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The presence of protein aggregates in numerous human diseases underscores the significance of detecting these aggregates to comprehend disease mechanisms and develop novel therapeutic approaches for combating these disorders. Despite the development of various biosensors and fluorescent probes that selectively target amyloid fibers or amorphous aggregates, there is still a lack of tools capable of simultaneously detecting both types of aggregates. Herein, we demonstrate the quantitative discernment of amorphous aggregates by QM‐FN‐SO3, an aggregation‐induced emission (AIE) probe initially designed for detecting amyloid fibers. This probe easily penetrates the membranes of the widely‐used prokaryotic model organism Escherichia coli, enabling the visualization of both amorphous aggregates and amyloid fibers through near‐infrared fluorescence. Notably, the probe exhibits sensitivity in distinguishing the varying aggregation propensities of proteins, regardless of whether they form amorphous aggregates or amyloid fibers in vivo. These properties contribute to the successful application of the QM‐FN‐SO3 probe in the subsequent investigation of the antiaggregation activities of two outer membrane protein (OMP) chaperones, both in vitro and in their physiological environment. Overall, our work introduces a near‐infrared fluorescent chemical probe that can quantitatively detect amyloid fibers and amorphous aggregates with high sensitivity in vitro and in vivo. Furthermore, it demonstrates the applicability of the probe in chaperone biology and its potential as a high‐throughput screening tool for protein aggregation inhibitors and folding factors. [ABSTRACT FROM AUTHOR]

Unpredictable in vivo therapeutic feedback of reactive oxygen species (ROS) efficiency is the major bottleneck of photodynamic therapy (PDT). Herein, novel PDT‐based nanotheranostics Pa–Mn&CH‐A@P are elaborately constructed for in vivo tracking biodistribution and in situ self‐reporting PDT, which innovatively unites magnetic resonance imaging (MRI) and chemiluminescence (CL) signals. Taking advantages of the versatility of lanthanide coordination chemistry and flash nanoprecipitation (FNP) technology, photosensitizers, MRI, and CL agents are unprecedently integrated within a stable and uniform nanotheranostic. Specifically, MRI signal offers detailed dose distribution of nanotheranostics with high‐spatial resolution, and CL signal timely performs in situ evaluation of ROS generation with high sensitivity. This dual‐modal MRI/CL nanotheranostic makes a breakthrough in high fidelity feedback for oral tumor, conquering the inherent unpredictable obstacles on spatially and sensitively reporting PDT. [ABSTRACT FROM AUTHOR]

Uniting photothermal therapy (PTT) with magnetic resonance imaging (MRI) holds great potential in nanotheranostics. However, the extensively utilized hydrophobicity‐driven assembling strategy not only restricts the intramolecular motion‐induced PTT, but also blocks the interactions between MR agents and water. Herein, we report an aggregation‐induced emission luminogen (AIEgen)‐mediated polyelectrolyte nanoassemblies (APN) strategy, which bestows a unique "soft" inner microenvironment with good water permeability. Femtosecond transient spectra verify that APN well activates intramolecular motion from the twisted intramolecular charge transfer process. This de novo APN strategy uniting synergistically three factors (rotational motion, local motion, and hydration number) brings out high MR relaxivity. For the first time, APN strategy has successfully modulated both intramolecular motion and magnetic relaxivity, achieving fluorescence lifetime imaging of tumor spheroids and spatio‐temporal MRI‐guided high‐efficient PTT. [ABSTRACT FROM AUTHOR]

The occurrence and transmission of chirality is a fascinating characteristic of nature. However, the intermolecular transmission efficiency of circularly polarized luminescence (CPL) remains challenging due to poor through‐space energy transfer. We report a unique CPL transmission from inducing the achiral acceptor to emit CPL within a specific liquid crystal (LC)‐based intermolecular system through a circularly polarized fluorescence resonance energy transfer (C‐FRET), wherein the luminescent cholesteric LC is employed as the chirality donor, and rationally designed achiral long‐wavelength aggregation‐induced emission (AIE) fluorophore acts as the well‐assembled acceptor. In contrast to photon‐release‐and‐absorption, the chirality transmission channel of C‐FRET is highly dependent upon the energy resonance in the highly intrinsic chiral assembly of cholesteric LC, as verified by deliberately separating the achiral acceptor from the chiral donor to keep it far beyond the resonance distance. This C‐FRET mode provides a de novo strategy concept for high‐level information processing for applications such as high‐density data storage, combinatorial logic calculation, and multilevel data encryption and decryption. [ABSTRACT FROM AUTHOR]

Design of controllable nanoprofragrances is critically challenging in cosmetic and decoration industries. Given that most profragrances based on physical encapsulation always suffer unreliable controllability, undefined loading efficiency, and poor stability, here we have for the first time constructed dual‐controllable profragrance platform based on pH‐activated polymer to achieve the specific pH‐triggered fragrance release, which consists of hydrophilic PEG unit, hydrophobic pH‐activated unit, and pH‐triggered unit, thereby guaranteeing profragrances with delicate controllability, homogeneous nanoparticles, well‐defined loading efficiency, and high stability. Dynamic laser scattering experiments demonstrate that the activated polymers possess excellent pH‐switchable property with high stability. Particularly, time‐dependent headspace release performance of all three profragrances is fitting to First‐Order kinetic model (R2 > 0.99). Finally, the step‐by‐step controllability of the profragrance platform with pH‐activated behavior and subsequently pH‐triggered release is realized both in aqueous solution and on targeted leather surface, which is highly desirable for the long‐lasting scent. [ABSTRACT FROM AUTHOR]

Directly converting sunlight into hydrogen fuels using particulate photocatalysts represents a sustainable route for clean energy supply. Organic semiconductors have emerged as attractive candidates but always suffer from optical and exciton recombination losses with large exciton "dead zone" inside the bulk material, severely limiting the catalytic performance. Herein, we demonstrate a facile strategy that combines a scalable flash nanoprecipitation (FNP) method with hydrophilic soluble polymers (PC‐PEG5 and PS‐PEG5) to prepare highly efficient nanosized photocatalysts without using surfactants. Significantly, a 70‐fold enhancement of hydrogen evolution rate (HER) is achieved for nanosized PC‐PEG5, and the FNP‐processed PS‐PEG5 shows a peak HER rate of up to 37.2 mmol h−1 g−1 under full‐spectrum sunlight irradiation, which is among the highest results for polymer photocatalysts. A scaling‐up production of nanocatalyst is demonstrated with the continuously operational FNP. [ABSTRACT FROM AUTHOR]

Photocaging holds promise for the precise manipulation of biological events in space and time. However, current near‐infrared (NIR) photocages are oxygen‐dependent for their photolysis and lack of timely feedback regulation, which has proven to be the major bottleneck for targeted therapy. Herein, we present a hypoxia‐dependent photo‐activation mechanism of dialkylamine‐substituted cyanine (Cy‐NH) accompanied by emissive fragments generation, which was validated with retrosynthesis and spectral analysis. For the first time, we have realized the orthogonal manipulation of this hypoxia‐dependent photocaging and dual‐modal optical signals in living cells and tumor‐bearing mice, making a breakthrough in the direct spatiotemporal control and in vivo feedback regulation. This unique photoactivation mechanism overcomes the limitation of hypoxia, which allows site‐specific remote control for targeted therapy, and expands the photo‐trigger toolbox for on‐demand drug release, especially in a physiological context with dual‐mode optical imaging under hypoxia. [ABSTRACT FROM AUTHOR]

Unpredictable in vivo therapeutic feedback of hydroxyl radical (.OH) efficiency is the major bottleneck of chemodynamic therapy. Herein, we describe novel Fenton‐based nanotheranostics NQ‐Cy@Fe&GOD for spatio‐temporally reporting intratumor.OH‐mediated treatment, which innovatively unites dual‐channel near‐infrared (NIR) fluorescence and magnetic resonance imaging (MRI) signals. Specifically, MRI signal traces the dose distribution of Fenton‐based iron oxide nanoparticles (IONPs) with high‐spatial resolution, meanwhile timely fluorescence signal quantifies.OH‐mediated therapeutic response with high spatio‐temporal resolution. NQ‐Cy@Fe&GOD can successfully monitor the intracellular release of IONPs and.OH‐induced NQO1 enzyme in living cells and tumor‐bearing mice, which makes a breakthrough in conquering the inherent unpredictable obstacles on spatio‐temporally reporting chemodynamic therapy, so as to manipulate dose‐dependent therapeutic process. [ABSTRACT FROM AUTHOR]

In vivo fluorescent monitoring of physiological processes with high‐fidelity is essential in disease diagnosis and biological research, but faces extreme challenges due to aggregation‐caused quenching (ACQ) and short‐wavelength fluorescence. The development of high‐performance and long‐wavelength aggregation‐induced emission (AIE) fluorophores is in high demand for precise optical bioimaging. The chromophore quinoline‐malononitrile (QM) has recently emerged as a new class of AIE building block that possesses several notable features, such as red to near‐infrared (NIR) emission, high brightness, marked photostability, and good biocompatibility. In this minireview, we summarize some recent advances of our established AIE building block of QM, focusing on the AIE mechanism, regulation of emission wavelength and morphology, the facile scale‐up and fast preparation for AIE nanoparticles, as well as potential biomedical imaging applications. [ABSTRACT FROM AUTHOR]

Chemiluminescence (CL)‐based technologies have revolutionized in vivo monitoring of biomolecules. However, significant technical hurdles have limited the achievement of trigger‐controlled, bright, and enriched CL signal. Herein, a dual‐lock strategy uses sequence‐dependent triggers for bright optical imaging with real‐time fluorescent signal and ultra‐sensitive CL signal. These probes can obtain an analyte‐triggered accumulation of stable pre‐chemiluminophore with aggregation‐induced emission (AIE), and then the pre‐chemiluminophore exhibits a rapid photooxidation process (1,2‐dioxetane generation) by TICT‐based free‐radical addition, thereby achieving an enrichment and bright CL signal. The dual‐lock strategy expands the in vivo toolbox for highly accurate analysis and has for the first time allowed access to accurately sense and trace biomolecules with high‐resolution, dual‐mode of chemo‐fluoro‐luminescence, and three‐dimensional (3D) imaging in living animals. [ABSTRACT FROM AUTHOR]

The rational design of high-performance fluorescent materials for cancer targeting in vivo is still challenging. A unique molecular design strategy is presented that involves tailoring aggregation-induced emission (AIE)-active organic molecules to realize preferable far-red and NIR fluorescence, well-controlled morphology (from rod-like to spherical), and also tumor-targeted bioimaging. The shape-tailored organic quinoline-malononitrile (QM) nanoprobes are biocompatible and highly desirable for cell-tracking applications. Impressively, the spherical shape of QM-5 nanoaggregates exhibits excellent tumor-targeted bioimaging performance after intravenously injection into mice, but not the rod-like aggregates of QM-2. [ABSTRACT FROM AUTHOR]

The simultaneous discrimination of Cys, Hcy, and GSH by a single probe is still an unmet challenge. The design and synthesis of a small molecule probe MeO-BODIPY-Cl (BODIPY=boron dipyrromethene) is presented, which can allow Cys, Hcy, and GSH to be simultaneously discriminated on the basis of three distinct fluorescence turn-on responses. The probe reacts with these thiols to form sulfenyl-substituted BODIPY, which is followed by intramolecular displacement to yield amino-substituted BODIPY. The kinetic rate of the intramolecular displacement reaction determines the observed different sensing behavior. Therefore, the probe responds to Cys, Hcy, and GSH with fluorescence turn-on colors of yellow, yellow and red, and red, respectively. With this promising feature in hand, the probe was successfully used in imaging of Cys, Hcy and GSH in living cells. [ABSTRACT FROM AUTHOR]

High‐fidelity trapping of mitochondrial dynamic activity is critical to value cellular functions and forecast disease but lack of spatial–temporal probes. Given that commercial mitochondria probes suffering from low photostability, aggregation‐caused quenching effect, and limited signal‐to‐noise ratio from fluorescence "always on" in the process of targeting mitochondria, here, the rational design strategy of a novel aggregation‐induced emission (AIE) molecular motif and unique insight into the high‐fidelity targeting of mitochondria is reported, thereby illustrating the relationship between tailoring molecular aggregation state and mitochondrial targeting ability. This study focuses on how to exactly modulate the hydrophilicity and the aggregated state for realizing "off‐on" fluorescence, as well as matching the charge density to go across the cell membrane for mitochondrial targeting. Probe tricyano‐methylene‐pyridine (TCM‐1) exhibits an unprecedented high‐fidelity feedback on spatial–temporal mitochondrial information with several advantages such as "off‐on" near‐infrared characteristic, high targeting capacity, favorable biocompatibility, as well as excellent photostability. TCM‐1 also produces reactive oxygen species in situ for image‐guided photodynamic anticancer therapy. Through unraveling the relationship between tuning molecular aggregation behavior and organelle‐specific targeting ability, for the first time, a unique guide is provided in designing AIE‐active probes to explore the hydrophilicity and membrane potential for targeting subcellular organelles. [ABSTRACT FROM AUTHOR]

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