Achieving outstanding narrow‐band emission and improving the triplet exciton utilization efficiency is crucial for high organic light‐emitting diodes (OLEDs) electroluminescence (EL) efficiency. Herein, novel 1,3‐asymmetrical substituted pyrene‐based blue “hot exciton” materials with aggregation‐induced emission (AIE) characteristics are synthesized, utilizing the pyrene ring's staggered energy levels for high‐performance OLEDs. The triphenylamine‐decorated pyrene‐based blue emitters exhibited narrow full width at half maxima (FWHM) < 60 nm, while the tetraphenylethylene‐decorated compounds displayed a higher fluorescence quantum yield but broader FWHM emission in the film state. These AIE luminogens (AIEgens) show good EL efficiency and high exciton utilization efficiency (>35.6%) in nondoped OLED devices. Meanwhile, both triphenylamine‐decorated and tetraphenylethylene‐decorated pyrenes are further utilized as an emitter layer in thermally activated delayed fluorescence (TADF)‐sensitized blue OLEDs with great EL performance. Moreover, the TPE‐decorated pyrene‐based TPE‐ m 2Ph demonstrated a maximum brightness, maximum current efficiency, maximum power efficiency, and maximum external quantum efficiency of 35230 cd m −2 , 42 cd A −1 , 48 lm W −1 , and 14.9%, respectively.

The transition from molecular-scale intramolecular non-covalent conformational locking (NoCL) to hierarchically organized intra- and intermolecular NoCL in aggregates presents transformative potential for engineering photo-theranostic aggregates (PTAs) with enhanced rigidity and light-harvesting ability. Nevertheless, the simultaneous achievement of intra- and intermolecular NoCL in the aggregate state remains significant challenge, primarily due to the inherent complexity of intermolecular interactions and the lack of effective regulation strategies, rendering this frontier largely underexplored. Herein, we proposed a side-chain isomerization strategy to manipulate intra-/intermolecular NoCL for constructing high performance NIR-II multimodal PTAs with planar structures. Two pairs of isomers, whose alkyl side-chains are linear (l-series) and branched (b-series) configurations, were designed and syn-thesized. Crystals of b-series demonstrated planar structures attributed to robust S‧‧‧O interactions for intramolecular NoCL and multiple acceptor-acceptor intermolecular interactions for intermolecular NoCL, in contrast to those of l-series with twisted structures. Theoretic calculation and femtosecond transient absorption spectra revealed the dual NoCL effectively narrowed the energy gap and optimized excited-state energy dissipation pathway, resulting in com-prehensively enhancement in phototheranostic performance including superior ROS generation, higher NIR-II bright-ness and excellent photothermal properties compared to l-series NPs. Notably, the exceptional performance of b-3CPFIC NPs enabled it as an ideal candidate in multimodal NIR-II phototheranostics of tumors. The successful imple-mentation of this side-chain isomerization strategy has unveiled a novel design paradigm for developing high-performance multifunctional NIR-II PTAs and established fundamental structure-properties relationship at aggregate level.

Helical structures such as right-handed double helix for DNA and left-handed α-helix for proteins in biological systems are inherently chiral. Importantly, chirality at the nanoscopic level plays a vital role in their macroscopic chiral functionalities. In order to mimic the structures and functions of natural chiral nanoarchitectures, a variety of chiral nanostructures obtained from artificial helical polymers are prepared, which can be directly observed by atomic force microscopy (AFM), scanning tunneling microscopy (STM), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). This review mainly focuses on the formation of chiral nanostructures and the morphology regulation triggered by polymer chain length, concentration, solvent, temperature, photoirradiation, and chemical additives. In addition, the distinct chiral functions including chiral recognition, circularly polarized luminescence, drug release, cell imaging, and antibiosis are also discussed.

Fe-N-C materials are emerging catalysts for replacing precious platinum in the oxygen reduction reaction (ORR) for renewable energy conversion. However, their potential is hindered by sluggish ORR kinetics, leading to a high overpotential and impeding efficient energy conversion. Using iron phthalocyanine (FePc) as a model catalyst, we elucidate how the local strain can enhance the ORR performance of Fe-N-Cs. We use density functional theory to predict the reaction mechanism for the four-electron reduction of oxygen to water. Several key differences between the reaction mechanisms for curved and flat FePc suggest that molecular strain accelerates the reductive desorption of *OH by decreasing the energy barrier by ∼60 meV. Our theoretical predictions are substantiated by experimental validation; we find that strained FePc on single-walled carbon nanotubes attains a half-wave potential (E1/2) of 0.952 V versus the reversible hydrogen electrode and a Tafel slope of 35.7 mV dec-1, which is competitive with the best-reported Fe-N-C values. We also observe a 70 mV change in E1/2 and dramatically different Tafel slopes for the flat and curved configurations, which agree well with the calculated energies. When integrated into a zinc-air battery, our device affords a maximum power density of 350.6 mW cm-2 and a mass activity of 810 mAh gZn-1 at 10 mA cm-2. Our results indicate that molecular strain provides a compelling tool for modulating the ORR activities of Fe-N-C materials.

Most covalent organic frameworks (COFs) exhibit minimal or weak emission, even when constructed with highly emissive AIEgens. The fluorescence quenching issues in COFs are typically attributed to nonradiative decay induced by molecular motion or intramolecular charge transfer. As a result, designing emissive COF materials remains a desirable yet challenging task. In this study, we present the construction of highly emissive COFs through the integration of dual-docking AIEgens. Mechanism studies reveal that this integration effectively restricts undesired molecular motion and reduces charge transfer to the imine linkage, thereby enhancing fluorescence generation and improving the crystallinity of the COFs. One benzothiadiazide-based COF, COF-DPQP-BT, exhibits notable brightness with a photoluminescence quantum yield of 36.5% and is successfully utilized for in vivo three-photon fluorescence imaging of brain vasculature in mice, achieving an imaging depth of approximately 1.2 mm. This work provides valuable insights for the design of emissive COFs.

Organic room-temperature phosphorescence (RTP) emitters have emerged as a compelling research field with broad applications in optoelectronics, anti-counterfeiting, and biomedical imaging. This interest stems from the efficient utilization of the radiative relaxation of the triplet excited state. An efficient intersystem crossing (ISC) process alone is not sufficient for efficient and long-lived RTP emission. It is also crucial to suppress molecular motion, including rotation, vibration, and translation. By rigidifying molecular structures to suppress these motions, triplet excitons are effectively stabilized, and non-radiative transitions are reduced, presenting a viable strategy for developing a variety of efficient and long-lived RTP materials. This review focuses on the current rational engineering efforts to suppress molecular motion for efficient and long-lived RTP generation, enhancing understanding of the interplay between molecular motion and RTP emission, and emphasizing the critical role of restricting molecular motion in the development of efficient and long-lived RTP materials.

Reverse intersystem crossing (RISC) process is critical for thermally activated delayed fluorescence (TADF) materials to realize spin–flip of triplet excitons in organic light-emitting diodes (OLEDs), but the RISC processes of most TADF materials are not fast enough, undermining electroluminescence (EL) efficiency stability and operational lifetime. Herein, a symmetry breaking strategy to accelerate RISC processes is proposed. By designing asymmetric electron-withdrawing backbone consisting of benzonitrile and xanthone/thioxanthone groups, two new asymmetric TADF molecules, 4 t CzCN- p XT and 4 t CzCN- p TXT, with multiple 3,6-di- tert -butylcarbazole donors are successfully developed. They own increased molecular vibrations, which promote intrinsic RISC process and enable multi-channel transitions via vibronic coupling of high-lying triplet states. Consequently, they exhibit fast RISC rates of up to 1.24 × 10 7 s −1 , being one order of magnitude higher than that of the symmetric control molecule. They can perform as luminescent materials in OLEDs, providing outstanding external quantum efficiencies (EQEs) of up to 31.2% and 35.8% in non-doped and doped devices, respectively, with very small roll-offs. The OLEDs using them as sensitizers for multi-resonance emitters achieve remarkable EQEs over 40%, and extraordinary operational stability with LT 90 of 24974 h at 1000 cd m −2 , demonstrating their great potentials in OLEDs.

Phototheranostic agents (PTA) control the process of phototheranostics for cancer. However, the existing PTA still cannot meet the needs of practical biomedical applications. Hence the development of new PTA will be imperative. In this contribution, a "3+2" cooperation pattern of amphipathicity PTA (named TDTMSB) with aggregation-induced emission (AIE) features is designed and synthesized to perform near-infrared I/II fluorescence imaging, photoacoustic imaging, photothermal imaging, and Type I/II photodynamic therapy (PDT)-photothermal therapy (PTT) synergistic phototherapy for malignant tumors. Briefly, the target products (TMSB, TTMSB and TDTMSB) are successfully prepared by the reaction of 2-methyl-1-(3-sulfonatepropyl)-benzothiazolium (MSB) and triphenylamine derivatives. They have high rotor twisted structure, doner-acceptor (D-A) conformation and unique AIE performances. Compared to TMSB and TTMSB, the TDTMSB exhibits a long near infrared emission that extends into the NIR II region, large Stokes shift (300 nm) and small energy gap. Simultaneously, it shows high ROSs generation capacity (1O2, OH, and O2 -), photothermal conversion efficiency (up to 40.5%), and specific recognition of lysosomes in tumor cells. Furthermore, TDTMSB not only exhibits excellent multimodal imaging capabilities, but also carry out Type I/II PDT-PTT synergistic enhancement effect for malignant tumor. Therefore, TDTMSB is expected to be a promising PTA for multimodal image-guided phototherapy of tumors.

Experimental and theoretical analysis demonstrated that the active intramolecular motions in the excited state of all molecules at single molecule level imparted them with more twisted structural conformations and weak emission. However, owing to the restriction of intramolecular motions in the nano/macro aggregate state, all the molecules assumed less twisted conformations with bright emission. Synergic strong and weak intermolecular interactions allowed their crystals to undergo reversible deformation, which effectively solved the problem of the brittles of organic crystals, meanwhile imparted them with excellent elastic performance.

Seeking methods to realize multiple fluorescence changes in a single luminogenic system is of great importance for both chemistry and bionics research. Due to the lack of effective strategies and functional motifs, luminogens with multiple switching and controllable models are still scarce. Herein, we report a chromone-based aggregation-induced emission luminogen called Z-CDPM, which exhibit six distinct, tunable thermal and photoswitchable states, offering controllable thermochromic or photochromic behavior under varying conditions. Specifically, five different reactions are involved: reversible Z/E isomerization, irreversible cyclization and elimination under thermal treatment, and photoarrangement of Z-CDPM and its thermal cyclization product under UV irradiation. The relative independence of the switching states is effectively maintained. Experimental and theoretical analyses validate our design strategies and provide valuable insights into the detailed mechanisms of these reactions, and single crystals further confirm their structures. Additionally, practical applications, including multiple-colored images, quick response codes, and an advanced information encryption system, are developed to demonstrate the utility. This work thus provides effective strategies and structural motifs for the design of multiresponsive luminogens and multifunctional systems.

Marching toward next-generation ultrahigh-definition and high-resolution displays, the development of high-performance blue organic light-emitting diodes (OLEDs) with narrow emission and high luminance is essential and requires conceptual advancements in both molecular and device design. Herein, a blue organic emitter is reported that exhibits hot-exciton and aggregation-induced emission characteristics, and use it as a sensitizer in the proposed triplet-triplet annihilation (TTA)-assisted hot-exciton-sensitized fluorescence (HSF) device, abbreviated THSF. Results show that through dual-channel stepwise Förster and Dexter energy transfer processes, the THSF system can simultaneously enhance exciton utilization, accelerate exciton dynamics, and reduce the concentration of triplet excitons. The smooth management of excitons makes the overall performance of the THSF device superior to the control TTA fluorescence and HSF devices. Furthermore, a high-performance narrowband blue (CIEx,y = 0.13, 0.12) OLED is achieved using a two-unit tandem device design, providing an excellent maximum external quantum efficiency of 18.3%, a record-high L90% (the luminance where the ƞext drops to 90% of its peak value) of ≈20 000 cd m-2, and a long half-lifetime at 100 cd m-2 initial luminance of ≈13 256 h. These results showcase the great potential of the THSF strategy in realizing efficient and stable blue OLEDs with narrow emission and high luminance.

Photodynamic immunotherapy presents a non-invasive strategy characterized by spatiotemporal control and minimal side effects to induce immunogenic cell death (ICD). This approach significantly enhances the release of tumor-associated antigens and damage-associated molecular patterns, thereby improving cancer immunotherapy outcomes. However, hypoxia and antioxidant defenses at tumor sites considerably diminish the efficacy of photodynamic immunotherapy. In this work, a covalent warhead, alkyneamide, is introduced into an AIE photosensitizer to develop a novel covalent photosensitizer, MBTP-PA, which targets redox systems and facilitates ferroptosis- and pyroptosis-mediated photodynamic immunotherapy by thiol-yne click reactions. The covalent photosensitizer interacts with intracellular thiol compounds such as cysteine and glutathione, disrupting the intracellular antioxidant system and alleviating hypoxia. This results in enhanced photodynamic therapy (PDT) efficacy compared to the non-covalent photosensitizer MBTP-A. Furthermore, in conjunction with PDT, this reaction therapy can activate ICD through ferroptosis and pyroptosis, thereby enhancing anti-tumor immunity. Notably, in vivo injection of MBTP-PA nanoparticles at the tumor site led to the elimination of primary tumors, inhibiting distal tumors and exhibiting minimal side effects. Therefore, this work not only integrates the thiol-yne click reactions into cellular systems, significantly enhancing the efficacy of photodynamic immunotherapy but also paves the way for developing novel photosensitizers.

Scintillators are vital components in high-energy radiation detectors and are used in fields like high-energy physics, non-destructive testing, radiochemistry, and medical diagnostics. Scintillators with aggregation-induced emission (AIE), through rational molecular design and preparation techniques, can be endowed with such properties that effectively overcome the inherent defects of existing inorganic and/or organic scintillators, such as high costs and poor mechanical properties in inorganic types and low light yield and aggregation-caused quenching for organic kinds, thus affording novel optoelectronic properties, superior performance, and broader applications. This review classifies AIE scintillators from a molecular perspective, based on their luminescence mechanisms and construction strategies, into fluorescent scintillators, thermally activated delayed fluorescence scintillators, metal cluster scintillators, organic-inorganic hybrid scintillators, and metal-organic framework scintillators. This review starts with analyses of these building strategies and the structure-performance relationships and then describes the applications of AIE scintillators based on their molecular structures and optoelectronic properties.

Aggregation-induced emission (AIE) luminogens, exemplified by tetraphenylethylene (TPE), exhibit enhanced fluorescence in aggregated states and have promising applications in display, photodetectors, fluorescent probes, bioimaging, and biomedicine. This study investigates the influence of varying degrees of deuteration on the photophysical properties of TPE across different aggregation states. Through the synthesis of partially and fully deuterated TPE derivatives (TPE-5d, TPE-10d, and TPE-20d), combined with steady-state fluorescence spectroscopy, time-resolved fluorescence measurements, transient absorption spectroscopy, and density functional theory (DFT) calculations, we elucidate the dual role of deuteration in modulating nonradiative decay pathways. In loosely packed nanoaggregates, increased deuteration enhances photoluminescence quantum yields (PLQY) and extends fluorescence lifetimes by reducing internal conversion rates. Conversely, in tightly packed crystalline states, deuteration leads to decreased PLQY and shortened lifetimes, attributable to the Duschinsky rotation effect (DRE), which enhances inter-mode coupling and internal conversion. Additionally, deuteration significantly prolongs the operational lifetime of blue organic light-emitting diode (OLED) devices, doubling the device lifespan in TPE-20d compared to TPE. This work underscores the necessity of evaluating structure-property relationships at the aggregate level, rather than solely at the molecular level, to fully comprehend and optimize AIE phenomena. These findings highlight the potential of isotope engineering in designing durable and efficient AIE luminogens for applications in optoelectronics and bioimaging.

Herein, a series of molecular actuators based on the crystals of (E)‐2‐(4‐fluorostyryl)benzo[d]oxazole (BOAF4), (E)‐2‐(2,4‐difluorostyryl)benzo[d]oxazole (BOAF24), (E)‐2‐(4‐fluorostyryl)benzo[d]thiazole (BTAF4) and (E)‐2‐ (2,4‐difluorostyryl)benzo[d]thiazole (BTAF24) showed unprecedented different bending behavior under UV irradiation. BOAF4 and BTAF4 bent towards light, whereas BOAF24 and BTAF24 bent away from light. Although the chemical structures of these compounds are similar, we found out the F‒H‒C interaction was the main driving force for the different molecular packing in the crystals, which led to the positive/negative phototropism of the actuators. Moreover, the theoretical calculation was carried out to reveal the mechanical properties of the crystals. Taking advantage of the photo responsive property, we achieved the potential application in pushing objects, as well as enriching and removing pollutants. This system not only achieved a class of molecular actuators with different bending behavior through introducing different number of F atom, but also realized pushing and catching behavior within one molecule, which opens a novel gate for crystal engineering

Breast cancer (BC), characterized by its heterogeneity and diverse subtypes, necessitates personalized treatment strategies. This study presents MF3Ec-TBPP nanoparticles (NPs) as a promising approach, integrating an aggregation-induced emission (AIE)-based photosensitizer, TBPP, with the MF3Ec aptamer to enhance targeted photodynamic therapy (PDT) for Luminal A subtype BC cells. The nanoparticles also feature a 1, 2-distearoyl-sn-glycero-3-phosphoethanolamine-poly(ethylene glycol) shell and dipalmitoyl phosphatidylcholine (DPPC), which stabilize the structure and inhibit singlet oxygen generation, effectively reducing off-target effects and protecting healthy tissues. Comprehensive in vitro and in vivo studies validate the NPs' specificity and effectiveness in targeting MCF-7 BC cells, achieving significant tumor growth inhibition with minimal damage to surrounding tissues. This study highlights the dual functionality of MF3Ec-TBPP NPs for both diagnosis and treatment, showcasing their potential to improve patient outcomes through precise diagnostic and therapeutic interventions.

Nanomedicine holds immense potential to revolutionize cancer therapy, yet its clinical translation remains hampered by insufficient tumor accumulation and an inability to dynamically monitor therapeutic penetration. While transcytosis-mediated transport offers a promising strategy to overcome biological barriers, existing carriers lack real-time imaging capabilities, particularly in the near-infrared II window, to guide optimization. Herein, we address this dual challenge through a multifunctional poly[L-γ-[2-( N -oxide- N,N -dimethylamino)ethyl]glutamine]-paclitaxel (OPGAX) conjugate integrated with aggregation-induced emission (AIE) luminogens. The OPGAX conjugate self-assembled into uniform nanoparticles (NPs) with a high drug-loading capacity (42.5%) and intense near-Infrared II (NIR-II) fluorescence (1000–1350 nm). The zwitterionic tertiary amine oxide (TAO) moiety endowed OPGAX with protein resistance and cell membrane affinity, leading to prolonged blood circulation and enhanced tumor accumulation. OPGAX NPs performed NIR-II imaging to visualize whole-body vasculature and dynamically track tumor penetration. In 4T1 tumor-bearing mice, OPGAX NPs achieved deep tumor infiltration via transcytosis, visualized dynamically by NIR-II imaging, and suppressed tumor growth. This platform bridges diagnostic certainty with therapeutic efficacy, offering a translatable strategy for image-guided precision oncology.

Ionic aggregates are among the most common forms of matter, yet the investigation of their molecular motion is often constrained by the instability of isolated anions and cations, as well as the lack of real-time monitoring techniques. This study presents a zwitterionic strategy that integrates both cations and anions into one fluorescent organic framework, forming a zwitterionic molecule. The zwitterionic strategy simplifies the intricate cation-anion systems that are typically found in conventional inorganic salts and imparts them with fluorescent properties, facilitating real-time tracking of ionic-interaction-induced molecular motion within ionic aggregates. Specifically, a blue shift in the fluorescence wavelength signified changes in aggregate states due to intermolecular motion, whereas a decrease in intensity was linked to intramolecular-motion-caused conformational changes. This spontaneous molecular motion enabled dynamic switching of the excited state energy-decay pathway, leading to switchable color-light responses. Overall, the zwitterionic strategy offers a novel framework for exploring the properties and behaviors of molecules in ionic aggregates.

Achieving long-lived room temperature phosphorescence (RTP) in organic materials has garnered significant attention in the field of optoelectronics. Although many host-guest systems with versatile performances have been developed, their photophysical mechanisms remain unclear due to the complicated intermolecular interactions and multiple energy transfer pathways, leading to unavoidable trial-and-error in molecular designs. Here we reveal that the dynamic coupling process in the excited state is crucial for inducing phosphorescence, where host and guest molecules firstly couple to enhance the intersystem crossing efficiency, and then decouple to transfer excitons to the triplet state of guest. Such a process shows universal applicability and tunable performance, with the longest lifetime for red RTP (τP = 2.4 s) reported so far. We anticipate the present work as a starting point for more sophisticated models on excited-state dynamic behaviors within host-guest systems.