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891 result(s) for "Liu, Minghua"
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Chirality and energy transfer amplified circularly polarized luminescence in composite nanohelix
Transfer of both chirality and energy information plays an important role in biological systems. Here we show a chiral donor π-gelator and assembled it with an achiral π-acceptor to see how chirality and energy can be transferred in a composite donor–acceptor system. It is found that the individual chiral gelator can self-assemble into nanohelix. In the presence of the achiral acceptor, the self-assembly can also proceed and lead to the formation of the composite nanohelix. In the composite nanohelix, an energy transfer is realized. Interestingly, in the composite nanohelix, the achiral acceptor can both capture the supramolecular chirality and collect the circularly polarized energy from the chiral donor, showing both supramolecular chirality and energy transfer amplified circularly polarized luminescence (ETACPL). Energy and chirality transfer play a crucial role in living systems. Here, the authors show that achiral acceptors and chiral donor gelators can assemble in a chirally-controlled manner into a supramolecular nanohelix that can additionally harvest circularly polarized energy.
Hierarchically self-assembled homochiral helical microtoroids
Fabricating microscale helical structures from small molecules remains challenging due to the disfavoured torsion energy of twisted architectures and elusory chirality control at different hierarchical levels of assemblies. Here we report a combined solution–interface-directed assembly strategy for the formation of hierarchically self-assembled helical microtoroids with micrometre-scale lengths. A drop-evaporation assembly protocol on a solid substrate from pre-assembled intermediate colloids of enantiomeric binaphthalene bisurea compounds leads to microtoroids with preferred helicity, which depends on the molecular chirality of the starting enantiomers. Collective variable-temperature spectroscopic analyses, electron microscopy characterizations and theoretical simulations reveal a mechanism that simultaneously induces aggregation and cyclization to impart a favourable handedness to the final microtoroidal structures. We then use monodispersed luminescent helical toroids as chiral light-harvesting antenna and show excellent Förster resonance energy transfer ability to a co-hosted chiral acceptor dye, leading to unique circularly polarized luminescence. Our results shed light on the potential of the combined solution–interface-directed self-assembly approach in directing hierarchical chirality control and may advance the prospect of chiral superstructures at a higher length scale.Homochiral helical toroids with micrometre-scale lengths are successfully fabricated by a combined solution–interface-directed hierarchical self-assembly strategy.
Double helical π-aggregate nanoarchitectonics for amplified circularly polarized luminescence
The canonical double helical π-stacked array of base pairs within DNA interior has inspired the interest in supramolecular double helical architectures with advanced electronic, magnetic and optical functions. Here, we report a selective-recognized and chirality-matched co-assembly strategy for the fabrication of fluorescent π-amino acids into double helical π-aggregates, which show exceptional strong circularly polarized luminescence (CPL). The single crystal structure of the optimal combination of co-assemblies shows that the double-stranded helical organization of these π-amino acids is cooperatively assisted by both CH-π and hydrogen-bond arrays with chirality match. The well-defined spatial arrangement of the π-chromophores could effectively suppress the non-radiative decay pathways and facilitate chiral exciton couplings, leading to superior CPL with a strong figure of merit ( g lum  = 0.14 and QY = 0.76). Our findings might open a new door for developing DNA-inspired chiroptical materials with prominent properties by enantioselective co-assembly initiated double helical π-aggregation. Synthesized or self-assembled helical architectures advance the development of chiral functional materials. Here the authors report a selective-recognized and chirality-matched co-assembly strategy for the fabrication of fluorescent π-amino acids into double helical π-aggregates with exceptional strong circularly polarized luminescence
Macroscopic homochiral helicoids self-assembled via screw dislocations
Chirality is a fundamental property in nature and is widely observed at hierarchical scales from subatomic, molecular, supramolecular to macroscopic and even galaxy. However, the transmission of chirality across different length scales and the expression of homochiral nano/microstructures remain challenging. Herein, we report the formation of macroscopic homochiral helicoids with ten micrometers from enantiomeric pyromellitic diimide-based molecular triangle (PMDI-Δ) and achiral pyrene via a screw dislocation-driven co-self-assembly. Chiral transfer and expression from molecular and supramolecular levels, to the macroscopic helicoids, is continuous and follows the molecular chirality of PMDI-Δ. Furthermore, the screw dislocation and chirality transfer lead to a unidirectional curvature of the helicoids, which exhibit excellent circularly polarized luminescence with large | g lum | values up to 0.05. Our results demonstrate the formation of a homochiral macroscopic organic helicoid and function emergence from small molecules via screw dislocations, which deepens our understanding of chiral transfer and expression across different length scales. Chirality is observed at hierarchical scales from subatomic to macroscopic but the transmission of chirality across different length scales and the expression of homochiral nano/microstructures remain challenging. Here, the authors report the formation of macroscopic homochiral helicoids via a screw dislocation-driven co-self-assembly.
Drug-loaded PEG-PLGA nanoparticles for cancer treatment
Nanoparticles based on single-component synthetic polymers, such as poly (lactic acid-co-glycolic acid) (PLGA), have been extensively studied for antitumor drug delivery and adjuvant therapy due to their ability to encapsulate and release drugs, as well as passively target tumors. Amphiphilic block co-polymers, such as polyethylene glycol (PEG)-PLGA, have also been used to prepare multifunctional nanodrug delivery systems with prolonged circulation time and greater bioavailability that can encapsulate a wider variety of drugs, including small molecules, gene-targeting drugs, traditional Chinese medicine (TCM) and multi-target enzyme inhibitors, enhancing their antitumor effect and safety. In addition, the surface of PEG-PLGA nanoparticles has been modified with various ligands to achieve active targeting and selective accumulation of antitumor drugs in tumor cells. Modification with two ligands has also been applied with good antitumor effects, while the use of imaging agents and pH-responsive or magnetic materials has paved the way for the application of such nanoparticles in clinical diagnosis. In this work, we provide an overview of the synthesis and application of PEG-PLGA nanoparticles in cancer treatment and we discuss the recent advances in ligand modification for active tumor targeting.
Stereospecific supramolecular polymerization of nanoclusters into ultra-long helical chains and enantiomer separation
During the construction of supramolecular polymers of smaller nanoparticles/nanoclusters bearing hierarchy and homochirality, the mechanism understanding via intuitive visualization and precise cross-scale chirality modulation is still challenging. For this goal, a cooperative self-assembly strategy is here proposed by using ionic complexes with uniform chemical composition comprising polyanionic nanocluster cores and surrounded chiral cationic organic components as monomers for supramolecular polymerization. The single helical polymer chains bearing a core-shell structure at utmost length over 20 μm are demonstrated showing comparable flexibility resembling covalent polymers. A nucleation-elongation growth mechanism that is not dealt with in nanoparticle systems is confirmed to be accompanied by strict chiral self-sorting. A permeable membrane prepared by simple suction of such supramolecular polymers displays high enantioselectivity (e.e. 98% after four runs) for separating histidine derivatives, which discloses a benefiting helical chain structure-induced functionalization for macroscopic supramolecular materials in highly efficient racemate separation. Understanding the mechanism for supramolecular polymer assembly from nanoclusters bearing hierarchy and homochirality is challenging. Here, the authors report a cooperative self-assembly strategy using ionic complexes with chiral surfactants through a nucleation-elongation growth mechanism with chiral self-sorting and prepare a permeable membrane for the separation of histidine derivatives.
Chiral porphyrin assemblies
Porphyrins are among the most important macrocycles because they perform many essential functions in living systems and serve as building blocks in many functional materials. Incorporating the chirality into porphyrins can aid biomimetic research and the exploration of new functional materials. In this review, recent developments in chiral porphyrin assemblies are highlighted. The review is mainly divided into two sections: the different strategies for constructing chiral porphyrin assemblies and the applications. The formation of chiral porphyrin assemblies can be from porphyrin molecules substituted with chiral groups; achiral porphyrins induced by chiral additives and spontaneous deracemizations of achiral porphyrins during the assemblies. We also provide an overview of the applications of chiral porphyrin assemblies in chiral sensing, asymmetry catalysis, circularly polarized luminescence, and so on. The further challenge in the field is discussed. The study of the chiral assembly of porphyrins can aid biomimetic research and the exploration of functional materials. In this review, recent developments of chiral porphyrins assemblies are highlighted. We also provide an overview of the applications of chiral porphyrin assemblies in the fields of sensing, catalysis, and optics.
Asymmetric catalysis mediated by a mirror symmetry-broken helical nanoribbon
Although chirality has been recognized as an essential entity for life, it still remains a big mystery how the homochirality in nature emerged in essential biomolecules. Certain achiral motifs are known to assemble into chiral nanostructures. In rare cases, their absolute geometries are enantiomerically biased by mirror symmetry breaking. Here we report the first example of asymmetric catalysis by using a mirror symmetry-broken helical nanoribbon as the ligand. We obtain this helical nanoribbon from a benzoic acid appended achiral benzene-1,3,5-tricarboxamide by its helical supramolecular assembly and employ it for the Cu 2+ -catalyzed Diels–Alder reaction. By thorough optimization of the reaction (conversion: > 99%, turnover number: ~90), the enantiomeric excess eventually reaches 46% (major/minor enantiomers = 73/27). We also confirm that the helical nanoribbon indeed carries helically twisted binding sites for Cu 2+ . Our achievement may provide the fundamental breakthrough for producing optically active molecules from a mixture of totally achiral motifs. If asymmetric catalysts were available by mirror symmetry breaking, an important insight may be given to how the biomolecular homochirality emerged in nature. Here, the authors report the first example of asymmetric catalysis by employing mirror symmetry-broken helical nanoribbons as the ligand.
Self-assembled Möbius strips with controlled helicity
Different from molecular level topology, the development of supramolecular topology has been limited due to a lack of reliable synthetic methods. Here we describe a supramolecular strategy of accessing Möbius strip, a fascinating topological object featured with only a single edge and single side. Through bending and cyclization of twisted nanofibers self-assembled from chiral glutamate amphiphiles, supramolecular nano-toroids with various twist numbers were obtained. Electron microscopic techniques could clearly identify the formation of Möbius strips when twist numbers on the toroidal fibers are odd ones. Spectroscopic and morphological analysis indicates that the helicity of the Möbius strips and nano-toroids stems from the molecular chirality of glutamate molecules. Therefore, M - and P -helical Möbius strips could be formed from L- and D-amphiphiles, respectively. Our experimental results and theoretical simulations may advance the prospect of creating chiral topologically complex structures via supramolecular approach. Different to exploring molecular topology, the development of supramolecular topology has been limited due to a lack of reliable synthetic methods. Here, the authors describe a supramolecular strategy to access Möbius strips through bending and cyclization of twisted nanofibers self-assembled from chiral glutamate amphiphiles.
Iterated Residual Graph Convolutional Neural Network for Personalized Three-Dimensional Reconstruction of Left Myocardium from Cardiac MR Images
Three-dimensional reconstruction of the left myocardium is of great significance for the diagnosis and treatment of cardiac diseases. This paper proposes a personalized 3D reconstruction algorithm for the left myocardium using cardiac MR images by incorporating a residual graph convolutional neural network. The accuracy of the mesh, reconstructed using the model-based algorithm, is largely affected by the similarity between the target object and the average model. The initial triangular mesh is obtained directly from the segmentation result of the left myocardium. The mesh is then deformed using an iterated residual graph convolutional neural network. A vertex feature learning module is also built to assist the mesh deformation by adopting an encoder–decoder neural network to represent the skeleton of the left myocardium at different receptive fields. In this way, the shape and local relationships of the left myocardium are used to guide the mesh deformation. Qualitative and quantitative comparative experiments were conducted on cardiac MR images, and the results verified the rationale and competitiveness of the proposed method compared to related state-of-the-art approaches.