Aggregation-induced emission luminogens(AIEgens)are typically largeπ-conjugated molecules,but their low affinity and noninvasiveness toward analytes limit practical applications.To address this,smaller,more planar AI...Aggregation-induced emission luminogens(AIEgens)are typically largeπ-conjugated molecules,but their low affinity and noninvasiveness toward analytes limit practical applications.To address this,smaller,more planar AIEgens are needed.Stilbene,though structurally suitable,lacks visible luminescence.Here,we report a minimally modified stilbene-based AIEgen-4-dipropylamino-4'-cyano-bridged stilbene(DpCBS[7])-that exhibits fluorescence solvatochromism and efficient AIE across a broad polarity range in the visible region.DpCBS[7]exhibits low quantum yields(Φ_(fl)=0.010.04)in solvents from nonpolar n-hexane to polar dimethyl sulfoxide,with large Stokes shifts,viscosity-sensitive luminescence,and highly efficient solid-state luminescence(Φ_(fl)=0.70).To elucidate its dual solvatochromic and AiE behavior,femtosecond transient absorption spectroscopy was conducted.In solution,DpCBS[7]displays transient absorption with lifetimes of 21 ps(toluene)and 56 ps(acetonitrile)at 293 K,indicating ultrafast nonradiative decay leading to low Φ_(fl).Arrhenius analysis over the temperature range of 263-313 K revealed activation energies(ΔE_(a))of 9.90kJ/mol in toluene and 12.8 kJ/mol in acetonitrile for the S_(1)→S_(0) decay of DpCBS[7].The ΔE_(a) values show no clear systematic dependence on solvent polarity.In contrast,pre-exponential factor A remains consistently high regardless of solvent polarity,indicating that the striking photophysical response is governed primarily by the pre-exponential factor rather than by modulation of the activation energy.These findings highlight the fundamental importance of tailoring the distribution function through structural modification as a robust strategy to control AiE characteristics.展开更多
Ionic phototheranostic agents have found extensive application in preclinical and clinical practice owing to their excellent biocompatibility and synergistic diagnostic-therapeutic integration.However,they still suffe...Ionic phototheranostic agents have found extensive application in preclinical and clinical practice owing to their excellent biocompatibility and synergistic diagnostic-therapeutic integration.However,they still suffer from certain limitations,such as short absorption/emission wavelengths,poor photostability,aggregation-caused fluorescence self-quenching,and diminished phototherapeutic efficacy upon aggregation,which collectively hinder their efficacy in complex clinical scenarios.To address these challenges,a second near-infrared(NIR-II)ionic phototheranostic agent,namely DT-BT-BIn,is rationally designed and synthesized via an innovative dual-acceptor engineering strategy.DT-BT-BIn ingeniously integrates benzothiadiazole and benzo[c,d]indolium as dual-acceptor units,which successfully achieves superior aggregation-induced NIR-II emission characteristics,highly efficient Type Ⅰ/Ⅱ photodynamic activity coupled with photothermal effect,and excellent photostability.Moreover,the self-assembled DT-BT-BIn nanoprobes(NPs)can be effectively internalized by cancer cells in vitro.Under irradiation,DT-BT-BIn NPs are capable of disrupting mitochondrial membrane potential,thereby inducing apoptotic cell death.Furthermore,in vivo investigations demonstrate DT-BT-BIn NPs can effectively accumulate at tumor location,enabling NIR-II fluorescence/photothermal imaging-guided precise tumor ablation,while simultaneously maintaining favorable biosafety toward normal tissues.Collectively,this study underscores the considerable promise of the dual-acceptor strategy in constructing high-performance NIR-II ionic phototheranostic agents and provides a new avenue for clinical precision cancer phototherapy.展开更多
Golgi apparatus(GA)-associated secretome runs through the endomembrane system and is critical for inter-and intracellular communication networks.However,achieving in situ dissection of the GA-associated secretome rema...Golgi apparatus(GA)-associated secretome runs through the endomembrane system and is critical for inter-and intracellular communication networks.However,achieving in situ dissection of the GA-associated secretome remains challenging owing to the scarcity of specific labeling methods.This work develops an aggregation-induced emission(AIE)luminogen-mediated photocatalytic proximity labeling strategy that allows profiling of the GA-associated secretome with high spatiotemporal precision.Leveraging an AIE luminogen-derived GA-targeting photocatalyst,this strategy achieves efficient labeling of proteins in minutes within the Golgi lumen upon light activation,which enables spatiotemporally resolved modification of histidine and tyrosine residues.We succeed in profiling secretome in both living HeLa cells and hard-to-transfect macrophage HMC3 cells,and a significant subset of GA-associated secretome with 80%specificity is determined,linking the distinct GA-associated secretory profiles to cellular characteristics.The method is further applied to proteome mapping of brain and bone metastatic lung cancer cells,which reveals the underlying roles the GA-associated secretome plays in extracellular matrix organization during metastasis.This work delivers a robust tool to break the dilemma of chemical labeling of GA-associated secretome in living cells,and provides mechanistic insights into secretion regulation at the subcellular level.展开更多
Aggregation-induced emission(AIE)polymers have been extensively studied;however,the integration of AIE units into polyelectrolytes remains largely limited by the laborious multistep synthesis of pre-designed emissive ...Aggregation-induced emission(AIE)polymers have been extensively studied;however,the integration of AIE units into polyelectrolytes remains largely limited by the laborious multistep synthesis of pre-designed emissive monomers.Herein,we report a one-pot multicomponent polymerization method that directly produces main-chain charged polyelectrolytes with intrinsic AIE characteristics from non-emissive building blocks.By optimizing the monomer structures and reaction conditions,a series of soluble high-molecular-weight polymers with welldefined backbones were obtained in high yields.The resulting polyelectrolytes displayed robust AIE behavior,exhibiting fluorescence enhancement up to about 60-fold in an aqueous environment,and maintained excellent thermal stability.Owing to their cationic backbones,these polymers interact strongly with microbial surfaces and exhibit remarkable antimicrobial activities.This study establishes a synthetically efficient route to AIE polyelectrolytes and highlights their potential applications as multifunctional materials for bioimaging,antimicrobial therapy,and other applications.展开更多
It is important to understand the evolution of the matter on the polymer membrane surface.The in situ and real-time monitoring of the membrane surface will not only favor the investigation of selective layer formation...It is important to understand the evolution of the matter on the polymer membrane surface.The in situ and real-time monitoring of the membrane surface will not only favor the investigation of selective layer formation but can also track the fouling process during operation.Herein,an aggregation-induced emission(AIE)-active polymer membrane was prepared by the interfacial polymerization of a cyclodextrin-based glycocluster(CD@Glucose)and a tetraphenylethylene derivative modified with boronic acid groups(TPEDB)on the surface of a polyacrylonitrile(PAN)ultrafiltration membrane.This interfacial polymerization method can be stacked layer-by-layer to regulate the hydrophilicity and pore structure of the membrane.With the increase in the number of polymer layers,the separation and antifouling properties of the membrane gradually improved.Owing to the AIE property of the crosslinking agent TPEDB,the occurrence of interfacial polymerization and the degree of fouling during membrane operation can be monitored by the fluorescence distribution and intensity.With the aggravation of membrane fouling,the fluorescence decreased gradually,but recovered after cleaning.Therefore,this AIE effect can be used for real-time monitoring of interfacial polymerization as well as membrane fouling.展开更多
In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especia...In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especially for developing new reaction pathway to afford the functional heterocycle compounds with aggregation-induced emission(AIE)property has been rarely reported.In present work,the multi-site functionalization of in situ generated alkenes with indoles has been developed for the synthesis of diversely functionalized carbazoles through the synergistic construction of multiple C–C bonds and C=O bond.A proposed reaction sequence involving C–H alkenylation/radical oxygen atom transfer/Diels-Alder cycloaddition/dehydrogenative aromatization was supported by experiments and density functional theory calculations.Further derivative carbazole-linked-quinoxaline skeletons represent a class of AIEgens with acceptor-donor-acceptor configuration,which generated the desired twisted intramolecular charge transfer(TICT)AIE properties and could be used as fluorescent probes for detecting the micrometer-sized phase separation of polymer blends.The protocol provides a concise route for the synthesis and application of carbazole-based AIE luminogens.展开更多
Carbon monoxide(CO)is a crucial gaseous signaling molecule that regulates various physiological and pathological processes,and may exert an anti-inflammatory and protective role in drug-induced liver injury(DILI).Desp...Carbon monoxide(CO)is a crucial gaseous signaling molecule that regulates various physiological and pathological processes,and may exert an anti-inflammatory and protective role in drug-induced liver injury(DILI).Despite this,understanding the exact relationship between CO and the occurrence and development of DILI remains challenging.Hence,there is an urgent need to develop a reliable and robust tool for the rapid visual detection and assessment of CO in this context.Herein,we presented a novel near-infrared(NIR)fluorescent nanoprobe with aggregation-induced emission(AIE)properties and excited-state intramolecular proton transfer(ESIPT)characteristics for the detection and imaging of CO both in vitro and in vivo.Simultaneously,the nanoprobe enables self-assembly form nanoaggregates in aqueous media with high biocompatible,which can sense CO in situ through the conversion of yellowto-red fluorescence facilitated aggregation-induced dual-color fluorescence.What is more,this nanoprobe shows ratiometric respond to CO,which demonstrates excellent stability,high sensitivity(with a detection limit of 12.5 nmol/L),and superior selectivity.Crucially,this nanoprobe enables the visual detection of exogenous and endogenous CO in living cells and tissues affected by DILI,offering a user-friendly tool for real-time visualization of CO in living system.Hence,it holds great promise in advancing our understanding of CO’s role.展开更多
With increasing drug resistance,Candida infections have posed serious threats to public health.Photodynamic therapy harnesses light to destroy pathomycete,providing a smart strategy for combating of Candida infections...With increasing drug resistance,Candida infections have posed serious threats to public health.Photodynamic therapy harnesses light to destroy pathomycete,providing a smart strategy for combating of Candida infections.However,due to lack of organelle targeting ability and bad extracellular polymeric substances penetrability,current photosensitizers(PSs)are far from desirable to clean biofilms and fight against drug resistance.Herein,a mitochondrion targeting aggregationinduced emission PS,LIQ-TPA-TZ,was developed for the efficient photodynamic treatment of oral Candida infection.LIQ-TPA-TZ has good singlet oxygen and hydroxyl radical generation ability,which can efficiently kill the Candida guilliermondii(C.guilliermondii)and eradicate the biofilm.It not only causes mitochondrial damage by disruption of mitochondrial respiratory chain and oxidative stress-related gene but also inhibits fungal adhesion and filamentous growth to prevent Candida colonization,mycelia growth and biofilm formation,which is favorable for eliminating the potential drug resistance.In the mouse oropharyngeal Candida biofilm infection model,LIQ-TPA-TZ significantly eliminates infection,alleviates inflammation,and accelerates mucosal defect healing.This study provides a favorable strategy for confronting drug resistance,which may be a potential Candidate for the treatment of Candida infection.展开更多
Aggregation-induced emission(AIE)is a phenomenon characterized by certain fluorescent molecules that exhibit weak or no luminescence in solution but demonstrate significantly enhanced luminescence upon aggregation.Acc...Aggregation-induced emission(AIE)is a phenomenon characterized by certain fluorescent molecules that exhibit weak or no luminescence in solution but demonstrate significantly enhanced luminescence upon aggregation.Accordingly,AIE materials have successfully addressed the limitations associated with aggregation-caused quenching effects and have made significant progress in the application of various fields of medicine in recent years.At present,the application of AIE materials in gastrointestinal(GI)diseases is mainly in GI imaging,diagnosis and treatment.In this review,we summarize the applications of AIE materials in GI pathogens and GI diseases,including inflammatory bowel disease and GI tumors,and outline combined treatment methods of AIE materials in GI tumor therapy.展开更多
Fluorescence imaging-guided photodynamic therapy holds great promise for application in precise cancer diagnosis and treatment,which has motivated high requirements for phototheranostic agents.However,current photosen...Fluorescence imaging-guided photodynamic therapy holds great promise for application in precise cancer diagnosis and treatment,which has motivated high requirements for phototheranostic agents.However,current photosensitizers(PSs)generally face limitations such as short emission wavelength and inadequate reactive oxygen species(ROS)production.Aggregation-caused quenching issue also hinders the phototheranostic efficiency of PSs.Herein,theπ-bridge modulation strategy is proposed to construct ionic PSs with enhanced bioimaging and therapeutic outcomes.Two donor-π-acceptor(D-π-A)molecules TPCPY and TFCPY were obtained by incorporating phenyl and furan units asπ-bridge,respectively.Both PSs feature aggregation-induced near-infrared emission.Under light irradiation,TPCPY and TFCPY can produce both typeⅠandⅡROS.Introducing furan ring in TFCPY enhances the ROS generation capacity by typeⅠphotosensitization process,which is consistent with the reduced energy gap between singlet and triplet states from theoretical calculation.Furthermore,TFCPY can achieve quick cellular uptake,accumulate in mitochondria,and then efficiently kill cancer cells,which is superior to TPCPY.Consequently,TFCPY exhibited good antitumor outcomes and excellent in vivo fluorescence imaging ability.This work provides an efficient molecular engineering of introducing heterocycles into the D-π-A skeleton to develop high-performance PSs with both typeⅠandⅡROS generation.展开更多
Photodynamic therapy(PDT)has received much attention in recent years.However,traditional photosensitizers(PSs)applied in PDT usually suffer from aggregation-caused quenching(ACQ)effect in H_(2)O,single and inefficient...Photodynamic therapy(PDT)has received much attention in recent years.However,traditional photosensitizers(PSs)applied in PDT usually suffer from aggregation-caused quenching(ACQ)effect in H_(2)O,single and inefficient photochemical mechanism of action(MoA),poor cancer targeting ability,etc.In this work,two novel Ru(II)-based aggregation-induced emission(AIE)agents(Ru1 and Ru2)were developed.Both complexes exhibited long triplet excited lifetimes and nearly 100%singlet oxygen quantum yields in H_(2)O.In addition,Ru1 and Ru2 displayed potent photo-catalytic reduced nicotinamide adenine dinucleotide(NADH)oxidation activity with turnover frequency(TOF)values of about 1779 and 2000 h^(−1),respectively.Therefore,both Ru1 and Ru2 showed efficient PDT activity towards a series of cancer cells.Moreover,Ru2 was further loaded in bovine serum albumin(BSA)to enhance the tumor targeting ability in vivo,and the obtained Ru2@BSA could selectively accumulate in tumor tissues and effectively inhibit tumor growth on a 4T1 tumor-bearing mouse model.So far as we know,this work represents the first report about Ru(Ⅱ)-)AIE agents that possess high singlet oxygen quantum yields and also potent photocatalytic NADH oxidation activity,and may provide new ideas for rational design of novel PSs with efficient PDT activity.展开更多
Icing detection is critically important for preventing safety accidents and economic losses,especially concerning ice formation from invalidated anti-icing fluids(water and ethylene glycol)under extreme conditions.Tra...Icing detection is critically important for preventing safety accidents and economic losses,especially concerning ice formation from invalidated anti-icing fluids(water and ethylene glycol)under extreme conditions.Traditional technologies like ultrasonics and capacitor-antenna face challenges with limited detection areas,lower accuracy,and susceptibility to electromagnetic interference.Here,we introduce a novel viscosity-ultrasensitive fluorescent probe 40,4‴-(2,2-diphenyle-thene-1,1-diyl)bis-(3,5-dicarboxylate)(TPE-2B4C)based on AIEgens for moni-toring ice formation of anti-icing fluids in low-temperature environments.TPE-2B4C,consisting of four sodium carboxylate groups and multiple freely rotating benzene rings,demonstrates outstanding solubility in anti-icing fluids and exhibits no fluorescent background signal even at low temperatures(<−20°C).Upon freezing,TPE-2B4C relocates from the water phase to higher viscosity ethylene glycol,causing restriction of benzene rings and a significantly increased green fluorescence signal.TPE-2B4C can successfully determine whether the anti-icing fluids are icing from−5 to−20°C with a high contrast ratio.Due to its simple setup,fast operation,and broad applicability,our new method is anticipated to be employed for rapid,real-time,and large-scale icing detection.展开更多
Hyperbranched polymer with highly branched three-dimensional topological structure, a large number of end groups, and multifaceted functionalities have gained much attention, while polymers with aggregation-induced em...Hyperbranched polymer with highly branched three-dimensional topological structure, a large number of end groups, and multifaceted functionalities have gained much attention, while polymers with aggregation-induced emission(AIE) properties become a group of popular luminescent materials recently. The design and synthesis of AIE-active hyperbranched polymers, which combine the advantages of these two types of materials, are attractive but challenging. In this work, four hyperbranched poly(tetrahydropyrimidine)s were synthesized from the metal-free room temperature multicomponent tandem polymerization of diester group-activated internal alkyne,polyfunctional aromatic amines, and formaldehyde in methanol under the catalysis of acetic acid. Through different monomer combination and controlling the monomer loading order, hyperbranched polymers with various topological structures as well as sequences of different functional groups in the polymer backbone were obtained with high molecular weights(up to 3.0 × 10~4 g/mol) in high yields(up to 98%). The hyperbranched poly(tetrahydropyrimidine) emitted faintly in solution, while its luminescence was notably enhanced in the aggregated state, suggesting its typical aggregation-induced emission property. It is anticipated that the multicomponent polymerization may provide a synthetic platform for the construction of hyperbranched polyheterocycles with diverse structures and functionalities.展开更多
Aggregation-induced emission(AIE) active photochromic molecules have attracted growing attention for their versatile applications.Here we designed and synthesized five newly unsymmetrical photochromic diarylethene(DAE...Aggregation-induced emission(AIE) active photochromic molecules have attracted growing attention for their versatile applications.Here we designed and synthesized five newly unsymmetrical photochromic diarylethene(DAE) dyads(BTE1-5) by connecting tetraphenylethene(TPE) and aromatic substituent via bithienylethene(BTE) bridge.The chemical structures of those compounds were identified by ^1H NMR,^(13)C NMR and HRMS.The absorption and emission of these dyads were investigated by UV-vis and fluore scence spectroscopy,respectively.The results showed that all those compounds exhibited typically AIE or aggregation-induced emission enhancement(AIEE) characteristic.Particularly,when an aggregationcaused quenching(ACQ) fluorophore(triphenylamine) was grafted to the molecule,connecting with TPE via BTE-bridge,the ACQ phenomenon was dissipated and converted to an AIE luminophore,and those compounds exhibited photochromism upon irradiation with alternative UV and visible light.The solution or solid of those compounds showed distinctly fluorescence switching "ON" or "OFF" observation upon irradiation with alternative UV and visible light.It is interesting that BTE1 could be applied in recording and rewritable information storage,and the cyclization quantum yields could be affected by substituent significantly.展开更多
Photodynamic therapy(PDT) employs accumulation of photosensitizers(PSs) in malignant tumor tissue followed by the light-induced generation of cytotoxic reactive oxygen species to kill the tumor cells. The success of P...Photodynamic therapy(PDT) employs accumulation of photosensitizers(PSs) in malignant tumor tissue followed by the light-induced generation of cytotoxic reactive oxygen species to kill the tumor cells. The success of PDT depends on optimal PS dosage that is matched with the ideal power of light. This in turn depends on PS accumulation in target tissue and light administration time and period.As theranostic nanomedicine is driven by multifunctional therapeutics that aim to achieve targeted tissue delivery and image-guided therapy, fluorescent PS nanoparticle(NP)accumulation in target tissues can be ascertained through fluorescence imaging to optimize the light dose and administration parameters. In this regard, zebrafish larvae provide a unique transparent in vivo platform to monitor fluorescent PS bio-distribution and their therapeutic efficiency. Using fluorescent PS NPs with unique aggregation-induced emission characteristics, we demonstrate for the first time the real-time visualization of polymeric NP accumulation in tumor tissue and, more importantly, the best time to conduct PDT using transgenic zebrafish larvae with inducible liver hyperplasia as an example.展开更多
Detection of mercury ions(Hg^(2+))in actual samples is of significant importance due to the toxicity of Hg^(2+)to human health.In this work,a simple tetraphenylethene(TPE)derived fluorescent probe TPE-Hg based on aggr...Detection of mercury ions(Hg^(2+))in actual samples is of significant importance due to the toxicity of Hg^(2+)to human health.In this work,a simple tetraphenylethene(TPE)derived fluorescent probe TPE-Hg based on aggregation-induced emission(AIE)mechanism was synthesized.TPE-Hg can visually recognize Hg^(2+)in THF/HEPES(1:9,v/v,HEPES 20 mmol/L,pH 7.3)system with rapid response,strong anti-interference ability,large Stokes shift(203 nm),and low detection limit(7.548×10^(-7)mol/L).The results show that Hg^(2+)triggered elimination of TPE-Hg lead to releasing of an AIE-active compound 2 is responsible to the sensing mechanism.TPE-Hg is applicable to detect Hg^(2+)in actual water samples and image Hg^(2+)in living MCF-7 cells.In addition,TPE-Hg is suitable to assay the Hg^(2+)level in seafood and tea samples,and it is alsoapplicable intest strips.展开更多
Compared with visible light,near infrared(NIR)light has deeper penetration in biological tisues.Three-photon fuorescence microscopy(3PFM)can effectively utilize the NIR excitation to obtain high-contrast images in the...Compared with visible light,near infrared(NIR)light has deeper penetration in biological tisues.Three-photon fuorescence microscopy(3PFM)can effectively utilize the NIR excitation to obtain high-contrast images in the deep tisue.However,the weak three photon fluorescence signals may be not well presented in the traditional fuorescence intensity imaging mode.Fluorescence lifetime of certain probes is insensitive to the intensity of the excitation laser.Moreover,fluorescence lifetimne imaging microscopy(FLIM)can detect weak signals by utilizing time correlated single photon counting(TCSPC)technique.Thus,it would be an improved strategy to combine the 3PFM imaging with the FLIM together.Herein,DCDPP-2TPA,a novel agegation-induced emission luminogen(AIEgen),was adopted as the fluorescent probes.The three-photon absorption cros-section of the AlEgen,which has a deep-red fluorescence emission,was proved to be large.DCDPP-2TPA nanoparticles were synthesized,and the three photon fluorescence lifetime of which was measured in water.Moreover,in vrivo thre-photon fuorescence lifetime microscopic imaging of a craniotomy mouse was conducted via a home made optical system.High contrast cerebrovascular images of different vertical depths were obtained and the maximun depth was about 600 pumn.Even reaching the depth of 600 pum,tiny capillary vessels as small as 1.9 pum could still be distinguished.The three photon fuorescence lifetimes of the capillaries in some representative images were in accord with that of DCDPP-2TPA nanoparticles in water.A vivid 3D reconstruction was further organized to present a wealth of lifetime information.In the future,the combination strategy of 3PFM and FLIM could be further applied in the brain functional imaging.展开更多
The development of solid-state smart materials, in particular those showing photoresponsive luminescence, is highly desirable for their cutting edge applications in displays, sensors, data-storage, and anticounterfeit...The development of solid-state smart materials, in particular those showing photoresponsive luminescence, is highly desirable for their cutting edge applications in displays, sensors, data-storage, and anticounterfeiting. However, to achieve both excellent photoresponsive performance and bright luminescence in solid state remains challenge. Herein, we integrate a novel photochromic fluorophore YL into flexible polymer chains, thereby enabling the resultant polymer PYL with reversible photoisomerization upon aggregation. Remarkably, the polymer PYL possesses excellent photochromic properties and aggregationinduced emission(AIE) activity, which can be attributed to the photoactive YL moiety. Upon light exposure, its film exhibits reversibly off-to-on fluorescent modulation with quick response, high emission efficiency and signal contrast, sharply different from the weak emission in solution. The novel photoresponsive AIE polymer with invisible/visible color and fluorescence transformation allows for advanced anti-counterfeiting applications. This work provides an efficient platform for constructing solid-state photocontrollable luminescent materials.展开更多
Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-viny...Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-vinylene)(u-COPV)suspended by the truxene skeleton,the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission(AIE)accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation.In particular,the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.展开更多
It is found that the fluorescence of aliphatic poly（amido amine）s including linear and hyperbranched ones can be dramatically enhanced by simple aggregation of polymer chains, attributing to the formation of a varie...It is found that the fluorescence of aliphatic poly（amido amine）s including linear and hyperbranched ones can be dramatically enhanced by simple aggregation of polymer chains, attributing to the formation of a variety of intra- and interchain clusters with shared lone-pair electrons and the restriction of intramolecular motions. Thanks to the combination of strong solid fluorescence and excellent biocompatibility, these non-conjugated polymers become promising candidates for bioimaging such as bacterial detection. This finding not only extends the aggregation-induced emission（AIE） systems from conjugated compounds to non-conjugated materials, which expands the bioapplication range of AIE systems, but also sheds light on the exploration of novel unconventional luminogens.展开更多
基金supported in part by MEXT/JSPS KAK-ENHI grants 23H02036(G.K.)JP23H04631,JP23K26670,JP23H03833,JP24K01471,JP24K01515(K.M.)+8 种基金JP23K01977,JP23K20039,JP25K01678(K.O.)24K08341(S.S.)Toyota Riken Scholar(K.M.)the Yoshida Aca-demic and Educational Promotion Foundation(K.M.)the Environment Research and Technology Development Fund(grant number 3RA-2502)of the Environmental Restoration and Conservation Agency provided by Ministry of the Environment of Japan(K.M.)Kyushu University Platform of Inter-/Transdisciplinary Energy Research(Q-PIT)Module-Research Program(K.M.)Kyushu University Integrated Initiative for Designing Future Society(K.M.)JST SPRING,Grant Number JPMJSP2180(T.T.)Network Joint Research Center for Materials and Devices(20253036)(K.I.)The Creative Research Encouragement Award,School of Materials and Chemical Technology,Institute of Science Tokyo(G.K.)。
文摘Aggregation-induced emission luminogens(AIEgens)are typically largeπ-conjugated molecules,but their low affinity and noninvasiveness toward analytes limit practical applications.To address this,smaller,more planar AIEgens are needed.Stilbene,though structurally suitable,lacks visible luminescence.Here,we report a minimally modified stilbene-based AIEgen-4-dipropylamino-4'-cyano-bridged stilbene(DpCBS[7])-that exhibits fluorescence solvatochromism and efficient AIE across a broad polarity range in the visible region.DpCBS[7]exhibits low quantum yields(Φ_(fl)=0.010.04)in solvents from nonpolar n-hexane to polar dimethyl sulfoxide,with large Stokes shifts,viscosity-sensitive luminescence,and highly efficient solid-state luminescence(Φ_(fl)=0.70).To elucidate its dual solvatochromic and AiE behavior,femtosecond transient absorption spectroscopy was conducted.In solution,DpCBS[7]displays transient absorption with lifetimes of 21 ps(toluene)and 56 ps(acetonitrile)at 293 K,indicating ultrafast nonradiative decay leading to low Φ_(fl).Arrhenius analysis over the temperature range of 263-313 K revealed activation energies(ΔE_(a))of 9.90kJ/mol in toluene and 12.8 kJ/mol in acetonitrile for the S_(1)→S_(0) decay of DpCBS[7].The ΔE_(a) values show no clear systematic dependence on solvent polarity.In contrast,pre-exponential factor A remains consistently high regardless of solvent polarity,indicating that the striking photophysical response is governed primarily by the pre-exponential factor rather than by modulation of the activation energy.These findings highlight the fundamental importance of tailoring the distribution function through structural modification as a robust strategy to control AiE characteristics.
基金supported by the National Natural Science Foundation of China(82572410,22405063,32300048,22307080)Guangdong Basic and Applied Basic Research Foundation(2023A1515110122,2024A1515010677,2024A1515012842,2024A1515012577)+3 种基金Characteristic Innovation Project of Guangdong Province General University(2024KTSCX166,2024KTSCX168)State Key Laboratory of Pathogenesis,Prevention and Treatment of High Incidence Diseases in Central Asia Fund(SKL-HIDCA-2024-GJ3)Clinical and Basic Science&Technology Innovation Special Project of Guangdong Medical University(GDMULCJC2024161,GDMULCJC2024120)Guangdong Medical University Undergraduate Innovation and Entrepreneurship Education Base Project(JDXM2024042).
文摘Ionic phototheranostic agents have found extensive application in preclinical and clinical practice owing to their excellent biocompatibility and synergistic diagnostic-therapeutic integration.However,they still suffer from certain limitations,such as short absorption/emission wavelengths,poor photostability,aggregation-caused fluorescence self-quenching,and diminished phototherapeutic efficacy upon aggregation,which collectively hinder their efficacy in complex clinical scenarios.To address these challenges,a second near-infrared(NIR-II)ionic phototheranostic agent,namely DT-BT-BIn,is rationally designed and synthesized via an innovative dual-acceptor engineering strategy.DT-BT-BIn ingeniously integrates benzothiadiazole and benzo[c,d]indolium as dual-acceptor units,which successfully achieves superior aggregation-induced NIR-II emission characteristics,highly efficient Type Ⅰ/Ⅱ photodynamic activity coupled with photothermal effect,and excellent photostability.Moreover,the self-assembled DT-BT-BIn nanoprobes(NPs)can be effectively internalized by cancer cells in vitro.Under irradiation,DT-BT-BIn NPs are capable of disrupting mitochondrial membrane potential,thereby inducing apoptotic cell death.Furthermore,in vivo investigations demonstrate DT-BT-BIn NPs can effectively accumulate at tumor location,enabling NIR-II fluorescence/photothermal imaging-guided precise tumor ablation,while simultaneously maintaining favorable biosafety toward normal tissues.Collectively,this study underscores the considerable promise of the dual-acceptor strategy in constructing high-performance NIR-II ionic phototheranostic agents and provides a new avenue for clinical precision cancer phototherapy.
基金support from the National Key R&D Program of China(2023YFA0913902)the National Natural Science Foundation of China(32088101,22074140,and 22474136)the Dalian Institute of Chemical Physics,Chinese Academy of Sciences(DICP-I202316).
文摘Golgi apparatus(GA)-associated secretome runs through the endomembrane system and is critical for inter-and intracellular communication networks.However,achieving in situ dissection of the GA-associated secretome remains challenging owing to the scarcity of specific labeling methods.This work develops an aggregation-induced emission(AIE)luminogen-mediated photocatalytic proximity labeling strategy that allows profiling of the GA-associated secretome with high spatiotemporal precision.Leveraging an AIE luminogen-derived GA-targeting photocatalyst,this strategy achieves efficient labeling of proteins in minutes within the Golgi lumen upon light activation,which enables spatiotemporally resolved modification of histidine and tyrosine residues.We succeed in profiling secretome in both living HeLa cells and hard-to-transfect macrophage HMC3 cells,and a significant subset of GA-associated secretome with 80%specificity is determined,linking the distinct GA-associated secretory profiles to cellular characteristics.The method is further applied to proteome mapping of brain and bone metastatic lung cancer cells,which reveals the underlying roles the GA-associated secretome plays in extracellular matrix organization during metastasis.This work delivers a robust tool to break the dilemma of chemical labeling of GA-associated secretome in living cells,and provides mechanistic insights into secretion regulation at the subcellular level.
基金supported by the National Natural Science Foundation of China(No.22431004)Fund of Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates(No.2023B1212060003)。
文摘Aggregation-induced emission(AIE)polymers have been extensively studied;however,the integration of AIE units into polyelectrolytes remains largely limited by the laborious multistep synthesis of pre-designed emissive monomers.Herein,we report a one-pot multicomponent polymerization method that directly produces main-chain charged polyelectrolytes with intrinsic AIE characteristics from non-emissive building blocks.By optimizing the monomer structures and reaction conditions,a series of soluble high-molecular-weight polymers with welldefined backbones were obtained in high yields.The resulting polyelectrolytes displayed robust AIE behavior,exhibiting fluorescence enhancement up to about 60-fold in an aqueous environment,and maintained excellent thermal stability.Owing to their cationic backbones,these polymers interact strongly with microbial surfaces and exhibit remarkable antimicrobial activities.This study establishes a synthetically efficient route to AIE polyelectrolytes and highlights their potential applications as multifunctional materials for bioimaging,antimicrobial therapy,and other applications.
基金supported by the Fundamental Research Funds for Central Universities(No.30922010811).
文摘It is important to understand the evolution of the matter on the polymer membrane surface.The in situ and real-time monitoring of the membrane surface will not only favor the investigation of selective layer formation but can also track the fouling process during operation.Herein,an aggregation-induced emission(AIE)-active polymer membrane was prepared by the interfacial polymerization of a cyclodextrin-based glycocluster(CD@Glucose)and a tetraphenylethylene derivative modified with boronic acid groups(TPEDB)on the surface of a polyacrylonitrile(PAN)ultrafiltration membrane.This interfacial polymerization method can be stacked layer-by-layer to regulate the hydrophilicity and pore structure of the membrane.With the increase in the number of polymer layers,the separation and antifouling properties of the membrane gradually improved.Owing to the AIE property of the crosslinking agent TPEDB,the occurrence of interfacial polymerization and the degree of fouling during membrane operation can be monitored by the fluorescence distribution and intensity.With the aggravation of membrane fouling,the fluorescence decreased gradually,but recovered after cleaning.Therefore,this AIE effect can be used for real-time monitoring of interfacial polymerization as well as membrane fouling.
文摘In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especially for developing new reaction pathway to afford the functional heterocycle compounds with aggregation-induced emission(AIE)property has been rarely reported.In present work,the multi-site functionalization of in situ generated alkenes with indoles has been developed for the synthesis of diversely functionalized carbazoles through the synergistic construction of multiple C–C bonds and C=O bond.A proposed reaction sequence involving C–H alkenylation/radical oxygen atom transfer/Diels-Alder cycloaddition/dehydrogenative aromatization was supported by experiments and density functional theory calculations.Further derivative carbazole-linked-quinoxaline skeletons represent a class of AIEgens with acceptor-donor-acceptor configuration,which generated the desired twisted intramolecular charge transfer(TICT)AIE properties and could be used as fluorescent probes for detecting the micrometer-sized phase separation of polymer blends.The protocol provides a concise route for the synthesis and application of carbazole-based AIE luminogens.
基金the National Natural Science Foundation of China(Nos.82272067,81974386,22107123 and M-0696)the Natural Science Foundation of Hunan Province(Nos.2021JJ41008,2022JJ80052,2022JJ40656,2023JJ20077)+2 种基金the Key Project of Changsha Science and Technology Plan(No.kh2201059)the Scientific Research Project of Health Commission of Hunan Province(No.B202313057213)the Youth Science Foundation of Xiangya Hospital(No.2022Q16).
文摘Carbon monoxide(CO)is a crucial gaseous signaling molecule that regulates various physiological and pathological processes,and may exert an anti-inflammatory and protective role in drug-induced liver injury(DILI).Despite this,understanding the exact relationship between CO and the occurrence and development of DILI remains challenging.Hence,there is an urgent need to develop a reliable and robust tool for the rapid visual detection and assessment of CO in this context.Herein,we presented a novel near-infrared(NIR)fluorescent nanoprobe with aggregation-induced emission(AIE)properties and excited-state intramolecular proton transfer(ESIPT)characteristics for the detection and imaging of CO both in vitro and in vivo.Simultaneously,the nanoprobe enables self-assembly form nanoaggregates in aqueous media with high biocompatible,which can sense CO in situ through the conversion of yellowto-red fluorescence facilitated aggregation-induced dual-color fluorescence.What is more,this nanoprobe shows ratiometric respond to CO,which demonstrates excellent stability,high sensitivity(with a detection limit of 12.5 nmol/L),and superior selectivity.Crucially,this nanoprobe enables the visual detection of exogenous and endogenous CO in living cells and tissues affected by DILI,offering a user-friendly tool for real-time visualization of CO in living system.Hence,it holds great promise in advancing our understanding of CO’s role.
基金supported by the National Natural Science Foundation of China(22177094)the Fundamental Research Funds for the Central Universities(YJ202419).
文摘With increasing drug resistance,Candida infections have posed serious threats to public health.Photodynamic therapy harnesses light to destroy pathomycete,providing a smart strategy for combating of Candida infections.However,due to lack of organelle targeting ability and bad extracellular polymeric substances penetrability,current photosensitizers(PSs)are far from desirable to clean biofilms and fight against drug resistance.Herein,a mitochondrion targeting aggregationinduced emission PS,LIQ-TPA-TZ,was developed for the efficient photodynamic treatment of oral Candida infection.LIQ-TPA-TZ has good singlet oxygen and hydroxyl radical generation ability,which can efficiently kill the Candida guilliermondii(C.guilliermondii)and eradicate the biofilm.It not only causes mitochondrial damage by disruption of mitochondrial respiratory chain and oxidative stress-related gene but also inhibits fungal adhesion and filamentous growth to prevent Candida colonization,mycelia growth and biofilm formation,which is favorable for eliminating the potential drug resistance.In the mouse oropharyngeal Candida biofilm infection model,LIQ-TPA-TZ significantly eliminates infection,alleviates inflammation,and accelerates mucosal defect healing.This study provides a favorable strategy for confronting drug resistance,which may be a potential Candidate for the treatment of Candida infection.
基金Supported by The Science and Technology Program of Gansu Province,No.23JRRA1015.
文摘Aggregation-induced emission(AIE)is a phenomenon characterized by certain fluorescent molecules that exhibit weak or no luminescence in solution but demonstrate significantly enhanced luminescence upon aggregation.Accordingly,AIE materials have successfully addressed the limitations associated with aggregation-caused quenching effects and have made significant progress in the application of various fields of medicine in recent years.At present,the application of AIE materials in gastrointestinal(GI)diseases is mainly in GI imaging,diagnosis and treatment.In this review,we summarize the applications of AIE materials in GI pathogens and GI diseases,including inflammatory bowel disease and GI tumors,and outline combined treatment methods of AIE materials in GI tumor therapy.
基金supported by the funding from Natural Science Foundation of Jilin Province(No.20220101191JC)National Natural Science Foundation of China(No.22175033)the 13th Five-Year Program for Science and Technology of Education Department of Jilin Province(No.JJKH20230800KJ)。
文摘Fluorescence imaging-guided photodynamic therapy holds great promise for application in precise cancer diagnosis and treatment,which has motivated high requirements for phototheranostic agents.However,current photosensitizers(PSs)generally face limitations such as short emission wavelength and inadequate reactive oxygen species(ROS)production.Aggregation-caused quenching issue also hinders the phototheranostic efficiency of PSs.Herein,theπ-bridge modulation strategy is proposed to construct ionic PSs with enhanced bioimaging and therapeutic outcomes.Two donor-π-acceptor(D-π-A)molecules TPCPY and TFCPY were obtained by incorporating phenyl and furan units asπ-bridge,respectively.Both PSs feature aggregation-induced near-infrared emission.Under light irradiation,TPCPY and TFCPY can produce both typeⅠandⅡROS.Introducing furan ring in TFCPY enhances the ROS generation capacity by typeⅠphotosensitization process,which is consistent with the reduced energy gap between singlet and triplet states from theoretical calculation.Furthermore,TFCPY can achieve quick cellular uptake,accumulate in mitochondria,and then efficiently kill cancer cells,which is superior to TPCPY.Consequently,TFCPY exhibited good antitumor outcomes and excellent in vivo fluorescence imaging ability.This work provides an efficient molecular engineering of introducing heterocycles into the D-π-A skeleton to develop high-performance PSs with both typeⅠandⅡROS generation.
基金supported by National Natural Science Foundation of China(NSFC,No.22371289).
文摘Photodynamic therapy(PDT)has received much attention in recent years.However,traditional photosensitizers(PSs)applied in PDT usually suffer from aggregation-caused quenching(ACQ)effect in H_(2)O,single and inefficient photochemical mechanism of action(MoA),poor cancer targeting ability,etc.In this work,two novel Ru(II)-based aggregation-induced emission(AIE)agents(Ru1 and Ru2)were developed.Both complexes exhibited long triplet excited lifetimes and nearly 100%singlet oxygen quantum yields in H_(2)O.In addition,Ru1 and Ru2 displayed potent photo-catalytic reduced nicotinamide adenine dinucleotide(NADH)oxidation activity with turnover frequency(TOF)values of about 1779 and 2000 h^(−1),respectively.Therefore,both Ru1 and Ru2 showed efficient PDT activity towards a series of cancer cells.Moreover,Ru2 was further loaded in bovine serum albumin(BSA)to enhance the tumor targeting ability in vivo,and the obtained Ru2@BSA could selectively accumulate in tumor tissues and effectively inhibit tumor growth on a 4T1 tumor-bearing mouse model.So far as we know,this work represents the first report about Ru(Ⅱ)-)AIE agents that possess high singlet oxygen quantum yields and also potent photocatalytic NADH oxidation activity,and may provide new ideas for rational design of novel PSs with efficient PDT activity.
基金support from the National Natural Science Foundation of China(9235630033,22105069)Shanghai Pujiang Program(20PJ1402900)+2 种基金Shanghai Natural Science Foundation(21ZR1418400)Innovation Program of Shanghai Municipal Education Commission(2023FGS01)Natural Science Foundation of Jiangsu Province(BK20231225).
文摘Icing detection is critically important for preventing safety accidents and economic losses,especially concerning ice formation from invalidated anti-icing fluids(water and ethylene glycol)under extreme conditions.Traditional technologies like ultrasonics and capacitor-antenna face challenges with limited detection areas,lower accuracy,and susceptibility to electromagnetic interference.Here,we introduce a novel viscosity-ultrasensitive fluorescent probe 40,4‴-(2,2-diphenyle-thene-1,1-diyl)bis-(3,5-dicarboxylate)(TPE-2B4C)based on AIEgens for moni-toring ice formation of anti-icing fluids in low-temperature environments.TPE-2B4C,consisting of four sodium carboxylate groups and multiple freely rotating benzene rings,demonstrates outstanding solubility in anti-icing fluids and exhibits no fluorescent background signal even at low temperatures(<−20°C).Upon freezing,TPE-2B4C relocates from the water phase to higher viscosity ethylene glycol,causing restriction of benzene rings and a significantly increased green fluorescence signal.TPE-2B4C can successfully determine whether the anti-icing fluids are icing from−5 to−20°C with a high contrast ratio.Due to its simple setup,fast operation,and broad applicability,our new method is anticipated to be employed for rapid,real-time,and large-scale icing detection.
基金financially supported by the National Natural Science Foundation of China (Nos. 21822102, 21774034, 21490573, 21490574, and 21788102)the Natural Science Foundation of Guangdong Province (Nos. 2016A030306045 and 2016030312002)the Innovation and Technology Commission of Hong Kong (No. ITC-CNERC14SC01)
文摘Hyperbranched polymer with highly branched three-dimensional topological structure, a large number of end groups, and multifaceted functionalities have gained much attention, while polymers with aggregation-induced emission(AIE) properties become a group of popular luminescent materials recently. The design and synthesis of AIE-active hyperbranched polymers, which combine the advantages of these two types of materials, are attractive but challenging. In this work, four hyperbranched poly(tetrahydropyrimidine)s were synthesized from the metal-free room temperature multicomponent tandem polymerization of diester group-activated internal alkyne,polyfunctional aromatic amines, and formaldehyde in methanol under the catalysis of acetic acid. Through different monomer combination and controlling the monomer loading order, hyperbranched polymers with various topological structures as well as sequences of different functional groups in the polymer backbone were obtained with high molecular weights(up to 3.0 × 10~4 g/mol) in high yields(up to 98%). The hyperbranched poly(tetrahydropyrimidine) emitted faintly in solution, while its luminescence was notably enhanced in the aggregated state, suggesting its typical aggregation-induced emission property. It is anticipated that the multicomponent polymerization may provide a synthetic platform for the construction of hyperbranched polyheterocycles with diverse structures and functionalities.
基金financially supported by the National Natural Science Foundation of China(Nos.21878136,21372194 and 21773103)。
文摘Aggregation-induced emission(AIE) active photochromic molecules have attracted growing attention for their versatile applications.Here we designed and synthesized five newly unsymmetrical photochromic diarylethene(DAE) dyads(BTE1-5) by connecting tetraphenylethene(TPE) and aromatic substituent via bithienylethene(BTE) bridge.The chemical structures of those compounds were identified by ^1H NMR,^(13)C NMR and HRMS.The absorption and emission of these dyads were investigated by UV-vis and fluore scence spectroscopy,respectively.The results showed that all those compounds exhibited typically AIE or aggregation-induced emission enhancement(AIEE) characteristic.Particularly,when an aggregationcaused quenching(ACQ) fluorophore(triphenylamine) was grafted to the molecule,connecting with TPE via BTE-bridge,the ACQ phenomenon was dissipated and converted to an AIE luminophore,and those compounds exhibited photochromism upon irradiation with alternative UV and visible light.The solution or solid of those compounds showed distinctly fluorescence switching "ON" or "OFF" observation upon irradiation with alternative UV and visible light.It is interesting that BTE1 could be applied in recording and rewritable information storage,and the cyclization quantum yields could be affected by substituent significantly.
基金financial support from National Research Foundation Investigatorship (R279-000-444-281)National University of Singapore (R279-000-482-133)
文摘Photodynamic therapy(PDT) employs accumulation of photosensitizers(PSs) in malignant tumor tissue followed by the light-induced generation of cytotoxic reactive oxygen species to kill the tumor cells. The success of PDT depends on optimal PS dosage that is matched with the ideal power of light. This in turn depends on PS accumulation in target tissue and light administration time and period.As theranostic nanomedicine is driven by multifunctional therapeutics that aim to achieve targeted tissue delivery and image-guided therapy, fluorescent PS nanoparticle(NP)accumulation in target tissues can be ascertained through fluorescence imaging to optimize the light dose and administration parameters. In this regard, zebrafish larvae provide a unique transparent in vivo platform to monitor fluorescent PS bio-distribution and their therapeutic efficiency. Using fluorescent PS NPs with unique aggregation-induced emission characteristics, we demonstrate for the first time the real-time visualization of polymeric NP accumulation in tumor tissue and, more importantly, the best time to conduct PDT using transgenic zebrafish larvae with inducible liver hyperplasia as an example.
基金funded by the National Natural Science Foundation of China(Nos.22278038,21878023),the Program for Distinguished Professor of Liaoning Province.
文摘Detection of mercury ions(Hg^(2+))in actual samples is of significant importance due to the toxicity of Hg^(2+)to human health.In this work,a simple tetraphenylethene(TPE)derived fluorescent probe TPE-Hg based on aggregation-induced emission(AIE)mechanism was synthesized.TPE-Hg can visually recognize Hg^(2+)in THF/HEPES(1:9,v/v,HEPES 20 mmol/L,pH 7.3)system with rapid response,strong anti-interference ability,large Stokes shift(203 nm),and low detection limit(7.548×10^(-7)mol/L).The results show that Hg^(2+)triggered elimination of TPE-Hg lead to releasing of an AIE-active compound 2 is responsible to the sensing mechanism.TPE-Hg is applicable to detect Hg^(2+)in actual water samples and image Hg^(2+)in living MCF-7 cells.In addition,TPE-Hg is suitable to assay the Hg^(2+)level in seafood and tea samples,and it is alsoapplicable intest strips.
基金supported by National Natural Science Foundation of China(61735016)Zhejiang Provincial Natural Science Foundation of China(LR17F050001).
文摘Compared with visible light,near infrared(NIR)light has deeper penetration in biological tisues.Three-photon fuorescence microscopy(3PFM)can effectively utilize the NIR excitation to obtain high-contrast images in the deep tisue.However,the weak three photon fluorescence signals may be not well presented in the traditional fuorescence intensity imaging mode.Fluorescence lifetime of certain probes is insensitive to the intensity of the excitation laser.Moreover,fluorescence lifetimne imaging microscopy(FLIM)can detect weak signals by utilizing time correlated single photon counting(TCSPC)technique.Thus,it would be an improved strategy to combine the 3PFM imaging with the FLIM together.Herein,DCDPP-2TPA,a novel agegation-induced emission luminogen(AIEgen),was adopted as the fluorescent probes.The three-photon absorption cros-section of the AlEgen,which has a deep-red fluorescence emission,was proved to be large.DCDPP-2TPA nanoparticles were synthesized,and the three photon fluorescence lifetime of which was measured in water.Moreover,in vrivo thre-photon fuorescence lifetime microscopic imaging of a craniotomy mouse was conducted via a home made optical system.High contrast cerebrovascular images of different vertical depths were obtained and the maximun depth was about 600 pumn.Even reaching the depth of 600 pum,tiny capillary vessels as small as 1.9 pum could still be distinguished.The three photon fuorescence lifetimes of the capillaries in some representative images were in accord with that of DCDPP-2TPA nanoparticles in water.A vivid 3D reconstruction was further organized to present a wealth of lifetime information.In the future,the combination strategy of 3PFM and FLIM could be further applied in the brain functional imaging.
基金financially supported by the National Natural Science Foundation of China for Science Center Program (No. 21788102)Creative Research Groups (No. 21421004)+4 种基金Key Project (No. 21636002)Shanghai Pujiang Program (No. 20PJ1402900)National key Research and Development Program (No. 2016YFA0200300)Shanghai Municipal Science and Technology Major Project (No. 2018SHZDZX03)Program of Introducing Talents of Discipline to Universities (No. B16017)。
文摘The development of solid-state smart materials, in particular those showing photoresponsive luminescence, is highly desirable for their cutting edge applications in displays, sensors, data-storage, and anticounterfeiting. However, to achieve both excellent photoresponsive performance and bright luminescence in solid state remains challenge. Herein, we integrate a novel photochromic fluorophore YL into flexible polymer chains, thereby enabling the resultant polymer PYL with reversible photoisomerization upon aggregation. Remarkably, the polymer PYL possesses excellent photochromic properties and aggregationinduced emission(AIE) activity, which can be attributed to the photoactive YL moiety. Upon light exposure, its film exhibits reversibly off-to-on fluorescent modulation with quick response, high emission efficiency and signal contrast, sharply different from the weak emission in solution. The novel photoresponsive AIE polymer with invisible/visible color and fluorescence transformation allows for advanced anti-counterfeiting applications. This work provides an efficient platform for constructing solid-state photocontrollable luminescent materials.
基金the National Natural Science Foundation of China(Nos.22101267,21672192,21803059,U2004191,U1904212,21801063)for financial support。
文摘Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxenepended base ligands.Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(pphenylene-vinylene)(u-COPV)suspended by the truxene skeleton,the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission(AIE)accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation.In particular,the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.
基金financially supported by the National Basic Research Program(No.2015CB931801)the National Natural Science Foundation of China(Nos.21204049 and 51473093)
文摘It is found that the fluorescence of aliphatic poly（amido amine）s including linear and hyperbranched ones can be dramatically enhanced by simple aggregation of polymer chains, attributing to the formation of a variety of intra- and interchain clusters with shared lone-pair electrons and the restriction of intramolecular motions. Thanks to the combination of strong solid fluorescence and excellent biocompatibility, these non-conjugated polymers become promising candidates for bioimaging such as bacterial detection. This finding not only extends the aggregation-induced emission（AIE） systems from conjugated compounds to non-conjugated materials, which expands the bioapplication range of AIE systems, but also sheds light on the exploration of novel unconventional luminogens.
