Electrolyte additive engineering greatly enhances the performance of aqueous zinc-ion batteries (AZIBs), yet most studies focus on functional groups while overlooking the molecular backbone effect. Herein, four sulfonate additives with gradient molecular skeletons, namely sodium benzenesulfonate (SBS), p-toluenesulfonate (STS), sodium dodecylbenzenesulfonate (SDBS) and sodium dodecylsulfonate (SDSN), are systematically investigated as functional electrolyte additives for AZIBs. Aromatic rings in SBS, STS and SDBS molecules introduce delocalized non-local π-electrons to trigger anisotropic polarization and local charge aggregation, which cause uneven Zn2+ flux distribution and localized zinc deposition behavior. Conversely, SDSN with an aliphatic skeleton displays superior chemisorption capability in comparison with aromatic sulfonate additives. Interfacial SDSN modulates the solvation shell of Zn2+ to establish a high-coordination yet weakly bound solvation configuration, which accelerates three-dimensional Zn2+ diffusion and homogenizes the interfacial electric field, thus achieving uniform and dense Zn deposition. Accordingly, the synergistic interplay between the aliphatic skeleton and functional groups in SDSN molecules contributes to the effective inhibition of parasitic side reactions, thereby significantly prolonging the lifespan and stability of Zn anodes. This work highlights the vital significance of molecular backbone engineering and offers an effective structural design principle for advanced electrolyte additives toward high-performance and long-lifespan AZIBs.

Organic materials with strong third-order nonlinear optical (NLO) responses are crucial for advancing laser protection technologies, such as optical limiters. However, achieving a high nonlinear absorption coefficient concurrently with an ultralow operational threshold remains a significant challenge. Herein, we report a combined experimental and theoretical study on the third-order NLO properties of a series of planar non-fused ring acceptors (NFRAs) featuring a unique A-D-A'-D-A architecture. Among them, the chlorinated derivative BDD2Cl exhibits superior performance, possessing a large nonlinear absorption coefficient (4.72 & times; 10-9 m/W) and an ultralow optical limiting threshold (0.44 J/cm2), outperforming its fluorinated analogue BDD2F and other counterparts. Femtosecond transient absorption and density functional theory calculations collaboratively unveil that this enhancement originates from its large dipole moment, second hyperpolarizability, and highly efficient excited-state absorption promoted by molecular planarity. This work not only identifies NFRAs as promising candidates for high-performance optical limiters but also establishes a structure-property paradigm, providing fundamental insights for the rational design of broadband organic NLO materials.

White organic light-emitting transistors (OLETs) are poised to be pivotal components in next generation smart displays. However, their development is hindered by the scarcity of ideal materials that concurrently exhibit high charge carrier mobility and efficient white-light emission. Herein, we present a novel molecular design strategy that achieves white electroluminescence by synergistically harnessing emissions from the monomer, excimer, and electromer within a single material. Guided by this approach, we designed and synthesized 2,6-bis(dibenzo[b,d]thiophen-3-yl)anthracene (DTA), which exhibits a photoluminescence quantum yield of 35% and a high saturation hole mobility of 5.8 cm2 V-1 s-1. Remarkably, in single-component OLET devices, DTA manifests an additional electromer emission. The combination of this red-shifted electromer band with the monomer and excimer emissions results in broad-spectrum white electroluminescence, with Commission Internationale de l'Eclairage coordinates of (0.3030, 0.3558). Moreover, the relative intensities of these three emissive species can be dynamically modulated by the gate voltage, enabling real-time tuning of the white color temperature and achieving a high color-rendering index. This work establishes a new design paradigm for high-mobility white-light emitters and represents a significant stride toward practical single-component white OLETs.

Abstract Circularly polarized light (CPL) photodetectors are of great interest for applications in polarization imaging, information encryption, and optical communication. Chiral organic small molecules have emerged as attractive active materials due to their structural tunability, well‐defined intrinsic chirality, and solution processability. However, in most chiral organic small molecule systems, molecular‐scale effects and optical selection rules lead to mismatch in magnitude and spatial orientation between the magnetic and electric transition dipole moments, resulting in low absorption dissymmetry factors (gabs) and poor compatibility between chiroptical response and charge transport. This review summarizes the recent progress in chiral organic small molecules for CPL detection from the perspective of group theory. By comparing the representative chiral point groups such as C1, Cn, and Dn, we elucidate how point group symmetry imposes constraints on the relative arrangement of transition dipole moments, thereby governing the molecular gabs. In particular, the D2 point group can enforce both electric and magnetic transition dipole alignment along the principal molecular axes, yielding an optimal orientation (0° or 180°) and thus enabling the high gabs. Recent advances in chiral organic small molecules D2 point group demonstrate their potential to simultaneously achieve strong chiroptical responses and efficient charge transport, offering a clear structural guideline for the rational design of high‐performance CPL photodetectors based on chiral organic small molecules.

The multicomponent strategy is widely recognized as an effective approach for enhancing the performance of organic solar cells (OSCs). While guest components can bring multiple benefits, the ability to precisely regulate molecular crystallization, ensuring inertness toward one host component while directing the assembly of the other, remains highly impactful and challenging. Herein, we propose a guest-mediated orthogonal crystallization strategy in which the guest component achieves dual functionality: it directs the crystallization of the acceptor without interfering with the donor, thereby preserving its optimal morphology. Based on this concept, we designed and synthesized a guest molecule, PPyBT, which incorporates benzodithiophene (BDT) units to ensure donor inertness and 4,5,9,10-pyrene diimide (PyDI) units to guide acceptor packing. PPyBT acts as a multifunctional regulator that not only templates the active layer morphology but also optimizes the energy level alignment. The resulting well-defined phase separation and molecular packing enable the corresponding PM6:L8-BO:PPyBT ternary device to achieve a power conversion efficiency of 19.15%, which is among the highest values reported to date, along with improved stability under both photo- and thermal-stress. This work establishes a feasible molecular framework for guest-induced crystallization control, offering a promising pathway toward high-performance OSCs.

Nitroxide radical-conjugated polymer additives (nr-PAs) have been employed as newly emerged additives to mitigate the non-radiative energy loss (Elossnon_ rad), thus to boost the performance and stability of the non-fullerene acceptors-based organic solar cells (NFAs-OSCs). Herein, the small molecular nitroxide radical compounds (SMTEMPO) of racemic 4-glycidyloxy-substituted 2,2,6,6-tetramethylpiperidine-1-oxyl (GTEMPO), the stereoisomers of (R)-GTEMPO and (S)-GTEMPO, are employed as the additives for NFAs-OSCs. Upon addition of 1.0 wt% (relative to the weight of polymer donor) of the SM-TEMPO radical additives, the power conversion efficiencies (PCEs) of the devices improved as follows: PM6:Y6: from 15.73% (pristine) to 16.46% (GTEMPO), 17.20% ((R)GTEMPO), and 16.91% ((S)-GTEMPO). D18-Cl:L8-BO: from 17.53% (pristine) to 18.66% (GTEMPO), 19.42% ((R)-GTEMPO), and 19.38% ((S)-GTEMPO). On the contrary, the addition of the unglycidylated 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) radical additive always results in a slight decrease in the PCEs of the PM6:Y6based NFAs-OSCs. Moreover, the reasons behind the performance enhancement, as well as the specific correlation between the improved performances of NFAs-OSCs and the difference in aggregation behaviours between the SM-TEMPO and TEMPO radical additives, are investigated and discussed through a set of physical investigations of representative PM6:Y6-based blends and devices. This work not only demonstrates that SMTEMPO radical additives, which tend to aggregate in the active layer, can serve as effective additives to improve the performance and stability of the NFAs-OSCs as their nr-PAs counterparts, but also points towards simpler avenues for the development of the nitroxide radical-based additives to achieve high-performance NFAsOSCs with enhanced stability.

Indium-based halide perovskites oftentimes exhibit limited photoluminescence quantum yield (PLQY) due to weak optical absorption, which restricts their utility in luminescent applications. However, self-trapped exciton (STE) modulation through crystal engineering offers a promising pathway to enhance emission efficiency. In this study, we report the low-temperature (20-85 degrees C) synthesis of centimeter-scale lead-free perovskite single crystals of CsIn1-xSbxCl4, which demonstrate intense broadband STE emission at room temperature and achieve an unprecedented PLQY of 100%, the highest reported value for indium-based halides to date. Femtosecond spectroscopy elucidated the physical origin by mapping the complete dynamics: the sub-picosecond (sub-ps) formation of the singlet (STE)-S-1, its transition to the triplet (STE)-S-3 within tens to hundreds of ps, and the subsequent mu s-scale radiative recombination. This work thus offers critical insights into STE-driven design strategies for next-generation optoelectronic devices of single component white-light emission.

Waveplate-free detection of near-infrared (NIR) circularly polarized light (CPL) has been limited by the absence of materials that simultaneously exhibit strong NIR circular dichroism and efficient charge transport. Here, we present a family of axially chiral conjugated polymers, S- and R-pDPP4TBN-X, designed by grafting S/R-6,6'-dimethoxy-1,1'-binaphthyl (S/R-MeBN) onto a diketopyrrolopyrrole (DPP)-bithiophene backbone. By tuning the MeBN: DPP ratio, the polymers exhibit extended absorption up to ∼1000 nm, enhanced circular dichroism in the 500-870 nm region, and optimized thin-film morphology for charge mobility. Organic phototransistors based on S/R-pDPP4TBN-10 achieve hole mobilities up to 0.13 cm2 V-1 s-1, responsivities as high as 12.52 A W-1, detectivities on the order of 1011 Jones, and dissymmetry factors (gIph) of 0.30 and -0.34 under 808 nm CPL, enabling unambiguous discrimination of left- and right-handed light. Beyond static sensing, these devices emulate synaptic plasticity under CPL stimulation and, when coupled with an artificial neural network, deliver classification accuracies exceeding 95%. This work establishes a modular design paradigm for compact, NIR-active CPL sensors that integrate high charge transport, pronounced chiroptical response, and neuromorphic function, paving the way for photonic encryption, wearable optoelectronics, and bioinspired computing platforms.

ABSTRACT Chiral hybrid organic–inorganic metal halides (HOIMHs) hold great promise for nonlinear optical (NLO) applications. However, their practical applications are severely hindered by the poor environmental stability and photostability. Herein, guided by the hard and soft acids and bases (HSAB) theory, we quantitatively calculated and compared the chemical hardness of all elements in the periodic table based on density functional theory, and found osmium (Os) exhibits the highest chemical hardness among Group VIII transition metals. Thus, we synthesized the chiral osmium‐based HOIMHs, ( R / S ‐3BrMBA) 2 OsCl 6 ( R / S ‐Os ), and systematically investigated their NLO properties and stability. As expected, the obtained chiral osmium halides remain stable after two months of exposure to air, and the second‐harmonic generation (SHG) intensity remains almost unchanged after the same period, confirming their outstanding long‐term stability. The efficient SHG responses with effective second‐order nonlinear susceptibility ( χ eff ) of 6.4 pm/V and strong SHG circular dichroism (SHG‐CD) with anisotropy factor (| g SHG‐CD |) of 0.33 are also observed. Our work provides valuable HSAB‐guided screening strategy for predicting and designing the highly stable NLO materials.

Recently, 2D materials have emerged as a focal point in materials science research. Conventional 2D systems predominantly derive from layered van der Waals (vdW) crystals, where individual atomic planes are held together by weak interlayer interactions. However, groundbreaking developments have challenged this paradigm through the successful isolation of 2D materials from non‐van der Waals (non‐vdW) bulk crystals. Non‐vdW 2D materials resemble their vdW counterparts in atomically thin sheets with strong in‐plane covalent/ionic bonding but manifest distinguished structural characteristics, including large lattice distortions, abundant dangling bonds, and coordinatively unsaturated surface atoms. These intrinsic features endow them with enhanced surface reactivity and dynamic electronic states, which promote chemisorption of reactive species and accelerate interfacial charge transfer kinetics‐properties that are highly advantageous for energy applications. Nevertheless, the absence of weak interlayer vdW forces poses significant challenges in exfoliation processes, with fundamental mechanisms remaining poorly understood. This review systematically examines state‐of‐the‐art liquid‐phase exfoliation (LPE) methodologies for non‐vdW nanoflakes synthesis, critically analyzing their mechanistic foundations, process‐structure‐property relationships, and performance benchmarks in energy‐related technologies. Furthermore, key challenges are identified in improving nanoflakes quality, precise kinetic control, and advancing next‐generation artificial intelligence (AI) and smart energy systems, while proposing interdisciplinary strategies to advance this burgeoning field.

Image-based iterative methods like Phase Diversity (PD) and Gerchberg-Saxton (GS) are widely used for wavefront sensing in space telescopes due to their simple hardware and high accuracy. However, harsh space conditions—such as CCD defects and noise—can degrade reconstruction performance. To address this, we propose a PD-GS cross-iterative method that selectively filters pixels during iterations, excluding unfavorable ones to mitigate their impact on phase estimation. Simulations and experiments show that the method significantly improves the robustness of phase retrieval, achieving a detection accuracy of ∼ 0.058λ even with noise and 10% defective CCD pixels.

Abstract The commercialization of polymer solid-state electrolytes (PSEs) is hindered by the persistent trade-off between ionic conductivity and mechanical stability, both of which are essential for high-performance energy storage systems. This review examines this challenge by analyzing the underlying mechanisms governing ion transport and mechanical degradation, while discussing targeted strategies to mitigate these limitations. Recent advances are summarized, spanning molecular-level modifications, such as dynamic crosslinking and heteroatom doping, as well as multiscale design approaches, including inorganic-organic composite architectures and engineered ion-conduction pathways. Collectively, these innovations have demonstrated the potential to achieve room-temperature ionic conductivities exceeding 1 mS·cm-1 while maintaining sufficient mechanical robustness to suppress lithium dendrite growth. Key strategies for enhancing ionic conductivity include molecular structure regulation to promote polymer segmental motion, optimization of ion transport pathways, and the design of composite electrolytes incorporating ionophilic fillers to establish continuous conduction networks. In parallel, engineering stable electrode-electrolyte interfaces is highlighted as a critical approach to improving overall electrochemical performance and long-term stability. Furthermore, emerging opportunities such as machine-learning-assisted material discovery and scalable manufacturing technologies are discussed as promising routes toward the practical implementation of PSEs. By integrating these advances, PSEs are expected to play a pivotal role in next-generation safe, flexible, and high-energy-density batteries. This review provides a comprehensive roadmap for addressing the conductivity-stability trade-off and accelerating the commercialization of advanced PSEs.

Flexible electronic devices demand semiconducting materials that combine high charge transport performance, mechanical resilience, and compatibility with advanced patterning techniques. Conventional photolithography is incompatible with polymer semiconductors, and existing photo-crosslinking strategies often compromise mobility due to backbone side reactions. Here we report an oxetane side‑chain engineering strategy that enables a diketopyrrolopyrrole (DPP)‑based random terpolymer, PDPPSe‑oxe17, to form robust crosslinked networks under mild UV irradiation with iodonium salt photoinitiators. Controlled incorporation of oxetane groups (17 mol%) preserves the electronic structure of the conjugated backbone while enabling rapid ring‑opening polymerization for high‑resolution photopatterning. The polymer exhibits a high hole mobility of 2.19 ± 0.28 cm2 V- 1 s- 1, which slightly increases to 2.27 ± 0.19 cm2 V- 1 s- 1 after crosslinking-representing one of the highest mobilities reported for photopatterned OFETs. The resulting 3D polyoxetane network imparts good mechanical robustness, allowing films to withstand 108% strain and retain ∼85% and ∼76% mobility at 30% and 50% strain. Even at 100% strain, the mobility remains ∼1.4 ± 0.12 cm2 V- 1 s- 1, whereas non‑crosslinked counterparts retain only ∼3% of their initial mobility. This work establishes a generalizable molecular design principle for intrinsically photopatternable and stretchable polymer semiconductors.

Random donor-acceptor (D-A) conjugated polymers offer exceptional mechanical compliance for flexible electronics, yet their vast compositional space makes rational optimization extremely challenging. Here, we introduce a combined side-chain self-doping and Bayesian optimization (BO) strategy that enables rapid, low-sample-count tuning of polarity in random terpolymers. Using a diketopyrrolopyrrole-based polymer (PDPPBT) as a model system, we introduced dimethylamino (NMe2) self-doping groups to modulate carrier polarity. The optimization process, navigating a non-linear structure-property landscape, converged to the optimal composition (PDPPBT-NM15.218) after a single BO iteration with only six experimental data points. The resulting polymer exhibits nearly perfectly balanced ambipolar transport (mu ave h/mu ave e = 1) in both rigid and flexible OFETs. Comprehensive characterizations reveal that BO successfully located the critical trade-off point where self-doping effectively modulates frontier orbital energies, aligns Fermi levels, and subtly reorganizes thin-film microstructures to enable balanced charge transport. This work demonstrates the power of BO in decoding complex composition-function relationships, offering a generalizable route to accelerate the discovery of high-performance functional polymers.image

This tutorial review introduces the fundamental principles, core materials, interfacial engineering, and key technologies/strategies for achieving fully printed organic electronics with high performance and high functional density.

ABSTRACT Fabrication of high‐performance circularly polarized organic light‐emitting diodes (CP‐OLEDs) remains greatly challenging, as simultaneous optimization of facile synthesis, easy chiral resolution, high efficiency, and large dissymmetry factor is difficult to realize. Here, we report an innovative chiral host engineering strategy featuring through‐space coupling (TSC) skeletons for sensitizing achiral multi‐resonance thermally activated delayed fluorescence (MR‐TADF) luminogens, which facilitates efficient chiral transfer and superior electroluminescence (EL) performance to resolve the above tradeoff. Two couples of TSC chiral hosts, ( R / S )‐BNM‐2T and ( R / S )‐BNM‐AT , were constructed by connecting ( R / S )‐binaphthylamine moieties acting as donors and chiral core to diphenyltriazine acceptors of different quantities, avoiding the demand for enantiomeric resolution. These TSC chromophores display intense circularly polarized luminescence, high photoluminescence quantum yields, and efficient exciton harvesting enabled by rapid high‐level reverse intersystem crossing. Non‐doped CP‐OLEDs based on ( R / S )‐BNM‐2T showed EL dissymmetry factors ( g EL ) of +7.60 × 10 −3 and −6.73 × 10 −3 at 450 nm. However, using ( R / S )‐BNM‐2T as the host to sensitize achiral MR‐TADF emitter ( BN2 ), the resulting devices yielded comparatively high g EL values up to +1.17 × 10 −2 and −1.06 × 10 −2 , accompanied by maximum external quantum efficiency over 21%, suppressed efficiency roll‐off, and narrowband emission.

Near-infrared circularly polarized luminescence (NIR-CPL) holds great promise for advanced photonic applications, however, simultaneously achieving both high photoluminescence quantum yield (PLQY) and large asymmetry factor (glum) in the NIR region remains challenging owing to the energy-gap law. Herein, we propose a chiral quantum-cutting strategy based on rare-earth ion-doped chiral perovskite quantum dots (PeQDs). Specifically, the obtained chiral PeQDs exhibit strong NIR-CPL at 985 nm with both a large glum of 0.092 and high PLQY of 157.2%, resulting in an exceptional figure of merit (FM = |glum| × PLQY) of 0.145, representing the highest value among the reported chiral perovskites. The femtosecond-transient absorption spectra confirmed an ultrafast energy transfer accompanied by efficient spin preservation owing to the chirality-induced spin selectivity (CISS) effect, which resulted in the imbalanced spin population of Yb3+ ions and enabled efficient NIR-CPL. Therefore, for the first time, we proposed and demonstrated the concept of chiral quantum-cutting effect and revealed the mechanism of spin flip and preservation during energy and chirality transfer based on the CISS effect. Our work provides a novel strategy for designing efficient NIR-CPL materials with large glum and high PLQY, opening new avenues for developing high-performance chiral optoelectronic and spintronic devices in the NIR region.

Neuromorphic computing, particularly memristor-based architectures, offers a promising route to overcome the von Neumann bottleneck. Single-molecule devices, with their high integration density and low energy consumption, represent an emerging platform for next-generation computing. Here, we report the first optoelectronic volatile single-molecule memristor based on the organic photovoltaic material Y6. The device exhibits reproducible conductance switching driven by electric-field-induced structural relaxation, enabling gradual and linear conductance modulation that mimics synaptic behavior. Under red-light illumination, the Y6 junction shows a remarkable 457% increase in conductance and a significantly reduced switching threshold, demonstrating strong photoresponsivity and low-power operation. Furthermore, frequency-dependent pulse tests clearly reproduce short-term synaptic plasticity (STP), demonstrating the memristor's ability to emulate dynamic synaptic functions. When the experimentally measured current response of the Y6 single-molecule memristor is incorporated into an artificial neural network (ANN) model, the system achieves a speech-recognition accuracy of 71.50%, closely matching that of the benchmark ANN (74.90%). This work pioneers the realization of synaptic functionality in a single-molecule memristor and validates its application within an artificial neural network. It provides a new strategy for developing highly integrated molecular-scale neuromorphic computing devices.

Organic field-effect transistors are fabricated by taking buckybowl single crystals as active semiconductors, and show ultrasensitive and highly selective detection of trifluoroacetic acid vapor.