ORCID Profile
0000-0001-7309-2506
Current Organisation
Zhejiang University
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Publisher: American Chemical Society (ACS)
Date: 27-05-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0MH01251C
Abstract: ICT-type AIEgens with twisted conformations are ideal candidates for high-contrast mechanochromic luminogens under external force.
Publisher: American Chemical Society (ACS)
Date: 12-11-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0QM00754D
Abstract: Changes of molecular conformation in the solid state play a vital role in many advanced technologies.
Publisher: Springer Science and Business Media LLC
Date: 24-06-2023
DOI: 10.1038/S41467-023-39479-1
Abstract: Proximity effect, which refers to the low-lying ( n ,π*) and (π,π*) states with close energy levels, usually plays a negative role in the luminescent behaviors of heterocyclic luminogens. However, no systematic study attempts to reveal and manipulate proximity effect on luminescent properties. Here, we report a series of methylquinoxaline derivatives with different electron-donating groups, which show different photophysical properties and aggregation-induced emission behaviors. Experimental results and theoretical calculation reveal the gradually changed energy levels and different coupling effects of the closely related ( n ,π*) and (π,π*) states, which intrinsically regulate proximity effect and aggregation-induced emission behaviors of these luminogens. With the intrinsic nature of heterocycle-containing compounds, they are utilized for sensors and information encryption with dynamic responses to acid/base stimuli. This work reveals both positive and negative impacts of proximity effect in heterocyclic aggregation-induced emission systems and provides a perspective to develop functional and responsive luminogens with aggregation-induced emission properties.
Publisher: American Chemical Society (ACS)
Date: 04-12-2020
Publisher: Wiley
Date: 03-08-2022
Abstract: Dynamic patterns based on luminescent materials play an essential role in the digital age. However, it is still challenging to develop highly emissive photofluorochromic materials with dynamic behaviors to store information with multiple characteristics. Here, we report a series of dihydroazulene‐based compounds which show typical aggregation‐induced emission (AIE) effect. Moreover, the photo‐switching ability of the dihydroazulene units, undergoing light‐induced ring‐opening, enables photofluorochromic properties. The photofluorochromism also shows quantitively described responses to time and temperature via a reverse ring‐closing process. Ultimately, a rewritable 4D information system, embedded with a quick response code, dot matrix with microstructures, color matrix of fluorescence, and time/temperature‐dependent intensity change, is established with dynamic patterns. This work not only develops a dynamic AIE skeleton with photofluorochromic properties but also provides a new strategy for information encryption and cybernetics.
Publisher: American Chemical Society (ACS)
Date: 06-06-2019
Publisher: Wiley
Date: 17-06-2021
Abstract: The unique advantages and the exciting application prospects of AIEgens have triggered booming developments in this area in recent years. Among them, stimuli‐responsive AIEgens have received particular attention and impressive progress, and they have been demonstrated to show tremendous potential in many fields from physical chemistry to materials science and to biology and medicine. Here, the recent achievements of stimuli‐responsive AIEgens in terms of seven most representative types of stimuli including force, light, polarity, temperature, electricity, ion, and pH, are summarized. Based on typical ex les, it is illustrated how each type of systems realize the desired stimuli‐responsive performance for various applications. The key work principles behind them are ultimately deciphered and figured out to offer new insights and guidelines for the design and engineering of the next‐generation stimuli‐responsive luminescent materials for more broad applications.
Publisher: American Chemical Society (ACS)
Date: 21-04-2022
DOI: 10.1021/JACS.2C02381
Abstract: Electronic conjugation through covalent bonds is generally considered as the basis for the electronic transition of organic luminescent materials. Tetraphenylethylene (TPE), an efficient fluorophore with aggregation-induced emission character, fluoresces blue emission in the aggregate state, and such photoluminescence is always ascribed to the through-bond conjugation (TBC) among the four phenyl rings and the central C═C bond. However, in this work, systematic spectroscopic studies and DFT theoretical simulation reveal that the intramolecular through-space interaction (TSI) between two vicinal phenyl rings generates the bright blue emission in TPE but not the TBC effect. Furthermore, the evaluation of excited-state decay dynamics suggests the significance of photoinduced isomerization in the nonradiative decay of TPE in the solution state. More importantly, different from the traditional qualitative description for TSI, the quantitative elucidation of the TSI is realized through the atoms-in-molecules analysis meanwhile, a theoretical solid-state model for TPE and other multirotor systems for studying the electronic configuration is preliminarily established. The mechanistic model of TSI delineated in this work provides a new strategy to design luminescent materials beyond the traditional theory of TBC and expands the quantum understanding of molecular behavior to the aggregate level.
Publisher: American Chemical Society (ACS)
Date: 11-12-2018
Abstract: Many highly ordered structures with smart functions are generated by self-assembly with stimuli responsiveness. Despite that electron microscopes enable us to directly observe the end products, it is hard to visualize the initial step and the kinetic stimuli-responsive behavior of self-assembly. Here, we report the design and synthesis of stereogenic hiphiles, namely, ( Z)-TPE-OEG and ( E)-TPE-OEG, with aggregation-induced emission (AIE) characteristics from the hydrophobic tetraphenylethene core and thermoresponsive behavior from the hydrophilic oligoethylene glycol monomethyl ether chain. The two isomers can be easily isolated by high-performance liquid chromatography and characterized by 2D NMR spectroscopy. While ( Z)-TPE-OEG self-assembles into vesicles, its ( E)-cousin forms micelles in water. The initial step of their self-assembly processes can be visualized based on AIE characteristics, with a sensitivity much higher than the method based on transmittance measurement. The entrapment and release capabilities of the ( Z)-stereogenic hiphile are demonstrated by employing pyrene as a guest. The thermoresponsive behavior of the ( Z)- hiphile results in its continuous phase transition from microscopic self-assembly to macroscopic aggregation, which is successfully visualized in situ by confocal laser scanning microscopy accompanied by the AIE technique. Such a kinetic process shows different stages according to the microscopic visualization, and these stages have never been monitored through roughly observing the appearance of precipitates. It is anticipated that this study can deepen the understanding of the self-assembly processes for better monitoring and controlling them in different systems.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3DT02522E
Publisher: American Chemical Society (ACS)
Date: 08-02-2018
Abstract: Luminescent molecules with aggregation-induced emission (AIE) property or AIE-active luminogens (AIE-gens) are typical stimuli-responsive materials. Many AIE-gens have shown luminescent responses to mechano-, thermo-, electro-, vapo-, and/or solvato-stimulus, but the detailed structure-property relationship has been addressed for only a few of them. Here, we report a tetraphenylethene (TPE) derivative with pyridyl modifiers and ethynylene bridges. The (Z)- and (E)-isomers are clearly purified, and both of them are AIE-active and demonstrate multiple luminescent responses to external stimuli. Distinct from other reported TPE derivatives, the two isomers show negative solvatochromism due to the large dipole in the ground electronic state. By correlating with the single crystal structures, the subtle differences in quantum efficiency and emission peak wavelength of the solids of the (Z)- and (E)-isomers are rationally explained. Moreover, the ground powder of the (E)-isomer can recover its emission color from green to blue in the air at room temperature but the (Z)-isomer cannot. This difference is interpreted by a mechanism of water-triggered conformational variation, which depends on the hydrogen bond formation between pyridyl moieties and water molecules in the air. In addition to the reversible emission color changes by cyclic grinding-fuming treatments, both of the isomers exhibit a reversible luminescent response to acid-base treatments by switching the emission color between green (basic) and yellow (acid), owing to the incorporation of pyridyl units into the molecule. The unprecedented multiple stimuli-responsive behaviors and clear mechanism explanations allow this kind of AIE-gens to be promising smart materials.
Publisher: Wiley
Date: 09-09-2020
Abstract: Aggregation‐induced emission (AIE) luminogens are an important type of advanced functional materials with fantastic optical properties and have found potential applications in organic electronics, biochemistry, and molecular imaging. Herein, this article presents a novel application of AIE luminogens (AIEgens) for efficient exfoliation of layered transition metal dichalcogenides (TMDs, such as MoS 2 and WSe 2 ). From the 1 H NMR spectroscopic analysis, the designed AIEgens can insert into the space between layers of MoS 2 in ethanol solution and the dynamic molecular rotation against the weak interactions affords large‐scale few‐layer MoS 2 nanosheets (7–8 layers) with enhanced smoothness. The 3D AIEgens play a significant role in preserving the crystal lattice of MoS 2 even at high pressure ( GPa). More importantly, the new approach can also be used for exfoliation of WSe 2 to achieve large‐scale few‐layer nanosheets. The present work thus provides a facile and high yielding synthetic method for accessing on a large scale 2D layered materials with enhanced properties for high‐technology applications.
Publisher: American Chemical Society (ACS)
Date: 27-12-2019
Abstract: To achieve super-resolution imaging in biological research using stimulated emission depletion (STED) nanoscopy, organic luminescent materials and their corresponding fluorescent nanoparticles with high brightness and photostability are of great significance. Herein, donor-acceptor-typed DBTBT-4C8 bearing flexible alkyl chains was developed, not only to afford deep-red emission from 600 to 800 nm but also to obtain high fluorescent brightness with the absolute photoluminescence quantum yields of 25%. After that, well-defined and monodispersed spherical nanoparticles using DBTBT-4C8 with bright emission, excellent biocompatibility, and photostability, which can easily mix with hipathic block polymers, were then produced for super-resolution in vitro and in vivo imaging using STED nanoscopy. The observations showed that in contrast to confocal microscopy with a full width at half-maximum (FWHM) value of ≈400 nm, superior resolution with a significantly improved FWHM value of only 100 nm was achieved in biomedical cell imaging, which was also used to reconstruct three-dimensional images of stained HeLa cells at an ultrahigh resolution. More importantly, by using the prepared fluorescent organic nanoparticles (FONPs) in STED nanoscopy, in vivo imaging in glass catfish with largely enhanced resolution was also successfully achieved, demonstrating that these developed deep-red FONPs here are highly suitable for super-resolution in vitro and in vivo imaging using STED nanoscopy.
Publisher: American Chemical Society (ACS)
Date: 07-01-2019
Publisher: American Chemical Society (ACS)
Date: 05-10-2020
DOI: 10.26434/CHEMRXIV.13046684.V1
Abstract: Fluorescence imaging in the near-infrared II (NIR-II, 1000-1700 nm) region opens up new avenues for biological systems due to suppressed scattering and low autofluorescence at longer-wavelength photons. Nonetheless, the development of organic NIR-II fluorophores is still limited mainly due to the shortage of efficient molecular design strategy. Herein, we propose an approach of designing Janus NIR-II fluorophores by introducing electronic donors with distinct properties into one molecule. As a proof-of-concept, fluorescent dye 2TT- m,o C6B with both twisted and planar electronic donors displayed balanced absorption and emission which were absent in its parent compound. The key design strategy for Janus molecule is that it combines the merits of intense absorption from planar architecture and high fluorescence quantum yield from twisted motif. The resulting 2TT- m,o C6B nanoparticles exhibit a high molar absorptivity of 1.12 ⨯10 4 M -1 cm -1 at 808 nm and a NIR-II quantum yield of 3.7%, displaying a typical aggregation-induced emission (AIE) attribute. The highly bright and stable 2TT- m,o C6B nanoparticles assured NIR-II image-guided cancer surgery to resect submillimeter tumor nodules. The present study may inspire further development of molecular design philosophy for highly bright NIR-II fluorophores for biomedical applications.
Publisher: American Chemical Society (ACS)
Date: 13-04-2021
DOI: 10.26434/CHEMRXIV.14400953.V1
Abstract: Apart from the traditional through-bond conjugation (TBC), through-space conjugation (TSC) is gradually proved as another important interaction in photophysical processes, especially for the recent observation of clusteroluminescence from nonconjugated molecules. Herein, simple and nonconjugated triphenylmethane (TPM) and its derivatives with electron-donating and electron-withdrawing groups were synthesized, and their photophysical properties were systematically studied. TPM was characterized with visible clusteroluminescence due to the intramolecular TSC. Experimental and theoretical results showed that the introduction of electron-donating groups into TPM could red-shift the wavelength and increase the efficiency of clusteroluminescence simultaneously, due to the increased electronic density and stabilization of TSC. However, TPM derivatives with electron-withdrawing groups showed inefficient or even quenched clusteroluminescence caused by the vigorous excited-state intramolecular motion and intermolecular photoinduced electron transfer process. This work provides a reliable strategy to manipulate TSC and clusteroluminescence.
Publisher: American Chemical Society (ACS)
Date: 13-03-2019
DOI: 10.1021/JACS.8B13889
Abstract: Planar donor and acceptor (D-A) conjugated structures are generally believed to be the standard for architecting highly efficient photothermal theranostic agents, in order to restrict intramolecular motions in aggregates (nanoparticles). However, other channels of extra nonradiative decay may be blocked. Now this challenge is addressed by proposing an "abnormal" strategy based on molecular motion in aggregates. Molecular rotors and bulky alkyl chains are grafted to the central D-A core to lower intermolecular interaction. The enhanced molecular motion favors the formation of a dark twisted intramolecular charge transfer state, whose nonradiative decay enhances the photothermal properties. Result shows that small-molecule NIRb14 with long alkyl chains branched at the second carbon exhibits enhanced photothermal properties compared with NIRb6, with short branched chains, and much higher than NIR6, with short linear chains, and the commercial gold nanorods. Both in vitro and in vivo experiments demonstrate that NIRb14 nanoparticles can be used as nanoagents for photoacoustic imaging-guided photothermal therapy. Moreover, charge reversal poly(β-amino ester) makes NIRb14 specifically accumulate at tumor sites. This study thus provides an excited molecular motion approach toward efficient phototheranostic agents.
Publisher: Wiley
Date: 18-12-2019
Publisher: Wiley
Date: 14-05-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9MH01909J
Abstract: Polymerization-induced emission: a chemical route for uniting nonluminescent monomers into luminescent polymers.
Publisher: AIP Publishing
Date: 08-2019
DOI: 10.1063/1.5110688
Abstract: Interfaces exist in almost all objects and processes. Investigation on the interface not only is fundamentally important but also has great application prospects. Traditionally, the interface structure is studied by electron microscopy, which cannot reflect its real structure considering the pretreated process before measurement. Monitoring the interface evolution process by these regular methods is time-consuming and unfeasible in many cases. In this perspective article, we discuss how to realize the visualizing and monitoring interface structures and dynamics by aggregation-induced emission technique, which is applicable to almost all kinds of interfaces, including gas-solid, liquid-solid, solid-solid, gas-liquid-solid, and liquid-liquid-solid. Meanwhile, it is anticipated that the circularly polarized luminescence property in prochiral aggregation-induced emission luminogens can make a great difference in this area.
Publisher: Elsevier BV
Date: 02-2022
Publisher: Wiley
Date: 04-06-2020
Publisher: American Chemical Society (ACS)
Date: 10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9PY01375J
Abstract: Ferrocene-based hb -PPTCs with redox activity are readily prepared by the catalyst-free phenylpropiolate-azide polycycloaddition. They could be used as precursors to produce nanostructured magnetoceramics upon pyrolysis.
Publisher: Springer Science and Business Media LLC
Date: 23-11-2018
DOI: 10.1038/S41467-018-07299-3
Abstract: The aggregation of molecules plays an important role in determining their function. Electron microscopy and other methods can only characterize the variation of microstructure, but are not capable of monitoring conformational changes. These techniques are also complicated, expensive and time-consuming. Here, we demonstrate a simple method to monitor in-situ and in real-time the conformational change of ( R )-1,1′-binaphthyl-based polymers during the aggregation process using circular dichroism. Based on results from molecular dynamics simulations and experimental circular dichroism measurements, polymers with “open” binaphthyl rings are found to show stronger aggregation-annihilated circular dichroism effects, with more negative torsion angles between the two naphthalene rings. In contrast, the polymers with “locked” rings show a more restrained aggregation-annihilated circular dichroism effect, with only a slight change of torsion angle. This work provides an approach to monitor molecular aggregation in a simple, accurate, and efficient way.
Publisher: Wiley
Date: 16-06-2023
Abstract: Clusteroluminescence (CL) and through‐space interactions (TSIs) of non‐conjugated molecules have drawn more attention due to their unique photophysical behaviors that are different from largely conjugated luminogens. However, achieving red and even near‐infrared (NIR) emission from such systems is still challenging due to the intrinsic drawbacks of non‐conjugated molecules and the lack of theories for structure–property relationships. In this work, six phenolic resins are designed and synthesized based on two molecule‐engineering strategies: increasing the number of TSIs units and introducing electron‐donating/‐withdrawing groups. All phenolic resins are verified as luminogens with CL property (CLgens), and the first ex le of CLgens with NIR emission (maximum emission wavelength ≥680 nm) and high absolute quantum yield (47 %) is reported. Experiments and theoretical analysis reveal that two TSIs types, through‐space locally excited state and through‐space charge transfer state, play essential roles in achieving CL from these non‐conjugated polymers, which could be manipulated via changing structural conformation and electron density or altering electron transition behaviors. This work not only provides an approach to manipulate TSIs and CL of non‐conjugated polymers but also endows commercially available phenolic resins with high practical value as luminescence materials.
Publisher: American Chemical Society (ACS)
Date: 30-10-2019
DOI: 10.1021/ACS.JPCLETT.9B02752
Abstract: The development of molecular machines has long been a dream of scientists and is expected to revolutionize many aspects of technology and medicine. As the prerequisite of a practicable molecular machine, studies on the solid-state molecular motion (SSMM) are not only of scientific importance but also practically useful. Herein, two nonconjugated molecules, 1,2-diphenylethane (
Publisher: American Chemical Society (ACS)
Date: 04-03-2021
DOI: 10.1021/JACS.1C00243
Publisher: American Chemical Society (ACS)
Date: 22-08-2019
DOI: 10.1021/JACS.9B06196
Abstract: Acrylonitriles with aggregation-induced emission (AIE) characteristics have been found to show promising applications in two-photon biomedical imaging. Generally, elaborate synthetic efforts are required to achieve different acrylonitriles with distinct functionalities. In this work, we first reported the synthesis of two different group-functionalized AIE-active acrylonitriles (TPAT-AN-XF and 2TPAT-AN) obtained simply by mixing the same reactants at different temperatures using a facile and transition metal-free synthetic method. These two AIE luminogens (AIEgens) exhibit unique properties such as bright red emission in the solid state, large Stokes shift, and large two-photon absorption cross section. Water-soluble nanoparticles (NPs) of 2TPAT-AN were prepared by a nanoprecipitation method. In vitro imaging data show that 2TPAT-AN NPs can selectively stain lysosome in live cells. Besides one-photon imaging, remarkable two-photon imaging of live tumor tissues can be achieved with high resolution and deep tissue penetration. 2TPAT-AN NPs show high biocompatibility and are successfully utilized in in vivo long-term imaging of mouse tumors with a high signal-to-noise ratio. Thus, the present work is anticipated to shed light on the preparation of a library of AIE-active functionalized acrylonitriles with intriguing properties for biomedical applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0QM00119H
Abstract: This work reports multicationic AIEgens for unimolecular photodynamic theranostics, and an investigation of the relationship between their structures and activities, including PDT performance, 2-photon bioimaging, and self-reporting characteristics.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2MH00808D
Abstract: A radical polymer without any delocalized π-stabilization was synthesized from a classical chromophore quencher, TEMPO, which surprisingly shows red emission.
Publisher: American Chemical Society (ACS)
Date: 09-04-2018
DOI: 10.1021/JACS.8B01991
Abstract: Heterocyclic polymers have gained enormous attention for their unique functionalities and wide applications. In contrast with the well-studied polymer systems with five- or six-membered heterocycles, functional polymers with readily openable small-ring heterocycles have rarely been explored due to their large synthetic difficulty. Herein, a facile one-pot multicomponent polymerization to such polymers is developed. A series of functional polymers with multisubstituted and heteroatom-rich azetidine frameworks are efficiently generated at room temperature in high atom economy from handy monomers. The four-membered azetidine rings in the polymer skeletons can be easily transformed into amide and amidine moieties via a fast and efficient acid-mediated ring-opening reaction, producing brand-new polymeric materials with distinctive properties. All the as-prepared azetidine-containing polymers exhibit intrinsic visible luminescence in the solid state under long-wavelength UV irradiation even without conventionally conjugated structures. Such unconventional luminescence is attributed to the clusteroluminogens formed by through-space electronic interactions of heteroatoms and phenyl rings. All the obtained polymers show excellent optical transparency, high and tunable refractive indices, low optical dispersions and good photopatternability, which make them promising materials in various advanced electronic and optoelectronic devices. The ring-opened polymers can also function as a lysosome-specific fluorescent probe in biological imaging.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0MH00447B
Abstract: In situ ACQ-to-AIE transformation was achieved by light-induced [2+2] cycloaddition via through-space conjugation.
Publisher: Wiley
Date: 22-10-2018
Abstract: A particular challenge in the design of organic photosensitizers (PSs) with donor-acceptor (D-A) structures is that it is based on trial and error rather than specific rules. Now these challenges are addressed by proposing two efficient strategies to enhance the photosensitization efficiency: polymerization-facilitated photosensitization and the D-A even-odd effect. Conjugated polymers have been found to exhibit a higher
Publisher: American Chemical Society (ACS)
Date: 05-03-2019
Abstract: Constructing artificial helical structures through hierarchical self-assembly and exploring the underlying mechanism are important, and they help gain insight from the structures, processes, and functions from the biological helices and facilitate the development of material science and nanotechnology. Herein, the two enantiomers of chiral Au(I) complexes ( S)-1 and ( R)-1 were synthesized, and they exhibited impressive spontaneous hierarchical self-assembly transitions from vesicles to helical fibers. An impressive chirality inversion and lification was accompanied by the assembly transition, as elucidated by the results of in situ and time-dependent circular dichroism spectroscopy and scanning electron microscope imaging. The two enantiomers could serve as ideal chiral templates to co-assemble with other achiral luminogens to efficiently induce the resulting co-assembly systems to show circularly polarized luminescence (CPL). Our work has provided a simple but efficient way to explore the sophisticated self-assembly process and presented a facile and effective strategy to fabricate architectures with CPL properties.
Publisher: American Chemical Society (ACS)
Date: 28-01-2021
Publisher: Chinese Chemical Society
Date: 14-07-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8SC01170B
Abstract: Photocyclized intermediate formation and quasi CC twisting are the dominant processes behind the AIE.
Publisher: Wiley
Date: 20-11-2019
Abstract: Supramolecular macrocyclic hosts have long been used in smart materials. However, their triplet emission and regulation at crystal level is rarely studied. Herein, ultralong and universal room-temperature phosphorescence (RTP) is reported for traditional crown ethers. A supramolecular strategy involving chain length adjustment and morphological locking through complexation with K
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0QM00877J
Abstract: We present a two-photon AIEgen, ABCXF with nonaromatic rotors (–CF 3 ), a high two-photon absorption cross-section, bright red emission in the solid-state, and remarkably high photostability for fatty liver disease diagnosis.
Publisher: American Chemical Society (ACS)
Date: 07-03-2018
Abstract: Polymers with aggregation-induced emission (AIE) characteristics have aroused tremendous interest because of their potential applications in large-area flexible display and luminescent self-assembling, and as stimuli-responsive and porous materials. However, the design of AIE-active polymers is always not as easy as that of small molecules because their properties are hard to predict. In some cases, the polymers prepared from the AIE-active monomers show the aggregation-caused quenching (ACQ) instead of AIE effect. To understand the structure-property relationship of the polymers constructed from the AIE monomers, in this paper, two pyrazine-containing AIE monomers were utilized to construct luminescent polymers by click polymerization. The photophysical property investigation indicates that the polytriazole containing tetraphenylpyrazine units is AIE-active, whereas that bearing 2,3-dicyano-5,6-diphenylpyrazine units suffers from the ACQ effect. Through systematical investigation, the cause for such difference was unveiled. Thus, this work provides a useful guidance for further design of AIE-active polymers.
Publisher: American Chemical Society (ACS)
Date: 27-08-2019
Publisher: American Chemical Society (ACS)
Date: 05-08-2020
DOI: 10.1021/JACS.0C07193
Publisher: Wiley
Date: 28-02-2019
Abstract: The development of molecular machines requires new building blocks which are easy to characterize and visualize to realize a complexity comparable to their natural counterparts such as biological enzymes. Furthermore, with the desire to build functional nanobots capable of navigating living organisms, it is necessary that the building blocks show mobility even in the solid state. Herein we report a system which is emissive in the amorphous state but is non-fluorescent in the crystalline state due to the formation of extensive π-π interactions. This dual nature could be exploited for easy visualization of its solid-state molecular rearrangement. The emission of the amorphous film was quenched as the molecules spontaneously formed π-π interactions even in the solid state. Scratching the non-emissive film destroyed the interactions and restored the emission of the film. The emission quickly disappeared with an average lifetime of 20 s as the compound reformed the π-network even at room temperature.
Publisher: American Chemical Society (ACS)
Date: 03-11-2017
DOI: 10.1021/JACS.7B08592
Abstract: π-Bonds connected with aromatic rings were generally believed as the standard structures for constructing highly efficient fluorophores. Materials without these typical structures, however, exhibited only low fluorescence quantum yields and emitted in the ultraviolet spectral region. In this work, three molecules, namely bis(2,4,5-trimethylphenyl)methane, 1,1,2,2-tetrakis(2,4,5-trimethylphenyl)ethane, and 1,1,2,2-tetraphenylethane, with nonconjugated structures and isolated phenyl rings were synthesized and their photophysical properties were systematically investigated. Interestingly, the emission spectra of these three molecules could be well extended to 600 nm with high solid-state quantum yields of up to 70%. Experimental and theoretical analyses proved that intramolecular through-space conjugation between the "isolated" phenyl rings played an important role for this abnormal phenomenon.
Publisher: American Chemical Society (ACS)
Date: 07-07-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC00821D
Abstract: A new platinum-AIEgen coordination complex was synthesized, enabling efficient imaging-guided annihilation of cisplatin-resistant cancer cells under mild white light irradiation.
Publisher: American Chemical Society (ACS)
Date: 11-06-2021
DOI: 10.1021/JACS.1C03882
Publisher: American Chemical Society (ACS)
Date: 07-07-2022
DOI: 10.1021/JACS.2C05948
Abstract: Single-molecule white-light emission (SMWLE) has many advantages in practical applications however, the fabrication of SMWLE from nonconjugated luminescent polymers, namely, clusteroluminogens (CLgens), is still a big challenge. Herein, the first ex le of linear nonconjugated polyesters with SMWLE is reported. Twenty-four kinds of nonconjugated aliphatic polyesters with tunable clusteroluminescence (CL) colors and efficiency were synthesized by the copolymerization of six epoxides and four anhydrides. Experimental and calculation results prove that, at the primary structure level, the balance of structural flexibility and rigidity via adjusting the side-chain length significantly enhances the efficiency of CL without wavelength change. However, altering the chemical structures of the monomer from succinic anhydride to
Publisher: Wiley
Date: 30-07-2020
Publisher: Wiley
Date: 23-04-2018
Abstract: A facile and efficient approach is demonstrated to visualize the polymerization in situ. A group of tetraphenylethylene (TPE)‐containing dithiocarbamates were synthesized and screened as agents for reversible addition fragmentation chain transfer (RAFT) polymerizations. The spatial‐temporal control characteristics of photochemistry enabled the RAFT polymerizations to be ON and OFF on demand under alternating visible light irradiation. The emission of TPE is sensitive to the local viscosity change owing to its aggregation‐induced emission characteristic. Quantitative information could be easily acquired by the naked eye without destroying the reaction system. Furthermore, the versatility of such a technique was well demonstrated by 12 different polymerization systems. The present approach thus demonstrated a powerful platform for understanding the controlled living radical polymerization process.
Publisher: American Chemical Society (ACS)
Date: 22-11-2022
Abstract: It remains a great challenge to design and synthesize organic luminescent molecules with strong emission in both dilute solution and aggregate state. Herein, an organic cage with dodecadansyl groups (D-RCC1) from an easy sulfonation reaction displays strong emissive behavior in dilute organic solution with a quantum yield of 42%. Moreover, D-RCC1 exhibits an ultrahigh quantum yield of 92% in the solid state, which is more than 3 times that of 27% for the model compound D-DEA. The results of the experiment and theoretical calculation show that the three-dimensional symmetrical skeleton of the organic cage anchored evenly by multiple dye molecules effectively satisfies both high local density and a symmetrical distribution of chromophores, which prevents the interaction of dye molecules and ensures that dye molecules have strong emission in both single-molecule and aggregate states.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9SC04239C
Abstract: A polymorphic AIEgen is capable of selective growth in amorphous and crystalline polymer phases with distinct color for microstructure visualization.
Publisher: Springer Science and Business Media LLC
Date: 07-01-2020
DOI: 10.1038/S41467-019-13844-5
Abstract: Host-guest complex solid state molecular motion is a critical but underexplored phenomenon. In principle, it can be used to control molecular machines that function in the solid state. Here we describe a solid state system that operates on the basis of complexation between an all-hydrocarbon macrocycle, D 4d -CDMB-8 , and perylene. Molecular motion in this solid state machine is induced by exposure to organic solvents or grinding and gives rise to different co-crystalline, mixed crystalline, or amorphous forms. Distinct time-dependent emissive responses are seen for different organic solvents as their respective vapours or when the solid forms are subject to grinding. This temporal feature allows the present D 4d -CDMB-8 ⊃perylene-based system to be used as a time-dependent, colour-based 4th dimension response element in pattern-based information codes. This work highlights how dynamic control over solid-state host-guest molecular motion may be used to induce a tuneable temporal response and provide materials with information storage capability.
Publisher: American Chemical Society (ACS)
Date: 21-06-2021
DOI: 10.1021/JACS.1C02594
Publisher: American Chemical Society (ACS)
Date: 25-05-2021
Publisher: Springer Science and Business Media LLC
Date: 09-03-2020
DOI: 10.1038/S41467-020-15095-1
Abstract: Fluorescence imaging in near-infrared IIb (NIR-IIb, 1500–1700 nm) spectrum holds a great promise for tissue imaging. While few inorganic NIR-IIb fluorescent probes have been reported, their organic counterparts are still rarely developed, possibly due to the shortage of efficient materials with long emission wavelength. Herein, we propose a molecular design philosophy to explore pure organic NIR-IIb fluorophores by manipulation of the effects of twisted intramolecular charge transfer and aggregation-induced emission at the molecular and morphological levels. An organic fluorescent dye emitting up to 1600 nm with a quantum yield of 11.5% in the NIR-II region is developed. NIR-IIb fluorescence imaging of blood vessels and deeply-located intestinal tract of live mice based on organic dyes is achieved with high clarity and enhanced signal-to-background ratio. We hope this study will inspire further development on the evolution of pure organic NIR-IIb dyes for bio-imaging.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0QM00682C
Abstract: A synergetic imaging platform was established to achieve LDs-specific imaging by STED nanoscopy and TPF microscopy. Benefiting from its high PLQYs, outstanding photo-stability, and high LDs specificity, a superior resolution in cells and a deep penetration depth in tissues were achieved.
Publisher: American Chemical Society (ACS)
Date: 04-10-2019
Abstract: Organic fluorophores for stimulated emission depletion (STED) nanoscopy usually suffer from quenched emission in the aggregate state and inferior photostability, which largely limit their application in real-time,
Publisher: American Chemical Society (ACS)
Date: 15-09-2023
DOI: 10.1021/JACS.3C08164
Publisher: American Chemical Society (ACS)
Date: 13-11-2019
DOI: 10.1021/JACS.9B09239
Abstract: Simple, rapid, and sensitive assays of DNA sequence hold great importance in genetic analysis, clinical diagnosis, and molecular biology research. Most current methods for DNA detection, based on the complementary base pairing, require hybridization with intricately modified single-stranded DNA (ssDNA) probes or analytes. Herein, we have developed a powerful molecule with aggregation-induced emission (AIE) characteristic, namely, TPBT, which can specifically recognize double-stranded DNA (dsDNA) by emitting out a unique dual-color fluorescent signal of red (∼640 nm) and green (∼537 nm). The red-color emission at around 640 nm is observed when TPBT binds with dsDNA, ssDNA, proteins, and other polyanionic analytes. However, the green emission at around 537 nm is demonstrated to be the exclusive response of TPBT to dsDNA, which is closely related to the conformational change of TPBT upon groove binding. More strikingly, TPBT can distinguish single-nucleotide polymorphisms (SNPs) in a dsDNA sequence and detect the DNA damage suffered from UV light with ultrahigh sensitivity and specificity. This label-free, AIEgen-based dsDNA assay method is facile, robust, and universal, which will lead to major advances in genomic and disease diagnosis.
Publisher: Wiley
Date: 03-08-2022
Abstract: Dynamic patterns based on luminescent materials play an essential role in the digital age. However, it is still challenging to develop highly emissive photofluorochromic materials with dynamic behaviors to store information with multiple characteristics. Here, we report a series of dihydroazulene‐based compounds which show typical aggregation‐induced emission (AIE) effect. Moreover, the photo‐switching ability of the dihydroazulene units, undergoing light‐induced ring‐opening, enables photofluorochromic properties. The photofluorochromism also shows quantitively described responses to time and temperature via a reverse ring‐closing process. Ultimately, a rewritable 4D information system, embedded with a quick response code, dot matrix with microstructures, color matrix of fluorescence, and time/temperature‐dependent intensity change, is established with dynamic patterns. This work not only develops a dynamic AIE skeleton with photofluorochromic properties but also provides a new strategy for information encryption and cybernetics.
Publisher: Wiley
Date: 11-02-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9QM00156E
Abstract: Excited-state “double-bond” torsion plays an important role in the nonluminescent behaviour of a stilbene-based twisted isomer.
Publisher: Wiley
Date: 28-02-2018
Publisher: Wiley
Date: 27-08-2019
Abstract: Restriction of intramolecular motion (RIM), as the working mechanism of aggregation-induced emission (AIE), cannot fully explain some heteroatom-containing systems. Now, two excited states are taken into account and a mechanism, restriction of access to dark state (RADS), is specified to elaborate RIM and complete the picture of AIE mechanism. A nitrogen-containing molecule named APA is chosen as a model compound its weak fluorescence in solution is ascribed to the easy access from the bright (π,π*) state to the close-lying dark (n,π*) state. By either metal complexation or aggregation, the dark state is less accessible due to restriction of the molecular motion leading to the dark state and elevation of the dark state energy, thus the bright state emission is restored. RADS is powerful in elucidating the AIE effect of molecules with excited states favoring non-radiative decay, including overlap-forbidden states such as (n,π*) and CT states, spin-forbidden triplet states, and so on.
Publisher: American Chemical Society (ACS)
Date: 07-05-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9QM00404A
Abstract: The special structure of AIEgens facilitates the understanding and application of polymers.
Publisher: Springer Science and Business Media LLC
Date: 11-02-2021
DOI: 10.1038/S41467-021-21208-1
Abstract: Nitric oxide (NO) is an important signaling molecule overexpressed in many diseases, thus the development of NO-activatable probes is of vital significance for monitoring related diseases. However, sensitive photoacoustic (PA) probes for detecting NO-associated complicated diseases (e.g., encephalitis), have yet to be developed. Herein, we report a NO-activated PA probe for in vivo detection of encephalitis by tuning the molecular geometry and energy transformation processes. A strong donor-acceptor structure with increased conjugation can be obtained after NO treatment, along with the active intramolecular motion, significantly boosting “turn-on” near-infrared PA property. The molecular probe exhibits high specificity and sensitivity towards NO over interfering reactive species. The probe is capable of detecting and differentiating encephalitis in different severities with high spatiotemporal resolution. This work will inspire more insights into the development of high-performing activatable PA probes for advanced diagnosis by making full use of intramolecular motion and energy transformation processes.
Publisher: American Chemical Society (ACS)
Date: 30-09-2019
Abstract: Efficient photoisomerization of chromophores is important in living systems, and structural constraints of protein pocket on chromophores are the probable reason for moving their dynamic reaction equilibrium forward. On the other hand, photochemical reaction to switch a molecule from one isomer to the other with different geometry and property in a high yield will continue to play a vital role in the synthetic chemistry and material science. Because of the important role of efficient photoisomerization, a biomimetic approach for "seeing" and controlling the photoisomerization is developed by using the technology of aggregation-induced emission (AIE) with supramolecular chemistry. It is revealed that a (
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9MH01041F
Abstract: A simple but versatile AIEgen with multi-stimuli responsive functions and multifarious real-life application potentials is reported.
Publisher: American Chemical Society (ACS)
Date: 30-09-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9SC06441A
Abstract: Mitochondria-targeted photosensitizers with highly efficient singlet oxygen generation, bright near-infrared AIE and good two-photon absorption are obtained through ingenious molecular engineering for cancer cell-selective photodynamic therapy.
No related grants have been discovered for Haoke Zhang.