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This article explores the shift in chemical physics research towards studying single molecules and nanoparticles instead of bulk samples. Advancements in experimental techniques, such as single-molecule absorption and fluorescence spectroscopy, have made this shift possible. The article discusses various observations made through single-molecule spectroscopy, as well as theoretical considerations and applications in biology, materials science, and nanophotonics. It provides a summary of studies conducted using single-molecule spectroscopy in different disciplinary categories, demonstrating its interdisciplinary nature. The article concludes by discussing the challenges and future directions in the field, including integrating particle tracking with time-dependent spectroscopy and actively manipulating nanoscale objects. [Extracted from the article]

Polymer dielectrics with excellent capacitive performance are urgently needed in advanced electrical and electronic systems. However, due to the dramatic increase in the conduction loss, the energy density and efficiency of polymers degrade severely at elevated temperatures, limiting their application in harsh environments up to 150 °C. Herein, an all-organic polyurea (PU)/polyetherimide (PEI) blend film is designed to prepare high-temperature polymer dielectric. It is found that carrier traps can be introduced by blending, and the hydrogen bond between PU and PEI increases the trap depth, leading to suppressed leakage current and enhanced breakdown strength, thus improving the energy storage performance. PU/30%PEI exhibits a high discharged energy density of ∼3.74 J/cm3 with an efficiency higher than 90% at 150 °C, which is 78% and 70% higher than pristine PU and PEI, respectively. This work provides a facile strategy to improve the energy storage performance of polymer dielectrics by introducing deep traps through blending. [ABSTRACT FROM AUTHOR]

Organic photovoltaic devices (OPVs) are attracting attention because of recent rapid enhancement of their power conversion efficiency. For further improvement, optimization of fabrication processes is one useful path to a solution. During OPV fabrication, particularly of the bulk heterojunction active layer, annealing treatments contribute to the device performance. Many studies have examined annealing-related properties. However, further research must clarify how paramagnetic species in the devices play their roles by annealing. Using well-known OPVs, we investigated the relation between spin-dependent recombination (SDR) current and the paramagnetic species, which vary the numbers by post-annealing with active layers consisting of poly(3-hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl-C 61 -butyric acid methyl ester (PC 61 BM). A simultaneous detection method of electron spin resonance (ESR) and electrically detected magnetic resonance (EDMR), which we originally developed, was applied to OPVs for the first time ever reported. Results show that PC 61 BM anion radicals generated by post-annealing of P3HT:PC 61 BM OPVs with a lithium fluoride (LiF)/aluminum (Al) electrode do not contribute to the SDR current at the interface and that P3HT cation radicals enhance the SDR current. By contrast, devices with an Al electrode without LiF decrease the total SDR current, although the quantities of cation radical molecules do not vary. This finding suggests that changes of the hole blocking layer in the devices caused by the annealing treatment affect the size of capture cross sections of P3HT cation radicals. Our new method of quantitative observation of the EDMR changes through the ESR signals is expected to be useful for investigating the capture cross sections in OPVs. [ABSTRACT FROM AUTHOR]

π-conjugated polymers have been used in a wide range of practical applications, partly due to their unique properties that originate in the delocalization of electrons through the polymer backbone. The level of delocalization can be characterized by the induced bond length alternation (BLA), with shorter BLA connected with strong delocalization and vice versa. The accurate description of this structural parameter can be considered a benchmark for testing the capability of different electronic structure methods for self-interaction error (SIE) removal and electron correlation inclusion. Density functional theory (DFT), in its local or semi-local flavors, suffers from SIE and, thus, underestimates the BLA compared to self-interaction-free methods. In this work, we utilize the Fermi–Löwdin orbital self-interaction correction (FLOSIC) method for one-electron self-interaction removal to characterize the BLA of five oligomers with increasing length extrapolated to the polymeric limit. We compare the self-interaction-free BLA to several DFT approximations, Møller–Plesset second-order perturbation theory (MP2), and the BLA obtained with the domain based local pair natural orbital CCSD(T) [DLPNO-CCSD(T)] approximation. Our findings show that FLOSIC corrects for the small BLA given by (semi-)local DFT approximations, but it tends to overcorrect with respect to CAM-B3LYP, MP2, and DLPNO-CCSD(T). [ABSTRACT FROM AUTHOR]

Understanding and modulating the spin-pair correlation of conjugated polymer materials in π-conjugated polymer light-emitting devices (PLEDs) plays a crucial role in the development of their applications. We investigated the relationships between the internal hyperfine interactions (HFIs), triplet–triplet annihilation (TTA), and triplet–charge annihilation (TCA) spin evolution processes in π-conjugated PLED. Research has shown that in a unipolar π-conjugated PLED, the "M" shaped ultra-small magnetic field effect is due to the HFI between hole polarons and the spin-mixing process of charge carriers. Under high magnetic fields (15 mT<|B|<350 mT), the TCA process dominates the negative magneto-conductance (MC), and its intensity and sign are not controlled by temperature. In polar π-conjugated PLED, excess carriers can provide conditions for the generation of TCA. Moreover, π-conjugated polymers (emission layers) have relatively strong electron–phonon coupling, which can capture triplet excitons into adjacent organic layers to obtain higher triplet exciton concentrations, resulting in the TTA process. Under low-temperature conditions, excess carriers induce the magneto-electroluminescence (MEL) effect to undergo TTA and form P-type delayed fluorescence. This study can provide a new mechanism explanation for the HFI in PLED devices and a new approach for the effective utilization of triplets. [ABSTRACT FROM AUTHOR]

The type of aggregation in conjugated polymers determines their use in electronic devices. H-type aggregates are most suitable for solar cell applications, while J-type aggregates are recommended for light-emitting diodes. In this work, we used three methods to determine the type of aggregates in a benzodithiophene–isoindigo-based (PBDTI-DT) copolymer, namely, Huang–Rhys factor evolution with temperature, Franck–Condon analysis, and relative quantum yield (QY) calculation. All three methods indicate that both aggregation types are present, and the QY calculation clearly indicates that H-aggregates are more dominant. Time-dependent density functional theory was used to identify the two absorption bands of PBDTI-DT as local π − π* and intramolecular charge-transfer transitions. [ABSTRACT FROM AUTHOR]

[Display omitted] The diversity of catalytic products determines the difficulty of selective product modulation, which usually relies on adjusting the catalyst and reaction conditions to obtain different main products selectively. Herein, we synthesized D-π-A-D conjugated organic polymers (TH-COP) using cyclotriphosphonitrile, alkyne, 2H-benzimidazole, and sulfur units as electron donors, π bridges, electron acceptors, and electron donors, respectively. TH-COP exhibited excellent photoinduced carrier separation and redox ability under different visible light wavelengths, and the main products of its CO 2 reduction are CH 4 (1000.0 μmol g−1) and CO (837.0 μmol g−1) under 400–420 nm and 420–560 nm, respectively. In addition, TH-COP could completely convert phenylmethyl sulfide to methyl phenyl sulfone at 400–420 nm and diphenyl disulfide at 480–485 nm in yields up to 95 %. This study presents a novel strategy for the targeted fabrication of various main products using conjugated polymers by simply changing the wavelength range of visible light. [ABSTRACT FROM AUTHOR]

The significant interfacial resistance between solid electrolyte‐electrode interfaces is a major bottleneck for the practical application of solid‐state lithium batteries. This resistance is primarily caused by the formation of space charge layers (SCLs), resulting from the redistribution of ionic carriers at the interface between dissimilar materials with varying chemical potentials, which lead to insufficient carriers and sluggish lithium‐ion transport. In this study, a conjugated structure polymer is constructed through in situ polymerization onto the oxide electrolyte, forming charge‐rich SCLs on the organic/inorganic interface, and enabling the interfacial layer to maintain superior ion transfer and contact. The Li solid NMR spectra and computational study suggest that optimized SCLs offer effective pathways for Li+ conduction in the electrolyte, thereby enhancing the interfacial conduction. Furthermore, the designed electrolyte induces the formation of an inorganic‐rich interphase layer on the lithium anode, enabling rapid lithium‐ion transport and uniform Li deposition. Consequently, the lithium symmetric cell with this electrolyte operates for more than 5100 h, while LiFePO4/Li solid‐state batteries can stably cycle up to 800 times at 5 C. This interfacial modification strategy provides a new perspective for the rational design of the charge‐rich SCLs and advances the understanding of the SCLs inside the electrolyte. [ABSTRACT FROM AUTHOR]

Low efficiency of photogenerated electron–hole separation has been a challenge for organic conjugated polymer photocatalysts. Our preceding studies have revealed that polymers containing B←N coordination bonds can form a localized built-in electric field that effectively promotes photogenerated charge separation. However, B←N coordination units are still scarce and require more examples to find regularities in their structural design. The systematic development and testing of B←N coordination units is necessary for the efficient development of subsequent polymers containing B←N coordination bonds. In this work, three conjugated polymers containing B←N coordination bonds, PBN–Ni, PBP–Ni, and PBS–Ni, were synthesized by changing the substituents of the boron atoms and introducing narrow-band thiophene units to form conjugate and energy band gradients. The energy band modulation and localized built-in electric field construction were both achieved as planned, while the bandgap and photogenerated charge transport capabilities caused performance discrepancies. The experimental results showed that PBN–Ni had a better photocatalytic hydrogen evolution (HER) performance, reaching 104.6 μmol h−1 (λ > 420 nm). The optimal optical absorption edge of PBS–Ni was up to 643 nm, but the HER was lower, at 33.2 μmol h−1 (λ > 420 nm, 1% Pt). PBP–Ni optimized some of the optical absorption efficiencies (511 nm) while ensuring the HER activity (96.6 μmol h−1, λ > 420 nm). This work tentatively explores the characterization of the B←N coordination bond-containing base units serving as photocatalysts and provides the basic model experience and data reference for the subsequent expansion of B←N coordination bond-containing units and the development of B←N coordination bond-containing copolymer systems. [ABSTRACT FROM AUTHOR]

We present a novel synthetic route for the rapid construction of dithieno[3′,2′:3,4;2′′,3′′:5,6]benzo[1,2‐c][1,2,5]thiadiazoles via Na2S‐promoted thiophene annulation. This method facilitated the synthesis of D18−Cl polymer, known for its efficacy as a polymer donor in bulk‐heterojunction polymer solar cells. Starting from commercially available 4,7‐dihalo‐5,6‐difluorobenzo[c][1,2,5]thiadiazole, various 4,7‐dialkynylated compounds were obtained through Sonogashira reaction conditions. Subsequent Na2S‐promoted thiophene annulations yielded DTBT and its derivatives in excellent yields within 10 minutes. DTBT was then utilized as a precursor for the concise synthesis of D18−Cl, benefiting from reduced synthetic steps, mild reaction conditions, decreased complexity, and high overall yields. In another route, a space group‐bridged DTBT was directly constructed via Na2S‐promoted thiophene annulations and converted into D18−Cl through a couple of steps. This developed protocol offers a straightforward and reliable synthetic tool, conducive to reducing complexities in the production of DTBT‐based organic electronic materials, thereby advancing the potential commercialization of organic solar cells. [ABSTRACT FROM AUTHOR]

This account summarizes the impact that the quest for sustainability is having on the field of organic polyconjugate molecules and polymers for plastic (opto)electronics. While at the proof-of-concept level, the design criteria as well as the preferred synthetic strategies to access new and improved materials have been dominated by the need for performance. The ongoing transition from the lab environment to the industrial scale imposes strict limitations on the cost and overall environmental impact of new materials. We here summarize our efforts on the development of new design criteria and synthetic strategies aimed at improving sustainability – without compromising performance – in organic polyconjugated molecules. The article is composed of three sections: Introduction and motivation, sustainability through improved synthetic methods and through improved design. Outline 1 Introduction and Motivation 2 Sustainable Reaction Methods 2.1 The New Tools: Reactions in Aqueous Solution of Surfactants 2.2 Intrinsically More Sustainable Reactions: Direct Arylation 2.3 Sustainable Multistep Protocols: Combining Micellar, Solventless, and Mechanochemical Methods 3 Sustainability as a Design Criterion: De Novo Design 4 Conclusion [ABSTRACT FROM AUTHOR]

Photocatalytic hydrogen evolution has attracted tremendous interest as it offers a process for generation of green hydrogen based on solar radiation. But the process is extremely complex as many factors influence photocatalytic hydrogen evolution. While novel photocatalysts such as MOFs, perovskites, conjugated polymers, carbon-based materials, quantum dots, and others face challenges such as stability and scalability, semiconductor photocatalysts and cocatalysts such as TiO 2 /Pt, Ni–CdS, CdS/ZnO, CdS/ZnS have the advantages of simplicity in synthesis, stability, and scalability. Despite decades of research, challenges such as charge separation, spectrum usage, low hydrogen generation efficiency, photocatalyst stability and scalability persist. This review discusses what has been achieved so far in the domain of photocatalytic hydrogen evolution and presents a critical analysis of challenges to be addressed in developing a robust and practical photocatalytic hydrogen generation system based on efficiency of photocatalysts and their stability and the extreme importance of efficient reactor designs. [Display omitted] • Challenges associated with photocatalytic hydrogen generation systems. • Photocatalysts, cocatalysts and their stability challenges in hydrogen evolution. • Potential of semiconductor nanostructures, plasmonic nanoparticles and QDs. • Importance of reactor designs in enhancing photocatalytic hydrogen evolution. [ABSTRACT FROM AUTHOR]

Organic conjugated polymers have received extensive attention due to their unique electronic properties. However, there have been relatively few reports on the dark photocatalytic reactions utilizing organic conjugated polymers. Herein, we report the successful synthesis of an organic conjugated polymer based on poly (heptazine imide) nanocrystals (CNNCs) for H2O2 evolution and biomedical applications using a simple salt molten method and sonication–centrifugation process. The results show that these colloid CNNCs have the characteristics of photogenerated electrons accumulation and realize dark photocatalysis with high reducibility under visible light irradiation. Notably, these accumulating photogenerated electrons can reduce O2 in darkness to produce H2O2. In addition, cytotoxicity tests were conducted and it was found that H2O2 produced under dark conditions could oxidize L-arginine (L-Arg) to NO, which effectively killed tumors in the dark. This work provides an important strategy to construct organic conjugated semiconductor nanocrystals and applying them to future energy and biomedical fields. [ABSTRACT FROM AUTHOR]

Temperature-responsive drug delivery systems offer the chance to better deliver anti-tumor drugs to tumor cells in a more controllable condition. In this work, a novel temperature-responsive nanocarrier was synthesized by grafting allyl alcohol and N-isopropyl acrylamide onto a nanodiamond surface and conjugated with polyester dendrimer for the controlled delivery of paclitaxel and photo-thermal therapy under near-infrared light irradiation. The morphology, chemical structure, and properties of this polymer were characterized through systematic characterization analyses. The data obtained from the non-linear isotherm model indicated that the sorption procedure followed Langmuir isotherm. Adsorption kinetic data shown that the pseudo-second-order model fitted well with the experimental results. The in-vitro drug release shown that about 92.10% of paclitaxel release was found to be occurred at the simulated physiological fluid within 48 h (pH 7.4; T = 45 °C), whereas about 64.38% of paclitaxel release occurred at the temperature of 37 °C (pH 7.4). Also, the released drug under near-infrared light irradiation reached up to 97.34% over 15 min, achieving the on-demand paclitaxel release. The release of the drug from the nanocarrier followed the mechanism of non-Fickian diffusion and best fitted to the Korsmeyer–Peppas model. The nanocarrier indicated dose dependent cytotoxicity towards MCF-7 cancer cells. [ABSTRACT FROM AUTHOR]

π‐Conjugated polyfluorenes (PPs) comprising 2,3‐diaminobenzene‐1,4‐diyl (unit A) and 9,9‐dihexylfluorene‐2,7‐diyl (polymer‐1) or 9,9‐bis(6‐N,N,N,‐trimethylammoniumhexyl)fluorene‐2,7‐diyl (unit B) (polymer‐2) units were synthesized using Suzuki‐Miyaura coupling polycondensation. To compare the chemical properties and functionality of polymer‐2, a water‐soluble PP comprising benzene‐1,4‐diyl and unit B (polymer‐3) was synthesized. Polymer‐1 exhibited solvatochromism: the photoluminescence (PL) peak of the polymer in solutions shifted to a longer wavelength with an increase in the dielectric constants of solvents. Polymer‐1 formed charge transfer (CT) complexes with organic electron acceptors. The CT complexation behavior was systematically elucidated by the PL measurements using Stern–Volmer and Benesi–Hildebrand methods. Water‐soluble polymer‐2 could be used as a sensor for the chain length of telomere DNA by monitoring the changes in its PL intensity upon the addition of the analyte. The DNA sensing performance of polymer‐2 surpassed that of polymer‐3, attributed to the presence of unit A in polymer‐2. This unit brought polymer‐2 closer to DNA through hydrogen bonding between the amino group of polymer‐2 and nucleic acids in DNA. This interaction facilitated the occurrence of CT from the polymer backbone to DNA. [ABSTRACT FROM AUTHOR]

Organic electrochemical transistors (OECTs) possess low operating voltage and excellent amplification capability and show promising applications in biosensors and flexible electronics. However, the active layers of OECTs are usually dense films, which show limited ion penetration/transport, resulting in limited performances of OECTs. Here, unprecedented high‐performance flexible multifunctional OECTs based on nanoporous (mainly 2–60 nm), high‐specific‐surface‐area (255–281 m2 g−1), and flexible conjugated polymer aerogel films are developed. The nanoporous structures effectively facilitate ion penetration/transport, leading to significantly enhanced transconductance (48.5–53.5 mS) and on/off ratio (6.4 × 104) of the OECTs compared with those of dense devices. The resulting OECT‐based glucose sensors exhibit an ultralow detection limit of 1 pm, approximately two to three orders of magnitude lower than those of the previously reported OECT glucose sensors, and an ultrabroad detection range of 1 pm–5 m. They can detect trace amounts of glucose in sweat, serum, saliva, and urine in real time. Moreover, the OECTs can be used for high‐performance flexible artificial synapses and electrocardiogram monitoring. This work provides a powerful strategy toward highly sensitive biosensors, artificial synapses, and electrophysiological signal monitoring. [ABSTRACT FROM AUTHOR]

The development of conjugated polymer–based water‐soluble nanoparticles for near‐infrared‐II (NIR‐II) fluorescence (FL; 1000–1700 nm)‐guided photothermal therapy holds promise in advancing cancer treatment. However, excessive nonradiative decay leads to almost complete quenching of conjugated polymers’ fluorescence. Therefore, a critical challenge is to suppress nonradiative decay while maintaining high‐quality fluorescence imaging and excellent photothermal conversion efficiency. In this study, a series of NIR‐II‐conjugated polymers with aggregation‐induced emission (AIE) effects are designed and synthesized using the Stille coupling reaction. The dual enhancement strategy of modulating the AIE units and introducing non‐conjugated backbone into the polymer backbone resulted in BCT1 with a high αAIE value of 3.27. BCT1 nanoparticles exhibit excellent NIR‐II fluorescence, a high photothermal conversion efficiency of 70.51%, and a tenfold enhancement in fluorescence compared with BT1. Both in vitro and in vivo experiments validated their good biocompatibility and outstanding performance in NIR‐II fluorescence imaging for accurately determining the location of tumors. This study provides a novel strategy and method for designing and developing multifunctional conjugated polymers for NIR‐II fluorescence imaging–guided photothermal therapy. [ABSTRACT FROM AUTHOR]

Polythiophenes are the most appealing donor materials in organic solar cells (OSCs) due to their simple chemical structures. However, the top‐performance polythiophenes are typically synthesized via Stille polycondensation, which is problematic due to significant toxicity and poor atom economy. By contrast, direct arylation polycondensation (DArP) is an eco‐friendly, and atom‐efficient alternative for synthesizing conjugated polymers, while the best efficiency for DArP‐derived polythiophenes is below 12%. This study reports a series of polythiophene‐based donors synthesized via DArP. Among these, PT4F‐Th reaches a power conversion efficiency (PCE) of 16.4%, which not only matches the current record for polythiophene‐based donor materials, but also marks the highest PCE achieved by DArP‐derived donors to date. The superior performance of PT4F‐Th is largely attributed to its optimal temperature‐dependent aggregation behavior and moderate miscibility with acceptors, along with the highest crystallinity among the candidates, resulting in the most favorable blend film morphology. This study underscores the significant potential of DArP‐derived polythiophenes in developing high‐performance and eco‐friendly OSCs. [ABSTRACT FROM AUTHOR]

Dibenzothiophene-S,S-dioxide (BTDO) is one of the cutting-edge electron-acceptor monomers for designing conjugated polymer based organic materials toward photocatalytic H 2 production from water. Normally, structure design of BTDO containing donor-acceptor (D-A) polymer photocatalyst mainly focuses on screening electron-donor motifs, the importance of modification on BTDO molecular toward improving charge carrier separation and photocatalytic performance is always ignored. Herein, a novel thienyl-fused BTDO building block (BTDO-DT) is prepared and utilized to synthesize B-BTDO-DT polymer photocatalyst by Sonogashira-Hagihara cross-coupling polycondensation using 1,4-Diethynylbenzene (B) and BTDO-DT as monomers. Experimental and density functional theory (DFT) calculation results demonstrate that modification of BTDO by thiophene not only enlarges light absorption region and promotes photogenerated e−/h+ separation, but also decreases H atom adsorption free energy (ΔG H*) on oxygen atom in the O S O group. As a result, B-BTDO-DT exhibits an outstanding visible light induced photocatalytic H 2 production rate of 156.6 μmol h−1 using 30 mg catalyst without Pt cocatalyst, which is 4.5 times higher than that of B-BTDO. And the H 2 production rate of B-BTDO-DT is further improved to be 259.8 μmol h−1 with 2.0 wt% Pt as co-catalyst. The present work may open a new direction for the design of conjugated polymer based photocatalysts with high photocatalytic activities. A novel thienyl-fused Dibenzothiophene-S,S-dioxide (BTDO) building block (BTDO-DT) is prepared and utilized to synthesize B-BTDO-DT polymer photocatalyst, which exhibits wider visible light absorption region, quicker photogenerated e−/h+ separation and smaller H atom adsorption free energy (ΔG H*) when compared with B-BDTO polymer, resulting in 4.5 times improvement on photocatalytic H 2 production performance. [Display omitted] • Dibenzothiophene-S,S-dioxide is fused by thiophene to prepare B-BTDO-DT polymer. • B-BTDO-DT exhibits narrower band-gap and quicker e−/h+ separation than B-BTDO. • Photocatalytic H 2 production rate of B-BTDO-DT is 4.5 times higher than B-BTDO. [ABSTRACT FROM AUTHOR]

Vanillin is often used in food and medicine because of its unique flavor and pharmacological effects. However, excessive vanillin intake can harm human health; therefore, rapid and simple vanillin detection methods are required. In this study, porphyrin‐based conjugated microporous polymer‐grafted graphene (CMP‐rGO) was synthesized via the Sonogashira–Hagihara coupling reaction and assembled into an electrochemical sensor for vanillin detection. Due to the enhanced electrical conductivity and electrocatalytic characteristics of CMP‐rGO, the sensor demonstrated a low detection limit of 0.07 μM and a broad response range of 0.08–20 μM. Furthermore, this reusable sensor exhibited acceptable recoveries when evaluating vanillin in pharmaceuticals and human serum. This study offers technological assistance for the rapid detection of vanillin in pharmaceuticals and broadens the application of CMP‐rGO. [ABSTRACT FROM AUTHOR]

Conjugated polymers are emerging as competitive candidates for organic thermoelectrics (OTEs). However, to make the device truly pervasive, both p‐ and n‐type conjugated polymers are essential. Despite great efforts, no n‐type equivalents to the p‐type benchmark PEDOT:PSS exist to date mainly due to the low electrical conductivity (σ). Herein, a near‐amorphous n‐type conjugated polymer, namely pDFSe, is reported with high σ by achieving the synergy between charge transport and doping efficiency. The polymer pDFSe is synthesized based on an acceptor‐triad moiety of diketopyrrolopyrrole‐difluorobenzoselenadiazole‐diketopyrrolopyrrole (DFSe), which has the noncovalently‐fused‐ring structure to reinforce the backbone rigidity. Furthermore, an axisymmetric thiophene‐selenophene‐thiophene donor is introduced, which enables the formation of near‐amorphous microstructures. The above merits ensure good doping efficiency without scarifying efficient intrachain charge‐carrier transport. Thus, pDFSe‐based n‐type transistors exhibit high electron mobility up to 6.15 cm2 V−1 s−1, much higher than its reference polymer pDSe without the noncovalently‐fused‐ring structure (0.77 cm2 V−1 s−1). Further upon n‐doping, pDFSe demonstrates excellent σ of 62.6 S cm−1 and maximum power factor of 133.1 μW m−1 K−2, which are among the highest values reported for solution‐processed n‐type polymers. The results demonstrate the great potential of near‐amorphous n‐type conjugated polymers with noncovalently‐fused‐ring structure for the next‐generation OTEs. [ABSTRACT FROM AUTHOR]

The document is a contents list for the journal "Chemical Communications" published in 2024. It includes articles on various topics such as photocatalysis, Raman imaging, glycosylation, and catalysis. The journal is published by The Royal Society of Chemistry, a leading chemistry community. The document provides a list of articles and authors, allowing library patrons to quickly identify articles of interest for their research. [Extracted from the article]

Photodetectors are a key sensing component in enabling emerging technologies. For weak light detection, phototransistors with high responsivity are needed. Furthermore, the ability to fabricate phototransistors using solution processing techniques will enable new form factors, including flexible and large‐area devices. In this work, a novel approach for synthesizing a photosensitive organic/inorganic hybrid semiconducting thin film through solution processing is introduced. The approach involves hierarchical patterning of semiconducting carbon nanotubes (CNTs) with poly(3‐hexylthiophene‐2,5‐dyl) (P3HT) through solution‐phase heterogeneous crystallization. The fabricated hybrid phototransistors are qualified through electrical testing at varied illumination profiles within the visible light range. At a wavelength of 470 nm with an optical excitation power of 0.37 µW cm−2, the device exhibits photoresponsivity of 3.53 × 105 AW−1, surpassing other solution‐processed, non‐lead‐containing devices in the literature. The optical response extends from both photogating (low excitation power) and photon‐induced carrier generation (high excitation power). The detectivity of the device is ≈8.7 × 1010 Jones. The transient response includes a rise time of 100 ms and a fall time of 200 ms which is similar to the metrics of other low‐dimensional photodetectors. These findings highlight the prospects of the solution‐processed P3HT/semi‐CNT hybrid platform for advanced photodetection applications with flexible and large‐area form factors. [ABSTRACT FROM AUTHOR]

The document is a contents list for the journal "Green Chemistry," published by The Royal Society of Chemistry. It highlights the articles and papers featured in the current issue, covering a range of topics related to sustainable chemistry and green technologies. The articles include research on bio-based polymers, nitrogen fixation strategies, carbon aerogels for energy storage, and the use of ionic liquids in new energy and biotechnologies. The journal aims to provide cutting-edge research for a greener and more sustainable future. [Extracted from the article]

Recent progress in conjugated polymer photocatalysts has opened avenues for enhancing photocatalytic hydrogen production (PHP) activity through structural design. This study highlights the impact of the acceptor-to-donor feed ratio on PHP activity in copolymers, influencing their energy level structures. Five conjugated porous polymers (CPPs) were synthesized by adjusting the acceptor-to-donor molar ratio. Notably, at a 2:1 acceptor-to-donor ratio, the polymer demonstrated a high hydrogen evolution rate (HER) of 61.9 mmol g−1 h−1 under full arc irradiation without co-catalysts and an apparent quantum yield (AQY) of 7.77% at 475 nm. However, further increasing the proportion of the donor unit in the copolymers decreases their HER. Experiments and theoretical simulation characterized that the feed ratios effectively tune the polymer's molecular structure, hydrophilicity, band gap, and the generation and transport efficiency of photo-induced charge carriers, ultimately affecting the hydrogen production kinetics and efficiency. This research demonstrates that tuning the band structure and chemical compositions of CPPs through statistical copolymerization significantly impacts their PHP activity. [Display omitted] • Conjugated porous polymers (CPPs) with donor-acceptor type were prepared as photocatalysts. • PProDOT-didecyl was used as the donor unit to tune the energy levels of the CPPs. • BS-4 shows an impressive hydrogen evolution rate of 61.9 mmol g−1 h−1 under full arc free of co-catalyst. • The optimum donor-to-acceptor ratio is crucial for improved photocatalytic activity. [ABSTRACT FROM AUTHOR]

Discovering a competent charge transport layer promoting charge separation in photoelectrodes is a perpetual pursuit in photoelectrochemical (PEC) water splitting to achieve high solar‐to‐hydrogen (STH) conversion efficiency. Here, a conjugated polythiophene framework (CPF‐TTB) on Ta3N5 is elaborately electropolymerized, substantiating the hole transport behavior in their heterojunction. Tailored band structures of the CPF‐TTB/Ta3N5 reinforce the separation of photogenerated carriers, elevating a fill factor of the photoanode modified with a cocatalyst. The enhanced hole extraction enables the NiFeOx/CPF‐TTB/Ta3N5/TiN photoanode to generate a remarkable water oxidation photocurrent density of 9.12 mA cm−2 at 1.23 V versus the reversible hydrogen electrode. A tandem device combining the photoanode with a perovskite/Si solar cell implements an unbiased solar water splitting with a STH conversion efficiency of 6.26% under parallel illumination mode. This study provides novel strategies in interface engineering for metal nitride‐based photoelectrodes, suggesting a promise of the organic–inorganic hybrid photoelectrode for high‐efficiency PEC water splitting. [ABSTRACT FROM AUTHOR]

A conjugated polymer, P4TTD-DPP, based on tetra-fused isoindigo-alt-diketopyrrolopyrrole, has been synthesized as a photothermal therapeutic nanotransducer within the near-infrared-II (NIR-II) window. P4TTD-DPP exhibits a notable mass extinction coefficient of 62.8 L g−1 cm−1 at 1064 nm. Additionally, P4TTD-DPP nanoparticles demonstrate remarkable photothermal conversion efficiency of 91.5% at 1064 nm and exhibit excellent anticancer efficacy under photothermal conditions. [ABSTRACT FROM AUTHOR]

Conjugated polymers with integrating properties of delayed fluorescence and photovoltaic responses simultaneously are scarcely reported due to the generally contradictory requirements for molecular structures to achieve the two properties. Herein, an O‐B(F)←N functionalized fused unit (M) with multiple resonance features, small energy gap between lowest singlet excited state (S1) and triplet excited state (T1) (ΔEST = 0.23 eV), and delayed fluorescence (τD = 0.75 µs), is designed. Selecting three benzodithiophene (BDT) derivatives as co‐units to copolymerize with M, leading to a series of O‐B(F)←N embedded polymers also maintaining delayed fluorescence (τD = 0.4–0.5 µs). Moreover, p‐type semiconductor characteristics are tested for these polymers with hole mobilities in the range of 10−6–10−5 cm2/Vs. Devices with obviously photovoltaic responses are prepared using these polymers as donors and Y6 as the acceptor, affording a preliminary efficiency of 5.05%. This work successfully demonstrates an effective strategy to design conjugated polymers with integrating properties of delayed fluorescence and photovoltaic performance simultaneously by introducing O‐B(F)←N functional groups to polymer backbones. [ABSTRACT FROM AUTHOR]

Stretchable conjugated polymers with conjugation break spacers (CBSs) synthesized via random terpolymerization have gained considerable attention because of their efficacy in modulating mobility and stretchability. This study incorporates a series of dianhydrohexitol diastereomers of isosorbide (ISB) and isomannide (IMN) units into the diketopyrrolopyrrole‐based backbone as CBSs. It is found that the distorted CBS (IMN) improves the mobility–stretchability properties of the polymer with a highly coplanar backbone, whereas the extended CBS (ISB) enhances those of the polymer with a noncoplanar backbone. Additionally, the different configurations of ISB and IMN sufficiently affect the solid‐state packing, aggregation capabilities, crystallographic parameters, and mobility–stretchability properties of the polymer. The IMN‐based polymers exhibit the highest mobility of 1.69 cm2 V−1 s−1 and crystallinity retentions of (85.7, 78.6)% under 20% and 60% strains, outperforming their ISB‐based or unmodified counterparts. The improvement is correlated with a robust aggregation capability. Furthermore, the CBS content affects aggregation behavior, notably affecting mobility. This result indicates that incorporating CBSs into the polymer can enhance backbone flexibility via movement and rotation of the CBS without affecting the crystalline regions. [ABSTRACT FROM AUTHOR]

This article from the Chinese Journal of Chemistry introduces a new member of the editorial board, Shaowei Shi, who is a professor at Beijing University of Chemical Technology. The article provides information about Shi's education, experience, and awards. It also highlights Shi's favorite area of chemistry, which is reconfigurable structured liquids. The article explains how these liquids can be structured through the interfacial assembly and jamming of nanoparticles, allowing for responsiveness and malleability. The concept of nanoparticle surfactants is also discussed, which enables the introduction of chemical functionality and takes advantage of the inherent functionality of nanoparticles. The article emphasizes the generality and potential applications of this concept. [Extracted from the article]

There is a clearly demonstrated relationship between the microstructure, processing and resulting optoelectronic properties of conjugated polymers. Here, we exploited this relationship by exposing polyfluorene thin films to various solvent vapors via confined-solvent vapor annealing to optimize their microstructure, with the final goal being to enhance their emission properties. Our results have demonstrated enlargements in photoluminescence intensity of up to 270%, 258% and 240% when thin films of polyfluorenes of average molecular weights of 105,491 g/mol, 63,114 g/mol and 14,000 g/mol, respectively, experienced increases in their β-phase fractions upon processing. [ABSTRACT FROM AUTHOR]

Conjugated polymers consist of complex backbone structures and side‐chain moieties to meet various optoelectronic and processing requirements. Recent work on conjugated polymers has been devoted to studying the mechanical properties and developing new conjugated polymers with low modulus and high‐crack onset strain, while the thin film mechanical stability under long‐term external tensile strain is less investigated. Here we performed direct mechanical stress relaxation tests for both free‐standing and thin film floated on water surface on both high‐Tg and low‐Tg conjugated polymers, as well as a reference nonconjugated sample, polystyrene. We measured thin films with a range of film thickness from 38 to 179 nm to study the temperature and thickness effect on thin film relaxation, where an apparent enthalpy–entropy compensation effect for glassy polymer PS and PM6 thin films was observed. We also compared relaxation times across three different conjugated polymers and showed that both crystalline morphology and higher modulus reduce the relaxation rate besides higher glass transition temperature. Our work provides insights into the mechanical creep behavior of conjugated polymers, which will have an impact on the future design of stable functional organic electronics. [ABSTRACT FROM AUTHOR]

The doping levels of conjugated polymers significantly influence their conductivity, energetics, and optical properties. Recently, a highly conductive n‐doped polymer called poly (3,7‐dihydrobenzo[1,2‐b:4,5‐b′]difuran‐2,6‐dione) (poly(benzodifurandione), n‐PBDF) is discovered, opening new possibilities for n‐type conducting polymers in printed electronics and other fields. Controlling the doping level of n‐PBDF is of great interest due to its wide range of potential applications. Here controlled dedoping and redoping of n‐PBDF is reported and a mechanistic understating of such a process is provided. Dedoping occurs through electron transfer and proton capture, wherein the ionic dopants, tris(4‐bromophenyl)ammoniumyl hexachloroantimonate (Magic Blue), exhibit efficient proton capture ability and stronger interaction with n‐PBDF, resulting in high dedoping efficiency. Moreover, chemically dedoped PBDF can be redoped using various proton‐coupled electron transfer agents. By manipulating the doping levels of n‐PBDF thin films, ranging from highly doped to dedoped states, the system demonstrates controllable conductivity in five orders of magnitude, adjustable optical properties, and energetics. As a result, these characteristics demonstrate the potential applications of n‐PBDF in organic electrochemical transistors and thermoelectrics. [ABSTRACT FROM AUTHOR]

Preparing well-ordered nanotubes on material surface is fundamental for a huge number of applications. Natural surfaces and theoretical approaches show that porous structures such as nanotubes are key parameters for both surface hydrophobicity and water adhesion. Here, a very easy soft-template electropolymerization approach is used to form nanotubes. A solvent of low water-solubility (dichloromethane) is mixed to water in the presence of a surfactant electrolyte for stabilizing the micelles formed in solution. The monomers investigated are thiophene and carbazole derivatives, and are all fully conjugated for favoring the deposition versus polymerization. Indeed, in all the electrodeposited films, the monomer is mostly present as confirmed by cyclic voltammetry. The key parameters in the resulting nanotubes is the monomer structure because a preferential growth is necessary and this one is induced here especially by π-stacking interactions in the direction perpendicular to monomer. The surfaces composed of nanoparticles or nanotubes are the most hydrophobic with an apparent contact angle up to 130.9° accompanied with strong water adhesion, as reported on gecko foot or rose petal. [ABSTRACT FROM AUTHOR]

Triazine-based conjugated polymers with high electron transfer efficiency obtained the enhanced photocatalytic activities by D-A polarization for degradation of BPA and benzene pollutants. [Display omitted] • Triazine-based D-A conjugated polymers were fabricated by simple Schiff-base reaction. • The separation and transfer of photogenerated carriers is improved by D-A configuration regulation. • The π-conjugated skeleton facilitates the adsorption and activation of aromatic pollutant molecules. • Tr-BTh exhibited complete photocatalytic degradation of 50 ppm BPA in 40 min. Photocatalysis is a green and environmentally friendly method for degrading dangerous and nonbiodegradable pollutants. In this study, a sequence of metal-free triazine-based electronic donor–acceptor (D-A) conjugated polymers Tr-X (X = Th, BT, BTh) were prepared by D-A configuration regulation between triazine (Tr) and monomers containing N and S, such as thiophene (Th), bithiophene (BTh) and benzothiadiazole (BT) units, for the photocatalytic degradation of bisphenol A (BPA) and benzene contaminants in water under visible light. Among these, Tr-BTh exhibited complete photocatalytic degradation owing to its excellent D-A configuration. Moreover, the N and S atoms, which are rich in triazine and thiophene units, serve as highly dispersed reactive sites. The separation and transfer of photogenerated carriers can be further improved by expanding the light-absorption range of polymers. In addition, the polymers showed good adsorption for BPA and other aromatic organic pollutants through π-π interaction and surface hydrogen bonding, which provides a facile strategy for efficient polymer-based photocatalysts for water purification. [ABSTRACT FROM AUTHOR]

Water‐dispersible fluorescent nano‐/microspheres have been widely used as fluorescent probes in many fields. In this paper, aldehyde‐functionalized fluorescent micelles are synthesized by self‐assembly of end‐modified hyperbranched poly(m‐phenyleneethynylene‐alter‐p‐phenyleneethynylene)(hb‐PMPE). First, hb‐PMPE with ‐Br end‐groups(hb‐PMPE‐Br) is obtained by the polymerization of AB2 monomer PhBr2–C≡C–Ph–C≡CH, then the reaction of hb‐PMPE‐Br with 4‐ethynylbenzaldehyde (EBA) gives end aldehyde‐functionalized hyperbranched polymer hb‐PMPE‐CHO. Hence, hb‐PMPE‐CHO is reacted with aminooxy methoxypolyethylene glycol‐2000 (NH2O‐MPEG2000) to link poly(ethylene glycol) (PEG) chains to the ends of hb‐PMPE‐CHO with partial residual aldehyde end‐groups, resulting in aldehyde‐functionalized amphiphilic polymer hb‐PMPE‐PEG. Fluorescent micelles with aldehyde‐containing fluorescent hb‐PMPE core and PEG shell are obtained by self‐assembling hb‐PMPE‐PEG in water. The micelle diameter is determined by the PEG content in hb‐PMPE‐PEG, which can be controlled by the reaction weight ratio of NH2O‐MPEG2000/hb‐PMPE‐CHO. When the ratio of NH2O‐MPEG2000/hb‐PMPE‐CHO > 0.75/1, micelles with a diameter < 50 nm are obtained. The water dispersion of hb‐PMPE‐PEG‐1/2 micelles (28.9 nm) emits bright green fluorescence with λmax ≈ 490 nm under UV irradiation, and the emission intensity increases with increasing concentration. [ABSTRACT FROM AUTHOR]

For advancing next‐generation optoelectronics, a versatile strategy for fabricating π‐conjugated polymer (π‐CP)/chiral‐small molecule (SM) hybrid films through co‐crystallization‐mediated chirality transfer is reported. The transfer of optical chirality from 1,1′‐binaphthyl–2,2′‐diamine (BN), a representative chiral inducer SM, to thin films of various achiral π‐CPs, including non‐fluorene π‐CPs, is achieved by simply blending the π‐CPs with BN using aromatic organic solvents. The resulting π‐CP/chiral‐SM hybrid films exhibit chiroptical responses at the main electronic absorption bands of various π‐CPs. Studies of the morphology, crystalline structure, and phase‐separation structure of a representative hybrid system of poly(3‐hexylthiophene) (P3HT) and BN reveal that these hybrid films exhibit a characteristic lamellar structure where the π‐CPs co‐crystallize with chiral BN molecules, facilitated by aromatic solvent‐assisted intermolecular π–π interactions. In‐depth photophysical analysis suggests that BN molecules co‐crystallized in the P3HT lamellar structure induce asymmetrically misaligned transition dipoles along the P3HT conjugated backbone, transferring optical chirality from BN to P3HT under circularly polarized light illumination. As a proof‐of‐concept, chiroptical photodiodes based on π‐CP/chiral‐SM hybrid films and printed micropatterns, exhibiting a distinguishable photocurrent response depending on the direction of circularly polarized light are successfully demonstrated. [ABSTRACT FROM AUTHOR]

Crystalline and soluble 1D linear conjugated polymers (LCPs) have garnered considerable interest as cost‐effective and efficient metal‐free electrocatalysts for the oxygen reduction reaction (ORR) due to their high exposure of catalytic sites and ease of processing. However, difficulties remain in achieving excellent ORR performance for 1D LCPs by conventional molecular design. Herein, it is demonstrated the utilization of quinoidal units as a promising strategy to develop 1D LCPs for ORR. The incorporation of quinoidal unit not only results in polymers with strong inter‐ and intra‐molecular interactions and low‐lying LUMO (lowest unoccupied molecular orbital) energy levels, but also provides polymers with good crystallinity and commendable charge carrier mobilities. The electronic properties of these polymers are fine‐tuned through the introduction of additional heteroatoms and/or substituents in the monomers and comonomers to understand and optimize their ORR catalytic activity. Evaluation of their catalytic performances reveals a remarkable half‐wave potential and limiting current density of up to 0.74 V (vs reversible hydrogen electrod) and 7.50 mA cm−2, respectively. Notably, these performances are achieved without the addition of carbon nanomaterials as support. This study offers a new insight into the design of highly efficient metal‐free organic electrocatalysts. [ABSTRACT FROM AUTHOR]

Direct printing of conjugated polymer thin‐film transistors enables the fabrication of deformable devices with low cost, high throughput, and large area. However, a relatively poor device performance of printed devices remains a major obstacle to their application in high‐end display backplanes and integrated circuits. In this study, high‐performance and highly stackable printed organic transistors is developed, arrays, and circuits using a near‐amorphous polymer, indacenodithiophene‐co‐benzothiadiazole (IDT‐BT). The printed devices exhibited high saturation mobility (>1 cm2 V−1 s−1), high on/off ratio (>107), and low subthreshold slope (245 mV dec−1). In addition, 16 × 16 printed IDT‐BT arrays achieved 100% fabrication yield, with excellent device‐to‐device uniformity and low variations of mobility (9.55%) and threshold voltage (4.51%), and good operational and environmental stability (>365 days). Furthermore, five stacked 3D transistors are demonstrated with an excellent 3D uniformity without compromising device performance due to a low required thermal budget for processing amorphous IDT‐BT. Finally, a new concept of 3D universal logic gate with high voltage gain (33.91 V/V) and record density (100 printed transistors per cm2) is proposed and fabricated, which is relevant for the commercialization of low‐cost printed display backplanes and high‐density integrated circuits based on highly processable polymeric semiconductors. [ABSTRACT FROM AUTHOR]

This study reports intrinsic multimodal memristivity of a nonconjugated radical polymer with ambient stability. Organic memristive devices represent powerful candidates for biorealistic data storage and processing. However, there exists a substantial knowledge gap in realizing the synthetic biorealistic systems capable of effectively emulating the cooperative and multimodal activation processes in biological systems. In addition, conventional organic memristive materials are centered on conjugated small and macromolecules, making them synthetically challenging or difficult to process. In this work, we first describe the intrinsic resistive switching of the radical polymer that resulted in an exceptional state retention of >105 s and on/off ratio of >106. Next, we demonstrate its bimodal cooperative switching, in response to the proton accumulation as a biological input. Last, we expand our system toward an advanced in-sensor computing system. Our research demonstrates a nonconjugated radical polymer with intrinsic memristivity, which is directly applicable to future electronics including data storage, neuromorphics, and in-sensor computing. [ABSTRACT FROM AUTHOR]

As a new class of organic photocatalysts, polymer dots show a potential application in photocatalytic hydrogen peroxide production coupled with chemical oxidation such as methanol oxidation. However, the poor methanol oxidation ability by polymer dots still inhibits the overall photocatalytic reaction occurring in the neutral condition. In this work, an organic molecular catalyst 4-amino-2,2,6,6-tetramethylpiperidine-1-oxyl radical is covalently linked to a fluorene unit in a polymer skeleton, eventually enabling photocatalytic hydrogen peroxide production coupled with methanol oxidation in the neutral condition. By conducting various spectroscopic measurements, charge transfer between components in this molecular catalyst-immobilized polymer dots system is studied and found to be very efficient for hydrogen peroxide production coupled with alcohol oxidation. This work proves a strategy for designing polymer dots photocatalysts with molecular catalysts, facilitating their future development and potential applications in other fields such as water splitting, CO2 reduction, photoredox catalysis and photodynamic therapy. A strategy of covalently grafting molecular catalysts to polymer backbones in polymer dots photocatalysts is proposed in this work, realizing a groundbreaking photocatalytic oxidation of various alcohols in neutral conditions. [ABSTRACT FROM AUTHOR]

As the demand for multifunctional optoelectronic devices rises, the integration of electrochromic and energy storage functionalities represents a cutting‐edge pursuit in the electrochromic devices domain. The realm of conductive polymer‐based electrochromic energy storage devices (EESDs) stands as a vibrant area marked by ongoing research and development. Despite a plethora of individual research articles exploring various facets within this domain, there exists a conspicuous dearth of comprehensive reviews systematically scrutinizing the advancements, challenges, and potentials intrinsic to these systems. To fill this void, this review systematically outlines the latest progressions in EESDs centered on conductive conjugated polymers (CPs). The review commences with a thorough exploration of the foundational principles underpinning EESDs, encompassing their operational mechanisms, device configurations, and representative key performance indicators. Furthermore, the review categorizes diverse conductive polymers, shedding light on the latest advancements in EESD research utilizing these specific CP variants. This in‐depth analysis centers on their collaborative role in shaping electrochromic energy storage devices. Overall, this review is poised to captivate the interest of researchers toward state‐of‐the‐art CP‐based EESDs, establishing these pioneering technologies as pivotal contenders in defining the forthcoming landscape of wearable electronics, portable devices, and advanced energy storage systems. [ABSTRACT FROM AUTHOR]

Carbon‐based nanomaterials have catalyzed breakthroughs across various scientific and engineering disciplines. The key to unlocking a new generation of tailor‐made nanomaterials based on single‐walled carbon nanotubes (SWCNTs) lies in the precise sorting of raw material into individual chiralities, each possessing unique properties. This can be achieved using conjugated polymer extraction (CPE), but to a very limited extent since the process generates only a few chirality‐enriched suspensions. Therefore, it is imperative to comprehend the mechanism of the wrapping of SWCNTs by polymers to unleash CPE's full potential. However, the lack of a diverse palette of chirality‐selective polymers with varying macromolecular parameters has hindered a comprehensive understanding of how the nature of the polymer affects the performance and selectivity of SWCNT isolation. To address this gap, multiple batches of such polymers are synthesized to elucidate the impact of molecular weight and dispersity on the purity and concentrations of the generated SWCNT suspensions. The obtained results explain the inconsistent outcomes reported in the literature, greatly improving the application potential of this promising SWCNT sorting approach. Concomitantly, the discovered significant influence of the macromolecular characteristics of conjugated polymers on the SWCNT isolation efficacy sheds considerable insight into the unresolved mechanism of this sorting technique. [ABSTRACT FROM AUTHOR]

The development of neuromorphic optoelectronic systems opens up the possibility of the next generation of artificial vision. In this work, the novel broadband (from 365 to 940 nm) and multilevel storage optoelectronic synaptic thin‐film transistor (TFT) arrays are reported using the photosensitive conjugated polymer (poly[(9,9‐dioctylfluorenyl‐2,7‐diyl)‐co‐(bithiophene)], F8T2) sorted semiconducting single‐walled carbon nanotubes (sc‐SWCNTs) as channel materials. The broadband synaptic responses are inherited to absorption from both photosensitive F8T2 and sorted sc‐SWCNTs, and the excellent optoelectronic synaptic behaviors with 200 linearly increasing conductance states and long retention time > 103 s are attributed to the superior charge trapping at the AlOx dielectric layer grown by atomic layer deposition. Furthermore, the synaptic TFTs can achieve IOn/IOff ratios up to 106 and optoelectronic synaptic plasticity with the low power consumption (59 aJ per single pulse), which can simulate not only basic biological synaptic functions but also optical write and electrical erase, multilevel storage, and image recognition. Further, a novel Spiking Neural Network algorithm based on hardware characteristics is designed for the recognition task of Caltech 101 dataset and multiple features of the images are successfully extracted with higher accuracy (97.92%) of the recognition task from the multi‐frequency curves of the optoelectronic synaptic devices. [ABSTRACT FROM AUTHOR]

Engineering a catalytic membrane capable of efficiently removing emerging organic microcontaminants under ultrahigh flux conditions is of significance for water purification. Herein, drawing inspiration from the functional attributes of lymphatic vessels involved in immunosurveillance and fluid transport with minimal energy consumption, a novel hierarchical porous catalytic membrane is engineered. This membrane, based on an innovative nitrogen‐rich conjugated microporous polymer (polytripheneamine, PTPA), is synthesized using an electrospinning coupled in situ polymerization approach. The resulting bioinspired membrane with hierarchical channels comprises a thin layer (≈1.7 µm) of crosslinked PTPA nanoparticles covering the interconnected electrospun nanofibers. This unique design creates an intrinsic microporous angstrom‐confined system capable of activating peroxymonosulfate (PMS) to generate 98.7% singlet oxygen (1O2), enabling durable and highly efficient degradation of microcontaminants. Additionally, the presence of a thin layer of mesoporous structure between PTPA nanoparticles and macroporous channels within the interwoven nanofibers enhances mass transfer efficiency and facilitates high flux rates. Notably, the prepared hierarchical porous organic catalytic membrane demonstrates enduring high‐efficiency degradation performance with a superior permeance (>95% and >2500 L m−2 h−1 bar−1) sustained over 100 h. This work introduces an innovative pathway for the design of high‐performance catalytic membranes for the removal of emerging organic microcontaminants. [ABSTRACT FROM AUTHOR]

The document is the contents list for an issue of the journal Chemical Communications. It includes the titles and authors of various articles and features that will be included in the issue. Some of the topics covered include silk-based intelligent fibers and textiles, advances in molecular engineering of perovskite heterostructures, and metal-organic framework based self-powered devices for human body energy harvesting. The journal is published by The Royal Society of Chemistry, a leading chemistry community. [Extracted from the article]

A BODIPY-containing conjugated microporous polymer (CMP, LBFD-1) was modified with calixarene to develop a hydrophilic CMP (LBFD-2) with broader absorption extending to the near-infrared-II region. LBFD-2 exhibited an H2O2 production rate of 2.14 mmol g−1 h−1 in the air without any sacrificial agents. The removal efficiency (η) of LBFD-2 towards methylene blue and rhodamine B reached >99.5% within 20 and 40 min in light. LBFD-2 can withstand diverse environmental changes, showing excellent reusability and potential for practical applications in real-water systems. [ABSTRACT FROM AUTHOR]

Due to the mismatched aggregation behavior and limited compatibility between the donor and acceptor, it is a challenge for the active layer of organic solar cells (OSCs) to spontaneously realize well‐developed morphology in nonhalogenated solvents. In this contribution, an aggregation regulation strategy for acceptors with strong aggregation is developed via thiophene‐substituted alkyl chain engineering to fabricate high‐performance nonhalogenated solvent‐processed OSCs without an additive or post‐treatment. With the replacement of alkyl chains with steric conjugated thiophene‐substituted alkyl chains, the resulting acceptor (namely BTP‐2T, BTP‐T, and BTP‐T‐BO) shows reduced aggregation to match the polymer donor D18‐Cl using toluene as a processing solvent, enabling ordered molecular arrangement and uniform phase separation morphology. Especially, the combined modification of the asymmetric thiophene‐substituted inner chain and branched outer side chains for BTP‐T‐BO enables the formation of a superior nanoscale bi‐continuous interpenetrating network along with ordered and compact molecular packing in the D18‐Cl:BTP‐T‐BO blend. As a result, an excellent PCE of 18.05% is achieved in the D18‐Cl:BTP‐T‐BO‐based device using toluene as the processing solvent without any extra treatment, which is the highest value for nonhalogenated solvent‐processed OSCs without any extra treatment. [ABSTRACT FROM AUTHOR]

The polymorphic behavior of conjugated polymers enables tunable optoelectronic properties, but their transport mechanism remains elusive due to the inherent complexity and uncontrollability of polymorphic self‐assembly behaviors and electronic processes at various length scales, alongside the ambiguous relationship between solution and solid states. Herein, precise control of multi‐level supramolecular self‐assembly of a polymorphic conjugated polymer, N‐PDPP4T‐HD with two distinct semi‐crystalline aggregated phases (β1 and β2) via solvent engineering is demonstrated. β1 forms 1D worm‐like nanostructures in solution, whereas β2 generates 2D nanoscale lamellar configuration, confirmed by experimental observation and molecular dynamic simulation. Such solution‐state features are inherited in the solid state (1D nanofibers for β1 and 2D granular‐like structures for β2). X‐ray characterizations reveal larger crystalline domains on the nanometer scale, reduced π‐stacking distance on the Ångstrom scale, and diminished paracrystallinity disorder for solid‐state β2. Going beyond conventional DC transistor characterizations, contact‐free ultrafast terahertz spectroscopy to unveil AC short‐range, intrinsic transport properties is employed. Longer charge carrier scattering time and thus intrinsic mobility of β2 result in threefold higher short‐range photoconductivity than β1. This work establishes the “solution structure – solid structure – local transport” relation in polymorphic conjugated polymers and provides new opportunities for high‐performance plastic electronic devices. [ABSTRACT FROM AUTHOR]

Conjugated homopolymers based on six-member rings, e.g., polyfluorene, always exhibit blue emission and conjugated homopolymers based on five-member rings, e.g., polythiophene, can give red emission with low efficiency. In this work, we report a series of new conjugated homopolymers based on six-member rings with high-efficiency deep-red emission. The repeating units of the red light emitting homopolymers are double B←N bridged bipyridine (BNBP) with the boron atoms functionalized with diphenyl, borafluorene, and 2,7-di-tert-butyl-borafluorene groups, respectively. The relationship between the chemical structures and the opto-electronic properties of the monomers and the homopolymers has been systematically studied. The three polymers emit pure red light (λmax=656 nm) or deep red light (λmax=693 nm) with fluorescence quantum efficiency in solution higher than 60%. The polymers can be used as the emitters in solution-processed organic light-emitting diodes with red emission and decent device performance. This work indicates a new strategy to design highly efficient light emitting conjugated polymers. [ABSTRACT FROM AUTHOR]