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| Open AccessDynamic metastable polymersomes enable continuous flow manufacturing
Polymersomes, as analogues of liposomes, have interesting physical and chemical properties, but have not yet been translated into clinical or industrial applications. Here, the authors report the development of a continuous flow process for the production of polymersomes at scale.
- Chin Ken Wong
- , Rebecca Y. Lai
- & Martina H. Stenzel
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Article
| 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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Article
| 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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| 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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Article
| Open AccessJanus particle-engineered structural lipiodol droplets for arterial embolization
Embolization is one of the most promising strategies for clinical disease treatments, however, the existing embolic materials normally have poor embolization effectiveness. Here, the authors report Janus particle-engineered structural lipiodol droplets by programming the self-assembly of Janus particles at the lipiodol-water interface to achieve highly efficient renal embolization.
- Sijian Tao
- , Bingquan Lin
- & Jun-Bing Fan
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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 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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Article
| Open AccessEarly-stage bifurcation of crystallization in a sphere
Thermodynamics predicts equilibrium crystal structures and kinetics discover the pathway to form them. The authors investigate the interplay of thermodynamics and kinetics in the formation of colloidal clusters and reveal a bifurcation at an early stage of the crystallization process.
- Chrameh Fru Mbah
- , Junwei Wang
- & Michael Engel
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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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| 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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Article
| 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 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 AccessImpact of hierarchical water dipole orderings on the dynamics of aqueous salt solutions
The behaviour of ions solvated in water is highly ion-specific. Introducing a length scale that captures the interplay between ion-water and inter-water interactions, along with considering the bond-orientational order of the hydration shell, provides an explanation for the ion-specific effects observed in salt solutions.
- Rui Shi
- , Anthony J. Cooper
- & Hajime Tanaka
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Article
| Open AccessSelf-organization of primitive metabolic cycles due to non-reciprocal interactions
It is generally accepted that non-equilibrium conditions would have been necessary for the formation of primitive metabolic structures, but the focus has mostly been on externally imposed non-equilibrium conditions. Here, the authors show that catalytically active particles like enzymes participating in a metabolic cycle can spontaneously self-organize into dynamically structured condensates composed of active mixtures, by employing non-reciprocal interactions.
- Vincent Ouazan-Reboul
- , Jaime Agudo-Canalejo
- & Ramin Golestanian
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Article
| Open AccessDurable organic nonlinear optical membranes for thermotolerant lightings and in vivo bioimaging
Organic nonlinear optical materials have potential in applications such as bioimaging, but tend to have low photoluminescent quantum yields and are prone to aggregation-caused quenching. Here, the authors report a host-guest approach for improving the luminescent properties of these materials.
- Tian Tian
- , Yuxuan Fang
- & Wu-Qiang Wu
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Article
| Open AccessMacroscopic photonic single crystals via seeded growth of DNA-coated colloids
DNA-programmed colloidal assembly of macroscopic crystals for photonic applications remains elusive. Here, the authors use insights from studies of nucleation and seeded growth to develop a two-step method for assembling macroscopic photonic crystals.
- Alexander Hensley
- , Thomas E. Videbæk
- & W. Benjamin Rogers
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| 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 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 AccessLight-driven self-assembly of spiropyran-functionalized covalent organic framework
Controlling the number of molecular switches and their relative positioning within porous materials is critical to their functionality and properties. Here the authors systematically control the number of spiropyran units in a covalent organic framework using a mixed-linker synthetic strategy which resulted in one photoresponsive unit per pore.
- Gobinda Das
- , Thirumurugan Prakasam
- & Ali Trabolsi
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Article
| Open AccessMorphogenesis of starfish polymersomes
Polymeric vesicles are promising candidates for use in a range of applications including drug delivery and cell mimics, however, control over the shape is still a challenge. Here, the authors report control over local curvature formation by addition of salt ions and stimuli responsive polymer to modulate its interaction with polymeric membrane.
- Jiawei Sun
- , Sandra Kleuskens
- & Daniela A. Wilson
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Article
| Open AccessVacuole dynamics and popping-based motility in liquid droplets of DNA
In this work, the authors report the appearance of vacuoles within the droplets of an enzyme-driven biomolecular liquid. The mechanisms of these behaviors are quantitatively explained with a diffusive capture model of enzyme dynamics.
- Omar A. Saleh
- , Sam Wilken
- & Tim Liedl
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Article
| 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
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| Open AccessA porous metal-organic cage liquid for sustainable CO2 conversion reactions
Preparation of porous liquids are fluids with the permanent porosity still requires complicated and tedious use of porous hosts and bulky liquids. Here, the authors develop a facile method to produce a porous metal-organic cage liquid by self-assembly of long polyethylene glycolimidazolium chain functional linkers, calixarene molecules and Zn ions.
- Chang He
- , Yu-Huang Zou
- & Yuan-Biao Huang
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Article
| Open AccessMechanosensitive non-equilibrium supramolecular polymerization in closed chemical systems
Chemical fuel-driven supramolecular systems have been developed showing out of-equilibrium functions such as transient gelation and oscillations but these systems suffer from undesired waste accumulation and they function only in open systems. Here, the authors we report non-equilibrium supramolecular polymerizations in a closed system, which is built by viologens and pyranine in the presence of hydrazine hydrate.
- Xianhua Lang
- , Yingjie Huang
- & Hui Zhao
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Article
| Open AccessMagnetic control of self-assembly and disassembly in organic materials
Organic molecules and materials are generally insensitive or weakly sensitive to magnetic fields due to their small diamagnetic force. Here, the authors show a strategy to amplify the magnetic responsiveness of self-assembled peptide nanostructures by synergistically combining the concepts of perfect α-helix and rod-coil supramolecular building blocks
- You-jin Jung
- , Hyoseok Kim
- & Yong-beom Lim
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Article
| Open Access[2,2] Paracyclophanes-based double helicates for constructing artificial light-harvesting systems and white LED device
The construction of efficient artificial lightharvesting (ALH) systems is of vital importance in utilizing solar energy. Here, the authors report the non-covalent syntheses of double helicates by metalcoordination interaction and their applications in ALHSs and white LED device
- Zhe Lian
- , Jing He
- & Hua Jiang
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Article
| Open AccessNon-enzymatic oligonucleotide ligation in coacervate protocells sustains compartment-content coupling
Achieving a form of coupling between molecular content, chemical reactions, and chassis in synthetic compartments represents a key step to the assembly of evolvable protocells but remains challenging. Here, the authors design coacervate droplets that promote non-enzymatic oligonucleotide polymerization and that restructure as a result of the reaction dynamics.
- Tommaso P. Fraccia
- & Nicolas Martin
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| Open AccessSwitching imidazole reactivity by dynamic control of tautomer state in an allosteric foldamer
Molecular biology achieves control over complex reaction networks by means of molecular systems that translate a chemical input into an orthogonal chemical output but the application of dynamic foldamers has been limited by the restriction to stereochemical changes that produce spectroscopic signals. Here, the authors present an artificial molecular translation device that converts a chemical input into an unrelated chemical output.
- David P. Tilly
- , Jean-Paul Heeb
- & Jonathan Clayden
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| Open AccessHierarchical porous photosensitizers with efficient photooxidation
Photosensitizers (PS) with nano- or micro-sized pore provide a great promise in the conversion of light energy into chemical fuel but pore deformation and blocking often decreases the catalytic efficiency. Here, the authors prepare an ordered porous PSs by cross-linking hierarchical porous assemblies of hydrogen donating PSs and functionalized acceptors.
- Yajun Fang
- , Yuntian Yang
- & Zhegang Huang
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Article
| Open AccessAlgal cell bionics as a step towards photosynthesis-independent hydrogen production
Low rate and limited duration are major challenges in photobiological hydrogen production. Here, the authors coat algal cells with a concentrically arranged shell comprising an ultra-thin Fe(III)-doped polypyrrole inner layer and outer exoskeleton of CaCO3, and achieve sustainable H2 production for over 200 days.
- Zhijun Xu
- , Jiarui Qi
- & Xin Huang
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Article
| Open AccessAmyloid-polysaccharide interfacial coacervates as therapeutic materials
Liquid-liquid phase separation offer a strategy for targeting biomaterial scaffolds, but controlling assembly to form functional materials is challenging. Here, the authors transform native proteins into amyloid fibres for assembly, and use the materials as a gastric ulcer protective agent.
- Mohammad Peydayesh
- , Sabrina Kistler
- & Raffaele Mezzenga
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Article
| Open AccessHigh-entropy alloy nanopatterns by prescribed metallization of DNA origami templates
Morphology, composition, and uniformity of highly entropic nanoalloys are critical to their properties and applications. Here, the authors develop a DNA origami-based metallization reaction concept for the precise synthesis of multimetallic nanopatterns.
- Mo Xie
- , Weina Fang
- & Huajie Liu
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Article
| Open AccessPolymerizable rotaxane hydrogels for three-dimensional printing fabrication of wearable sensors
While hydrogels find applications in wearable sensors and electronic skins, they are prone to fatigue fractures upon deformation cycling. Xiong et al. report the synthesis of conductive polymerizable rotaxane hydrogels, exhibiting large fatigue resistance, for 3D printable flexible sensors.
- Xueru Xiong
- , Yunhua Chen
- & Yanli Zhao
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Article
| Open AccessBioinspired crowding directs supramolecular polymerisation
Crowding effects have long been established as powerful guiding forces in natural assembly processes. Here the authors report a bioinspired approach translating this phenomenon to artificial supramolecular polymers.
- Nils Bäumer
- , Eduardo Castellanos
- & Gustavo Fernández
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Article
| Open AccessSupramolecular framework membrane for precise sieving of small molecules, nanoparticles and proteins
Synthetic framework materials are appealing candidates for the fabrication of separation membranes but realizing precise control of aperture distribution and separation threshold remains challenging. Here, the authors show a two-dimensional processible supramolecular framework which can be used in the fabrication of separation membranes by integrating directional organic host-guest motifs and inorganic functional polyanionic clusters.
- Guohua Zhang
- , Xinyue Li
- & Lixin Wu
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Article
| Open AccessHybrid assembly of polymeric nanofiber network for robust and electronically conductive hydrogels
Mechanically robust and electrically conductive hydrogels remain challenging to fabricate. Here, the authors present polymeric nanofiber networks with structural robustness and high electronic conductivity and show that cardiomyocytes cultured on these hydrogels exhibit spontaneous and synchronous beating.
- Huimin He
- , Hao Li
- & Lizhi Xu
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Article
| Open AccessSpatially non-uniform condensates emerge from dynamically arrested phase separation
Biomolecular condensates with internal structure allow cells to further organise their processes. In this work the authors investigate how condensates can obtain an internal structure with droplets of dilute phase inside via kinetic, rather than purely thermodynamic driving forces.
- Nadia A. Erkamp
- , Tomas Sneideris
- & Tuomas P. J. Knowles
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Article
| Open AccessSelf-spinning filaments for autonomously linked microfibers
Bio-inspired assembly of mesoscale materials presents a unique challenge due to complex machinery or labor-intensive processing involved in engineering. Barber et al. report chiral filaments self-assembled into free-standing, anisotropic bundles through pre-programmed, light-mediated structural deformations.
- Dylan M. Barber
- , Todd Emrick
- & Alfred J. Crosby
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Article
| Open AccessBiomolecular condensates formed by designer minimalistic peptides
The molecular mechanisms underlying the formation of biomolecular condensates have not been fully elucidated. Here the authors show that the LLPS propensity, dynamics, and encapsulation efficiency of designed peptide condensates can be tuned by subtle changes to the peptide composition.
- Avigail Baruch Leshem
- , Sian Sloan-Dennison
- & Ayala Lampel
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Article
| Open AccessMolecular-level enhanced clusterization-triggered emission of nonconventional luminophores in dilute aqueous solution
Luminophores based on clustering-triggered emission have drawn emerging attention in recent years but they tend to be nonluminescent in dilute solution. Here, the authors design novel clusteroluminogens through modification of cyclodextrin (CD) with amino acids to enable clusterization of chromophores in CD-based confined space and realize blue to cyan fluorescence even in the dilute solution.
- Qiuju Li
- , Xingyi Wang
- & Shun Mao
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Article
| Open AccessA self-standing three-dimensional covalent organic framework film
Fabrication of 3D covalent organic framework thin films is challenging. Here the authors report on a liquid-liquid interfacial approach based on physical-organic considerations to synthesize an ultrathin covalent crystal film.
- Yizhou Yang
- , Yanyan Chen
- & Karl Börjesson
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Article
| Open AccessSymmetry-breaking host–guest assembly in a hydrogen-bonded supramolecular system
Self-assembly processes usually yield symmetric compounds. Here, the authors report the distortion of a symmetric hydrogen-bonded resorcin[4]arene cage upon encapsulation of an iridium complex.
- Shinnosuke Horiuchi
- , Takumi Yamaguchi
- & Keisuke Umakoshi
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Article
| Open AccessMultiscale structural control of thiostannate chalcogels with two-dimensional crystalline constituents
Chalcogenide aerogels (chalcogels) are 3D porous materials with unique properties. Here the authors present a multiscale structure-controlled chalcogel that is synthesized via thiostannate motif-transformation-induced self-assembly.
- Thanh Duy Cam Ha
- , Heehyeon Lee
- & Myung-Gil Kim
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Article
| Open AccessPhotoprogrammable circularly polarized phosphorescence switching of chiral helical polyacetylene thin films
‘Pure organic room-temperature phosphorescence (RTP) materials with circularly polarized luminescence (CPL) gained increasing interest. Here, the authors propose a photoinduced circularly polarized RTP material by homogeneously dispersing phosphorescent chiral polyacetylenes into a processable polymer matrix.
- Zizhao Huang
- , Zhenyi He
- & Xiang Ma