally, the theoretical results show that rubidium incorporation causes lower surface energy of (110) plane, facilitating growth in the dominating plane and suppressing growth of other competing planes. Consequently, the methylammonium‐rubidium Sn‐Pb perovskite photodetectors simultaneously achieve larger photocurrent and lower noise current. Finally, highly efficient UV–vis–NIR (300–1100 nm) photodetectors with record‐high linear dynamic range of 110 and 3 dB cut‐off frequency reaching 1 MHz are demonstrated. This work contributes to enriching the cation selection in Sn‐Pb perovskite systems and offering a promising candidate for low‐cost UV–vis–NIR photodetection. [ABSTRACT FROM AUTHOR]

Abstract: Hole transport layer (HTL) plays a critical role for achieving high performance solution‐processed optoelectronics including organic electronics. For organic solar cells (OSCs), the inverted structure has been widely adopted to achieve prolonged stability. However, there are limited studies of p‐type effective HTL on top of the organic active layer (hereafter named as top HTL) for inverted OSCs. Currently, p‐type top HTLs are mainly 2D materials, which have an intrinsic vertical conduction limitation and are too thin to function as practical HTL for large area optoelectronic applications. In the present study, a novel self‐assembled quasi‐3D nanocomposite is demonstrated as a p‐type top HTL. Remarkably, the novel HTL achieves ≈15 times enhanced conductivity and ≈16 times extended thickness compared to the 2D counterpart. By applying this novel HTL in inverted OSCs covering fullerene and non‐fullerene systems, device performance is significantly improved. The champion power conversion efficiency reaches 12.13%, which is the highest reported performance of solution processed HTL based inverted OSCs. Furthermore, the stability of OSCs is dramatically enhanced compared with conventional devices. The work contributes to not only evolving the highly stable and large scale OSCs for practical applications but also diversifying the strategies to improve device performance. [ABSTRACT FROM AUTHOR]

Abstract: The effects of alkyl chain regiochemistry on the properties of donor polymers and performances of non‐fullerene organic solar cells are investigated. Two donor polymers (PfBTAZ and PfBTAZS) are compared that have nearly identical chemical structures except for the regiochemistry of alkyl chains. The optical properties and crystallinity of two polymers are nearly identical yet the PfBTAZ:O‐IDTBR blend exhibits nearly double domain size compared to the blend based on PfBTAZS:O‐IDTBR. To reveal the origins of the very different domain size of two blends, the morphology of neat polymer films is characterized, and it is found that PfBTAZ tends to aggregate into much larger polymer fibers without the presence of O‐IDTBR. This indicates that it is not the polymer:O‐IDTBR interactions but the intrinsic aggregation properties of two polymers that determine the morphology features of neat and blend films. The stronger aggregation tendency of PfBTAZ could be explained by its more co‐planar geometry of the polymer backbone arising from the different alkyl chain regiochemistry. Combined with the similar trend observed in another set of donor polymers (PTFB‐P and PTFB‐PS), the results provide an important understanding of the structure–property relationships that could guide the development of donor polymers for non‐fullerene organic solar cells. [ABSTRACT FROM AUTHOR]

Luminogens with aggregation-induced emission characteristics (AIEgens) are intriguing due to its rapid expansion in various high-tech applications. However, there is still in high demand on the development of novel AIEgens with easy preparation and functionalization, stable structures, tunable emissions, and high quantum efficiency. In this contribution, three AIEgens based on diphenyl isoquinolinium (IQ) derivatives are reported. They can be facilely synthesized and possess high structural stability, favorable visible light excitation, large Stokes shifts, high quantum yields, tunable colors, and sufficient two-photon absorption of near-infrared light. Importantly, they exhibit multifunctionalities. They exhibit mechanochromic property, making them capable to be applied for rewritable papers. They can also be applied in mitochondrial imaging with high specificity, cell permeability, brightness, biocompatibility, and photostability. They are promising for the applications in evaluation of mitochondrial membrane potential and image-guided cancer cell ablation. Last, they are able to stain bacteria in a wash-free manner. All these intriguing results suggest such readily accessible and multifunctional diphenyl IQ-based AIEgens provide a new platform for construction of advanced materials for practical applications. [ABSTRACT FROM AUTHOR]

The mixed perovskite (FAPbI3)1− x(MAPbBr3) x, prepared by directly mixing different perovskite components, suffers from phase competition and a low-crystallinity character, resulting in instability, despite the high efficiency. In this study, a dual ion exchange (DIE) method is developed by treating as-prepared FAPbI3 with methylammonium brodide (MABr)/tert-butanol solution. The converted perovskite thin film shows an optimized absorption edge at 800 nm after reaction time control, and the high crystallinity can be preserved after MABr incorporation. More importantly, it is found that the threshold electrical field to initiate ion migration is greatly increased in DIE perovskite thin film because excess MABr on the surface can effectively heal structural defects located on grain boundaries during the ion exchange process. It contributes to the over-one-month moisture stability under ≈65% room humidity (RH) and greatly enhanced light stability for the bare perovskite film. As a result of preserved high crystallinity and simultaneous grain boundary passivation, the perovskite solar cells fabricated by the DIE method demonstrate reliable reproducibility with an average power conversion efficiency (PCE) of 17% and a maximum PCE of 18.1%, with negligible hysteresis. [ABSTRACT FROM AUTHOR]

In article number 1601882, Keyou Yan, Jianbin Xu, and co‐workers report a simple intermediate halide exchange reaction between nonstoichiometric FAI and unstable intermediate HPbI2Br to produce high‐quality FAPbI3‐xBrx thin films with crystal domain up to 2‐3 μm, eliminating the use of antisolvent dripping process. And it demonstrates outstanding opto‐electronic performances as well as enhanced stability under moisture and heat stress. [ABSTRACT FROM AUTHOR]

While indirectly patterned organic-inorganic hybrid perovskite nanostructures have been extensively studied for use in perovskite optoelectronic devices, it is still challenging to directly pattern perovskite thin films because perovskite is very sensitive to polar solvents and high-temperature environments. Here, a simple and low-cost approach is proposed to directly pattern perovskite solid-state films into periodic nanostructures. The approach is basically perovskite recrystallization through phase transformation with the presence of a periodic mold on an as-prepared solid-state perovskite film. Interestingly, this study simultaneously achieves not only periodically patterned perovskite nanostructures but also better crystallized perovskites and improved optical properties, as compared to its thin film counterpart. The improved optical properties can be attributed to the light extraction and increased spontaneous emission rate of perovskite gratings. By fabricating light-emitting diodes using the periodic perovskite nanostructure as the emission layers, approximately twofold higher radiance and lower threshold than the reference planar devices are achieved. This work opens up a new and simple way to fabricate highly crystalline and large-area perovskite periodic nanostructures for low-cost production of high-performance optoelectronic devices. [ABSTRACT FROM AUTHOR]

A new chiral tetraphenylethene derivative with two l -leucine-containing attachments, TPE-DLEU, has been designed and synthesized by Cu(I)-catalyzed azide-alkyne cycloaddition “click” reaction. It emits faintly and gives weak circular dichroism (CD) signals in solutions, but shows strong fluorescence and Cotton effects in the aggregated state, showing aggregation-induced emission (AIE) and CD (AICD) characteristics. Furthermore, its film displays circularly polarized luminescence (CPL) with an emission dissymmetry factor of +3.2 × 10 −3 . Interestingly, TPE-DLEU exhibits controllable helical self-assembly behaviours. It could readily assemble into right-handed helical nanofibers upon the evaporation of its 1,2-dichloroethane (DCE) solution, but form left-handed helical nanofibers by the addition of hexane to its DCE solution. [ABSTRACT FROM AUTHOR]

A series of newly synthesized dicyanoplatinum(II) 2,2′-bipyridine complexes exhibits self-assembly properties in solution after the incorporation of the l-valine amino units appended with various hydrophobic motifs. These l-valine-derived substituents were found to have critical control over the aggregation behaviors of the complexes in the solution state. On one hand, one of the complexes was found to exhibit interesting circularly polarized luminescence (CPL) signals at low temperature due to the formation of chiral spherical aggregates in the temperature-dependent studies. On the other hand, systematic transformation from less uniform aggregates to well-defined fibrous and rod-like structures via Pt⋅⋅⋅Pt and π-π stacking interactions has also been observed in the mixed-solvent studies. These changes were monitored by UV/Vis absorption, emission, circular dichroism (CD), and CPL spectroscopies, and morphologies were studied by electron microscopy. [ABSTRACT FROM AUTHOR]

NiO is a promising hole transporting material for perovskite solar cells due to its high hole mobility, good stability, easy processibility, and suitable Fermi level for hole extraction. However, the efficiency of NiO-based cells is still limited by the slow hole extraction due to the poor perovskite/NiO interface and the inadequate quality of the two solution-processed material phases. Here, large influences of a monolayer surface modification of NiO nanocrystal layers with ethanolamine molecules are demonstrated on the enhancement of hole extraction/transport and thus the photovoltaic performance. The underlying causes have been revealed by a series of studies, pointing to a favorable dipole layer formed by the molecular adsorption along with the enhanced perovskite crystallization and the improved interface contact. Comparatively, the solar cells based on a diethanolamine-modified NiO layer have achieved a rather high fill factor, indeed one of the highest among NiO-based perovskite solar cells, and high short-circuit photocurrent density ( Jsc), resulting in a power conversion efficiency of ≈16%, most importantly, without hysteresis. [ABSTRACT FROM AUTHOR]

Carbon-based hole transport material (HTM)-free perovskite solar cells (PSCs) have shown much promise for practical applications because of their high stability and low cost. However, the efficiencies of this kind of PSCs are still relatively low, especially for the simplest paintable carbon-based PSCs, in comparison with the organic HTM-based PSCs. This can be imputed to the perovskite deposition methods that are not very suitable for this kind of devices. A solvent engineering strategy based on two-step sequential method is exploited to prepare a high-quality perovskite layer for the paintable carbon-based PSCs in which the solvent for CH3NH3I (MAI) solution at the second step is changed from isopropanol (IPA) to a mixed solvent of IPA/Cyclohexane (CYHEX). This mixed solvent not only accelerates the conversion of PbI2 to CH3NH3PbI3 but also suppresses the Ostwald ripening process resulting in a high-quality perovskite layer, e.g., pure phase, even surface, and compact capping layer. The paintable carbon-based PSCs fabricated from IPA/CYHEX solvent exhibits a considerable enhancement in photovoltaic performance and performance reproducibility in comparison with that from pure IPA, especially on fill factor (FF), owing mainly to the better contact of perovskite/carbon interface, lower trap density in perovskite, higher light absorption ability, and faster charge transport of perovskite layer. As a result, the highest power conversion efficiency (PCE) of 14.38% is obtained, which is a record value for carbon-based HTM-free PSCs. Furthermore, a PCE of as high as 10% is achieved for the large area device (1 cm2), also the highest of its kind. [ABSTRACT FROM AUTHOR]

The photovoltaic performance of perovskite solar cells (PVSCs) is extremely dependent on the morphology and crystallization of the perovskite film, which is affected by the deposition method. In this work, a new approach is demonstrated for forming the PbI2 nanostructure and the use of high CH3 N3 I concentration which are adopted to form high-quality (smooth and PbI2 residue-free) perovskite film with better photovoltaic performances. On the one hand, self-assembled porous PbI2 is formed by incorporating small amount of rationally chosen additives into the PbI2 precursor solutions, which significantly facilitate the conversion of perovskite without any PbI2 residue. On the other hand, by employing a relatively high CH3NH3 I concentration, a firmly crystallized and uniform CH3NH3 PbI3 film is formed. As a result, a promising power conversion efficiency of 16.21% is achieved in planar-heterojunction PVSCs. Furthermore, it is experimentally demonstrated that the PbI2 residue in perovskite film has a negative effect on the long-term stability of devices. [ABSTRACT FROM AUTHOR]

We present a nitrogen-containing polycyclic aromatic hydrocarbon (N-PAH), namely 12-methoxy-9-(4-methoxyphenyl)-5,8-diphenyl-4-(pyridin-4-yl)pyreno[1,10,9- h, i, j]isoquinoline ( c-TPE-ON), which exhibits high quantum-yield emission both in solution (blue) and in the solid state (yellow). This molecule was unexpectedly obtained by a three-fold, highly regioselective photocyclodehydrogenation of a tetraphenylethylene-derived AIEgen. Based on manifold approaches involving UV/Vis, photoluminescence, and NMR spectroscopy as well as HRMS, we propose a reasonable mechanism for the formation of the disk-like N-PAH that is supported by density functional theory calculations. In contrast to most PAHs that are commonly used, our system does not suffer from entire fluorescence quenching in the solid state due to the peripheral aromatic rings preventing π-π stacking interactions, as evidenced by single-crystal X-ray analysis. Moreover, its rod-like microcrystals exhibit excellent optical waveguide properties. Hence, c-TPE-ON comprises a N-PAH with unprecedented luminescent properties and as such is a promising candidate for fabricating organic optoelectronic devices. Our design and synthetic strategy might lead to a more general approach to the preparation of solution- and solid-state luminescent PAHs. [ABSTRACT FROM AUTHOR]