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| Open AccessSelective amide bond formation in redox-active coacervate protocells
Coacervate droplets are promising protocells that sequester nutrients, but how new peptides could be synthesized inside coacervates remains a mystery. Here, the authors develop redox-active coacervates that facilitate the formation of new peptide bonds.
- Jiahua Wang
- , Manzar Abbas
- & Evan Spruijt
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Article
| Open AccessSolvent-pair surfactants enabled assembly of clusters and copolymers towards programmed mesoporous metal oxides
A solvent-pair surfactants enabled assembly method is developed to achieve a general and programmable synthesis of mesoporous metal oxides via the association of POMs with block copolymers through indirect interaction.
- Wenhe Xie
- , Yuan Ren
- & Yonghui Deng
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Article
| Open AccessSite-selective chemical reactions by on-water surface sequential assembly
Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, the authors demonstrate the assembly of amino-substituted porphyrins on a water surface into J-aggregate structures in the presence of charged surfactants.
- Anupam Prasoon
- , Xiaoqing Yu
- & Xinliang Feng
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Article
| Open AccessThermally-induced atropisomerism promotes metal-organic cage construction
While heat modification is ubiquitous in biologic systems, it remains a significant challenge in artificial systems. Here the authors demonstrate thermal regulation of conversion between different rigid macrocycle atropisomers and related self-assemblies.
- Jiaqi Liang
- , Shuai Lu
- & Han-Yuan Gong
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Article
| Open AccessAnti-Kasha triplet energy transfer and excitation wavelength dependent persistent luminescence from host-guest doping systems
Anti-Kasha processes have potential in organic luminogens, but design of materials with these characteristics is challenging. Here, the authors report the development of a host-guest system with anti-Kasha behaviour and triplet energy transfer.
- Weiwei Xie
- , Wenbin Huang
- & Ben Zhong Tang
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Article
| Open AccessA dodecamethoxy[6]cycloparaphenylene consisting entirely of hydroquinone ethers: unveiling in-plane aromaticity through a rotaxane structure
“Cycloparaphenylenes consisting of are cyclic π-conjugated structures presetting interesting physical properties upon functionalization. However, the ring strain and steric hindrance of the substituents hamper the functionalization of small sized cycloparaphenylenes. Here, the authors describe a [6]cycloparaphenylene with twelve methoxy units employed to form a rotaxane with in-plane aromaticity upon oxidation.”
- Naoki Narita
- , Yusuke Kurita
- & Yoshitaka Tsuchido
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Article
| Open AccessSelective synthesis of tightly- and loosely-twisted metallomacrocycle isomers towards precise control of helicity inversion motion
Molecular twist is a characteristic component of molecular machines. Here the authors report a kinetically selective synthesis of tightly- and loosely-twisted isomers of a trinuclear Pd-macrocycle and their markedly different molecular behaviours.
- Tomoki Nakajima
- , Shohei Tashiro
- & Mitsuhiko Shionoya
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Article
| Open AccessCooperative supramolecular polymerization of styrylpyrenes for color-dependent circularly polarized luminescence and photocycloaddition
Strategies to construct circularly polarized luminescence (CPL)-active materials with color modulation and handedness of CPL are desirable for the synthesis of chiral photo-responsive devices. Here the authors develop a CPL system based on styrylpyrenes. Benefiting from CH-π interactions between chromophores, the styrylpyrene aggregates show color-dependent CPL property and photo-responsive behavior.
- Wei Yuan
- , Letian Chen
- & Yanli Zhao
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Article
| Open AccessSelection of isomerization pathways of multistep photoswitches by chalcogen bonding
Multistep photoswitches can engage in different photoisomerization pathways, but are challenging to control. Here, the authors report the development of multistep photoswitches by manipulation of the strength and mechanism of chalcogen bonding interactions.
- Shuaipeng Jia
- , Hebo Ye
- & Lei You
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Article
| Open AccessDirect prediction of gas adsorption via spatial atom interaction learning
Accurate end-to-end deep learning models for adsorption prediction in porous materials would help its discovery. Here, the authors present DeepSorption, a spatial atom interaction learning network to predict structure-adsorption from atomic coordinates and chemical element types.
- Jiyu Cui
- , Fang Wu
- & Huabin Xing
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Article
| Open AccessAtomically precise ultrasmall copper cluster for room-temperature highly regioselective dehydrogenative coupling
Three-component dehydrogenative coupling reactions represent important and practical methodologies for forging new C–N bonds and C–C bonds but achieving all-in-one dehydrogenative coupling functionalization by a single catalytic system remains a great challenge. Here, the authors develop a rigid flexible-coupled copper using a tridentate N-heterocyclic carbene ligand to achieve dehydrogenative coupling using a single catalyst system.
- Teng Jia
- , Yi-Xin Li
- & Shuang-Quan Zang
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Article
| Open AccessStapling strategy for slowing helicity interconversion of α-helical peptides and isolating chiral auxiliary-free one-handed forms
In nature, α-helical peptides adopt right-handed conformations dictated by L-amino acids, but isolating one-handed α-helical peptides composed of only achiral components remains a challenge. Here, the authors achieve this by optical resolution of the corresponding racemic (quasi-)static α-helical peptide with double stapling, which effectively freezes the interconversion between the right-handed (P)- and left-handed (M)-α-helices.
- Naoki Ousaka
- , Mark J. MacLachlan
- & Shigehisa Akine
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Article
| Open AccessHighly efficient color-tunable organic co-crystals unveiling polymorphism, isomerism, delayed fluorescence for optical waveguides and cell-imaging
Co-crystals of donor-acceptor functional material pairs give switchable optical properties despite challenging aggregation-caused quenching effects. Here, the authors report several organic co-crystals with thermally-activated delayed fluorescence, waveguiding and bio-imaging application.
- Debasish Barman
- , Mari Annadhasan
- & Parameswar Krishnan Iyer
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Article
| Open AccessAutonomous self-healing organic crystals for nonlinear optics
There are many potential applications for non-centrosymmetric molecular crystals, but due to their typical brittle nature, efficiency of applications declines on prolonged use. Here, the authors report an autonomous self-healing ability of dibenzoate derivative single crystals that can retain its non-linear optical response.
- Saikat Mondal
- , Pratap Tanari
- & C. Malla Reddy
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Article
| Open AccessNIR-dye bridged human serum albumin reassemblies for effective photothermal therapy of tumor
Human serum albumin (HSA) can be used as a drug delivery material for cancer therapy. Here, the authors report an HSA-based photothermal platform that improves drug loading and photothermal therapeutic performance in breast cancer mouse models.
- Zhaoqing Shi
- , Miaomiao Luo
- & Hongzhong Chen
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Article
| Open AccessDynamic and transformable Cu12 cluster-based C-H···π-stacked porous supramolecular frameworks
The assembly of cluster-based π-stacked porous supramolecular frameworks presents daunting challenges. Here, the authors report a dynamic and transformable supramolecular framework based on Cu12 cluster and C-H···π-stacking with permanent porosity
- Chengkai Zhang
- , Zhi Wang
- & Di Sun
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Article
| Open AccessSupramolecular catalysis with ethers enabled by dual chalcogen bonding activation
The activation of ethers by weak interactions in supramolecular catalysis remains challenging. Here, the authors describe an activation mode based on dual Se···π and Se···O bonding, that can activate benzylic as well as allylic ether C-O σ-bonds to achieve cyclization, coupling and elimination reactions.
- Zhiguo Zhao
- , Yuanling Pang
- & Yao Wang
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Article
| Open AccessCounteranion-mediated efficient iodine capture in a hexacationic imidazolium organic cage enabled by multiple non-covalent interactions
The development of efficient adsorbents to capture iodine originating from radioactive wastes is of importance. Here, the authors synthesize hexacationic imidazolium organic cages and study the crucial role of the counter anions for iodine capture and the iodine binding modes at the molecular level on the solid state.
- Jian Yang
- , Shao-Jun Hu
- & Qing-Fu Sun
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| Open AccessGrinding-induced supramolecular charge-transfer assemblies with switchable vapochromism toward haloalkane isomers
The use of macrocycles to develop charge-transfer complexes in the solid state was recently demonstrated. Here, the authors develop an on-off type vapochromic system toward positional bromoalkane isomers by the reassembly and disassembly of charge-transfer complexes between a pillar[5]arene and electron-deficient aromatic guests in the solid state.
- Jia-Rui Wu
- , Gengxin Wu
- & Ying-Wei Yang
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Article
| Open AccessDual enzyme-powered chemotactic cross β amyloid based functional nanomotors
Nanomotor chassis constructed from biological precursors and powered by biocatalytic transformations can offer important applications in the future. Here, the authors prepare short-peptide-based cross β amyloid nanomotors which can host dedicated enzymes with orthogonal substrates for motility and navigation.
- Chandranath Ghosh
- , Souvik Ghosh
- & Dibyendu Das
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| Open AccessHistidine modulates amyloid-like assembly of peptide nanomaterials and confers enzyme-like activity
In this work, the authors report that Histidine residues play a critical role in modulating amyloid-like assembly and building active sites for Fmoc–F–F and Aβ aggregates. Aβ1-42 filaments were found to perform peroxidase-like activity to enhance oxidative stress, which might also be ascribed to the interaction mode of His and F-F.
- Ye Yuan
- , Lei Chen
- & Lizeng Gao
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Article
| Open AccessNongenetic surface engineering of mesenchymal stromal cells with polyvalent antibodies to enhance targeting efficiency
Limited delivery of therapeutic cells to diseased tissue hampers the effective application of mesenchymal stromal cells (MSCs). Here, authors modify the cell surface with polyvalent antibodies using DNA-templated assembly, and show that polyvalent interactions can be used to improve the targeting efficiency of MSCs.
- Tenghui Ye
- , Xi Liu
- & Peng Shi
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| Open AccessChiral recognition of neutral guests by chiral naphthotubes with a bis-thiourea endo-functionalized cavity
Chiral receptors with an endo-functionalized cavity for chiral recognition are of interest in the field of molecular recognition. Here, the authors develop chiral naphthotubes containing a bis-thiourea endo-functionalized cavity to effectively recognize neutral chiral molecules with high enantioselectivity.
- Song-Meng Wang
- , Yan-Fang Wang
- & Liu-Pan Yang
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Article
| Open AccessDual hypoxia-responsive supramolecular complex for cancer target therapy
The natural product BE-43547A2 (BE) could potentially serve as a template of hypoxia target strategy for treating pancreatic cancer, but the unsatisfactory pharmacokinetics profile and severe toxicity impeded the application of BE or its derivatives. Here the authors report a supramolecular dual hypoxia-responsive BE-based complex for achieving efficient drug delivery within tumors.
- Jian-Shuang Guo
- , Juan-Juan Li
- & Yue Chen
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Article
| Open AccessCoupled reaction equilibria enable the light-driven formation of metal-functionalized molecular vanadium oxides
The introduction of metal sites into polyoxometalates is key for tuning their structure and reactivity but the complex mechanisms which govern metal functionalization of polyoxometalates are still poorly understood. Here, the authors report a coupled set of light-dependent and light-independent reaction equilibria controlling the mono- and di- metal-functionalization of a prototype molecular vanadium oxide cluster
- Stefan Repp
- , Moritz Remmers
- & Carsten Streb
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Article
| Open AccessNonporous amorphous superadsorbents for highly effective and selective adsorption of iodine in water
Porous or crystalline materials are generally employed as adsorbents for environmental remediation. Here the authors employ nonporous and amorphous covalent organic superphane cages for aqueous iodine adsorption achieving good selectivity, high adsorption capability and fast kinetics.
- Wei Zhou
- , Aimin Li
- & Qing He
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Article
| Open AccessIntegration of AIEgens into covalent organic frameworks for pyroptosis and ferroptosis primed cancer immunotherapy
Pyroptosis and ferroptosis are typically induced by metal species or chemotherapeutic drugs, and able to boost a robust antitumor immunity, however their therapeutic uses have been hindered by the risks arising from metal species or chemotherapeutic drugs. Here the authors report a pyroptosis and ferroptosis dual-inducer based on non-metallic AIEgen-based covalent organic frameworks.
- Liang Zhang
- , An Song
- & Zhi-Jun Sun
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| Open AccessStimuli-responsive rotaxane-branched dendronized polymers with tunable thermal and rheological properties
Enriching the toolbox of polymers, the design and construction of novel polymers with desired properties and functions remains an attractive topic in polymer chemistry. Here the authors demonstrate rotaxane-branched dendronized polymers with rotaxane-branched dendrons attached onto the polymer chains as polymers with attractive dynamic properties.
- Yu Zhu
- , Hanqiu Jiang
- & Hai-Bo Yang
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Article
| Open AccessA route to metalloligands consolidated silver nanoclusters by grafting thiacalix[4]arene onto polyoxovanadates
Metalloligands provide a potent strategy for manipulating the surface metal arrangements of metal nanoclusters (NCs), but their synthesis and subsequent installation onto metal NCs remains a significant challenge. Here, the authors demonstrate the synthesis of two atomically precise silver NCs by controlling reaction temperature and demonstrate thermal induced structure transformation between the clusters during a temperature-dependent assembly process.
- Zhi Wang
- , Yan-Jie Zhu
- & Di Sun
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Article
| Open AccessDual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis
In this study, benzotrithiophene-based covalent organic frameworks with spatially separated oxidative and reductive reaction centers are rationally designed for photocatalytic production of H2O2 from water and oxygen without sacrificial agents.
- Chencheng Qin
- , Xiaodong Wu
- & Hou Wang
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Article
| Open AccessA cage-on-MOF strategy to coordinatively functionalize mesoporous MOFs for manipulating selectivity in adsorption and catalysis
Functionalising porous materials is a route to enhancing properties of hybrid materials. Here authors present a “Cage-on-MOF” strategy to modify the surface of mesoporous MOFs by using molecular cages to achieve selective dyes adsorption behavior and heterogeneous catalysis.
- Yu Liang
- , Xiaoxin Yang
- & Yu Fang
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Article
| Open AccessData-mining unveils structure–property–activity correlation of viral infectivity enhancing self-assembling peptides
Certain peptides can boost viral infectivity. However, the requirements for their activity remain unclear. Here, the authors demonstrate that peptides are efficient viral enhancers if they form hydrophobic β-sheet-rich, positively charged μm-sized aggregates.
- Kübra Kaygisiz
- , Lena Rauch-Wirth
- & Tanja Weil
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| Open AccessAllosteric control of olefin isomerization kinetics via remote metal binding and its mechanochemical analysis
The mechanisms by which changes in local geometries of receptor sites lower activation reaction barriers in electronically uncoupled, remote reaction moieties remain relatively unexplored. Here, the authors demonstrate allosteric acceleration in the thermal isomerization of an alkene triggered by the binding of a metal ion to a remote receptor site.
- Yichen Yu
- , Robert T. O’Neill
- & Stephen L. Craig
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| Open AccessProgrammable supramolecular chirality in non-equilibrium systems affording a multistate chiroptical switch
The dynamic regulation of supramolecular chirality in non-equilibrium systems can provide valuable insights into molecular self-assembly in living systems. Here, the authors demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of a non-equilibrium assembled system.
- Jingjing Li
- , Yihan Cui
- & Chun-Sen Liu
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| Open AccessCe-mediated molecular tailoring on gigantic polyoxometalate {Mo132} into half-closed {Ce11Mo96} for high proton conduction
Polyoxometalates (POMs) are molecular clusters with diverse structures. Here authors present the synthesis of POMs by Ce-mediated molecular tailoring from gigantic {Mo132} into half-closed {Ce11Mo96}, with proton conductivity nearly two orders of magnitude higher than {Mo132}.
- Xue-Xin Li
- , Cai-Hong Li
- & Zhong-Min Su
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Article
| Open AccessPillararene incorporated metal–organic frameworks for supramolecular recognition and selective separation
Frameworks containing flexible macrocycle units provide opportunities in molecular recognition and separation. Here authors present MOFs with uniformly embedded pillar[5]arene that can recognise paraquat and 1,2,4,5-tetracyanobenzene in solution and selectively remove trace pyridine from toluene.
- Yitao Wu
- , Meiqi Tang
- & Feihe Huang
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Article
| Open AccessEffector-dependent structural transformation of a crystalline framework with allosteric effects on molecular recognition ability
Porous crystals with molecular recognition sites in the inner pores are promising for achieving functional control, where the local binding of effectors triggers a distortion which propagates throughout the structure. Here the authors report that the structure of a porous molecular crystal can be allosterically controlled by local adsorption of effectors within low-symmetry nanochannels with multiple molecular recognition sites.
- Ryunosuke Hayashi
- , Shohei Tashiro
- & Mitsuhiko Shionoya
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Article
| Open AccessSaddles as rotational locks within shape-assisted self-assembled nanosheets
Self-assembly in the formation of two dimensional materials typically relies upon strong, directional interactions instead of covalent bonds but control over less directional forces remains challenging. Here, the authors show the process of shape-assisted self-assembly to be consistent across a range of derivatives that highlights the restriction of rotational motion.
- Joseph F. Woods
- , Lucía Gallego
- & Michel Rickhaus
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Article
| Open AccessA stretchable, mechanically robust polymer exhibiting shape-memory-assisted self-healing and clustering-triggered emission
Polymers formed with non-covalent bonds are increasingly being developed, but often show inferior mechanical properties. Here, the authors report the development of high performances polyurethane-urea elastomer with shape-memory assisted self-healing behaviour
- Xiaoyue Wang
- , Jing Xu
- & Xinrui Zhang
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Article
| Open AccessThe sharp structural switch of covalent cages mediated by subtle variation of directing groups
Controlling the self-assembly on noncovalent components is possible by suppressing entropy loss with templates but this is challenging for covalent components. Here the authors employed directing groups to endow purely covalent molecular building blocks with different conformations which favor the formation of specific self-assembled products.
- Qiong Chen
- , Zhaoyong Li
- & Hao Li
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Article
| Open AccessThe host–guest inclusion driven by host-stabilized charge transfer for construction of sequentially red-shifted mechanochromic system
The understanding of the structure-property relationship of mechanochromic luminescent molecules remains challenging. Here, the authors elucidate the effect of host-guest interactions on the mechanochromic properties of organic molecules.
- Dongdong Sun
- , Yong Wu
- & Simin Liu
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Article
| Open AccessA supramolecular metalloenzyme possessing robust oxidase-mimetic catalytic function
The de novo synthesis of enzyme-like active sites remains a challenge, due to the difficulties in imitating the spatial arrangement of the functional groups. Here, the authors report the construction of a supramolecular mimetic enzyme possessing catechol oxidase-like copper-cluster active sites.
- Shichao Xu
- , Haifeng Wu
- & Zhen-Gang Wang
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Article
| Open AccessPhotoswitchable dynamic conjugate addition-elimination reactions as a tool for light-mediated click and clip chemistry
Photoinduced dynamic covalent bonds have the advantage of light-mediated bond making and breaking. Here, the authors report photoswitchable dynamic conjugate addition-elimination reactions with a broad scope and demonstrate diverse applications.
- Hanwei Lu
- , Hebo Ye
- & Lei You
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Article
| Open AccessAssembly drives regioselective azide-alkyne cycloaddition reaction
Metal-free versions of azide–alkyne cycloadditions could find widespread applications in biomedical contexts. Here, the authors report an assembly-driven, regioselective azide–alkyne cycloaddition.
- Qiaochu Jiang
- , Wenjun Zhan
- & Gaolin Liang
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Article
| Open AccessCucurbit[8]uril-based water-dispersible assemblies with enhanced optoacoustic performance for multispectral optoacoustic imaging
The applications of organic small-molecule contrast agents for multispectral optoacoustic imaging have been restrained by several challenges including relatively low extinction coefficient, poor water solubility and weak optoacoustic performance. Here, the authors address these limitations by constructing water-dispersible supramolecular optoacoustic assemblies based on cucurbit[8]uril.
- Yinglong Wu
- , Lihe Sun
- & Yanli Zhao
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Article
| Open AccessAccelerating the prediction and discovery of peptide hydrogels with human-in-the-loop
Accurate prediction of peptidic hydrogels could prove useful for diverse biomedical applications. Here, the authors develop a “human-in-the-loop” approach that integrates coarse-grained molecular dynamics, machine learning, and experimentation to design natural peptide hydrogels.
- Tengyan Xu
- , Jiaqi Wang
- & Huaimin Wang
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Article
| Open AccessRapid and reversible optical switching of cell membrane area by an amphiphilic azobenzene
The surface area of living cells is tightly regulated. Here, authors show that the surface area and shape of cells can be reversibly manipulated with light using amphiphilic molecular photoswitches that enter and leave the membrane.
- Fabian Höglsperger
- , Bart E. Vos
- & Bart Jan Ravoo
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| Open AccessAn approach to MOFaxanes by threading ultralong polymers through metal–organic framework microcrystals
Mechanically interlocked architectures inspired the fabrication of numerous molecular systems, but the topological design of such architectures has not been fully explored from the nano- to the macroscopic scale. Here, the authors propose a MOFaxane, comprised of long chain molecules penetrating a microcrystal of metal– organic framework.
- Tomoya Iizuka
- , Hiroyuki Sano
- & Takashi Uemura
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| Open AccessMulti-chiral materials comprising metallosupramolecular and covalent helical polymers containing five axial motifs within a helix
The axial helical structure of supramolecular and covalent polymers provides communication mechanisms among monomer repeating units. Here, the authors present multi-helical materials comprising five axial motifs that combine information from both metallosupramolecular and covalent helical polymers
- Francisco Rey- Tarrío
- , Emilio Quiñoá
- & Félix Freire