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| Open AccessA switchable self-assembling and disassembling chiral system based on a porphyrin-substituted phenylalanine–phenylalanine motif
Artificial light-harvesting systems cannot self-assemble into photon-capturing structures that can reversibly switch into an inactive state. Here, the authors describe a simple and robust dipeptide construct which self-assembles to fibrils, platelets or nanospheres with varying optical properties.
- Georgios Charalambidis
- , Evangelos Georgilis
- & Teodor Silviu Balaban
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Article
| Open AccessChemoselective single-site Earth-abundant metal catalysts at metal–organic framework nodes
Catalysis with non-precious metals presents many advantages including ease of availability, security of supply and low cost. Here, the authors report a metal–organic framework with cobalt or iron sites for use as single-site solid catalysts in a number of chemoselective reactions.
- Kuntal Manna
- , Pengfei Ji
- & Wenbin Lin
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| Open AccessShaping polymersomes into predictable morphologies via out-of-equilibrium self-assembly
Polymersomes are used in many applications, ranging from drug delivery to microfluidics, but controlling their shape is difficult. Here, Christianen and co-workers have precisely controlled polymersome shape via an out-of-equilibrium process and fully understood the mechanism of this procedure.
- R. S. M. Rikken
- , H. Engelkamp
- & P. C. M. Christianen
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| Open AccessAssembled molecular face-rotating polyhedra to transfer chirality from two to three dimensions
Protein subunits on the capsids of icosahedral viruses can form patterns with rotational symmetry, which are difficult to recreate in the laboratory. Here the authors report a strategy to construct 3D chiral polyhedra with rotational faces from 2D chiral truxene-based units through dynamic covalent chemistry.
- Xinchang Wang
- , Yu Wang
- & Xiaoyu Cao
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| Open AccessChirality imprinting and direct asymmetric reaction screening using a stereodynamic Brønsted/Lewis acid receptor
Determining results of asymmetric reactions can take long periods of time and consume large amounts of organic solvents during work-up and analysis. Here, the authors report a bifunctional organic probe that can bind to chiral hydroxyacids, and provide yield, enantiomeric excess and absolute configuration even with crude mixtures.
- Keith W. Bentley
- , Daysi Proano
- & Christian Wolf
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Article
| Open AccessMicrofibres and macroscopic films from the coordination-driven hierarchical self-assembly of cylindrical micelles
Anisotropic nanoparticles made from block copolymers are important building blocks for synthetic hierarchical materials. Here, the authors report a reversible coordination-driven self-assembly strategy for the preparation of micron-scale fibres and macroscopic films based on monodisperse cylindrical micelles.
- David J. Lunn
- , Oliver E. C. Gould
- & Ian Manners
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| Open AccessLong-range movement of large mechanically interlocked DNA nanostructures
Rotaxanes are interlocked molecules that can undergo sliding and rotational movements and can be used in artificial molecular machines and motors. Here, Simmel and co-workers show a rigid rotaxane structures consisting of DNA origami subunits that can slide over several hundreds of nanometres.
- Jonathan List
- , Elisabeth Falgenhauer
- & Friedrich C. Simmel
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| Open AccessPeptide–oligonucleotide conjugates as nanoscale building blocks for assembly of an artificial three-helix protein mimic
Peptide and oligonucleotide systems are known to self-assemble both in nature and artificial systems. Here, the authors combine both forms of self-assembly through the synthesis of peptideoligonucleotide conjugates and show formation of a three-helix structure that dimerises at higher concentrations.
- Chenguang Lou
- , Manuel C. Martos-Maldonado
- & Knud J. Jensen
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Article
| Open AccessHighly stable and self-repairing membrane-mimetic 2D nanomaterials assembled from lipid-like peptoids
Biomimetic membranes can be used for various applications such as sensors and separations. Here, Chen et al. report the assembly of lipid-like peptoids into stable and self-repairing 2D membrane nanomaterials that change in thickness when under external stimuli.
- Haibao Jin
- , Fang Jiao
- & Chun-Long Chen
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Article
| Open AccessRoom temperature molecular up conversion in solution
Up conversion is an Anti-Stokes luminescent process by which photons of low energy are piled up to generate light at a higher energy. Here, the authors report a supramolecular assembly of fluoride-bridged erbium complexes which exhibit this behaviour in D2O solution at room temperature.
- Aline Nonat
- , Chi Fai Chan
- & Loïc J. Charbonnière
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| Open AccessSuperior thermoelasticity and shape-memory nanopores in a porous supramolecular organic framework
Designing porous materials with empty shape-switchable pores remains a formidable challenge. Here, the authors fabricate a supramolecular organic framework possessing empty shape-memory nanopores which operates via a ferroelastic transition, endowing it with switchable sorption properties.
- You-Gui Huang
- , Yoshihito Shiota
- & Osamu Sato
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Article
| Open AccessProtein-directed self-assembly of a fullerene crystal
Self-assembly enables complex structures to be fabricated from a few relatively simple components, but requires a detailed understanding of how the constituents may interact. Here, the authors report the rational assembly and crystallographic characterization of a fullerene-protein superstructure.
- Kook-Han Kim
- , Dong-Kyun Ko
- & Gevorg Grigoryan
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| Open AccessSupramolecular macrocycles reversibly assembled by Te…O chalcogen bonding
Similarly to halogen bonding, the heavier chalcogens are capable of forming supramolecular links with electron rich sites. Here, the authors show that these forces can allow the formation of well-defined cyclic structures that are stable in solution and are capable of forming host-guest complexes.
- Peter C. Ho
- , Patrick Szydlowski
- & Ignacio Vargas-Baca
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| Open AccessIn situ microscopy of the self-assembly of branched nanocrystals in solution
Understanding the structure and transformation of colloidal matter requires probing configurations from monomers to extended assemblies. Here, the authors use liquid-cell electron microscopy to elucidate the nucleation and growth properties of linear chains of branched nanocrystals in solution.
- Eli Sutter
- , Peter Sutter
- & Liberato Manna
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| Open AccessMaking hybrid [n]-rotaxanes as supramolecular arrays of molecular electron spin qubits
Paramagnetic heterometallic rings have long been considered as possible qubits within a quantum information processing system. Here, the authors employ supramolecular chemistry to fabricate multiple rings around multi-armed threads, as an important step towards generating useful qubit arrays.
- Antonio Fernandez
- , Jesus Ferrando-Soria
- & Richard E.P. Winpenny
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| Open AccessDirect observation of mineral–organic composite formation reveals occlusion mechanism
The occlusion of biomacromolecules can endow biominerals with enhanced mechanical properties. Here, the authors usein situatomic force microscopy and micromechanical simulations to trace micelle incorporation in calcite to shed light on the mechanism of occlusion and cavity formation.
- Kang Rae Cho
- , Yi-Yeoun Kim
- & James J. De Yoreo
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Article
| Open AccessBio-inspired electron-delivering system for reductive activation of dioxygen at metal centres towards artificial flavoenzymes
Activated atmospheric dioxygen is potentially an environmentally friendly oxidant. Here, the authors incorporate a flavin mononucleotide into a water soluble polymer, demonstrating single electron reduction of a metalloporphyrin centre, and subsequent activation of dioxygen for the oxidation of organic substrates.
- Yoann Roux
- , Rémy Ricoux
- & Jean-Pierre Mahy
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| Open AccessTransient signal generation in a self-assembled nanosystem fueled by ATP
Natural and synthetic systems have fundamentally different approaches to signal generation. Here, the authors report a strategy that enables transient signal generation in a self-assembled system and show that it can be used to mimic several key features of natural signalling pathways.
- Cristian Pezzato
- & Leonard J. Prins
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| Open AccessSupramolecular motifs in dynamic covalent PEG-hemiaminal organogels
Control of supramolecular chemistry and dynamic covalent crosslinking are ideal ways to generate soft materials with desirable mechanical behaviours. Here, the authors report on practical and computational methods used to elucidate the structural properties of PEG-hemiaminal organogel networks.
- Courtney H. Fox
- , Gijs M. ter Hurrne
- & Jeannette M. García
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| Open AccessMechanically selflocked chiral gemini-catenanes
Mechanically locked molecules provide interesting topological structures and can present challenging synthetic targets. Here the authors report the synthesis of mechanically self-locked molecules, including chiral endo-spirobicyclics containing multiply interlocked rings within a single molecule.
- Sheng-Hua Li
- , Heng-Yi Zhang
- & Yu Liu
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| Open AccessChirality- and sequence-selective successive self-sorting via specific homo- and complementary-duplex formations
The recognition and self-sorting of chiral molecules is a vital feature of many biomolecules. Here, the authors report chirality- and sequence-specific self-sorting of organic strands containing carboxylic acid or amidine groups, leading to selective duplex formation.
- Wataru Makiguchi
- , Junki Tanabe
- & Eiji Yashima
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| Open AccessSelf-assembly of dynamic orthoester cryptates
Cryptands and related molecules are macrocyclic polyethers capable of strongly binding cations. Here, the authors use orthoester exchange for the dynamic one-pot synthesis of crypates, which can bind cations and, given their constitutionally dynamic nature, can also be decomposed to release their guest.
- René-Chris Brachvogel
- , Frank Hampel
- & Max von Delius
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| Open AccessThree-dimensional positioning and control of colloidal objects utilizing engineered liquid crystalline defect networks
Topological defects can be used not only to modify the properties of liquid crystals but also as scaffolds to build new structures by trapping particles. Here, Yoshida et al. construct three-dimensional colloidal superstructures in a nematic host, which are reconfigurable in an electric field.
- H. Yoshida
- , K. Asakura
- & M. Ozaki
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| Open AccessSupramolecular block copolymers by kinetically controlled co-self-assembly of planar and core-twisted perylene bisimides
Block co-polymers are becoming of ever-increasing importance in polymer science. Here, the authors show that the co-assembly of two perylene bisimide dyes leads to supramolecular block copolymer structures with a regular alternating sequence of short blocks of respective homoaggregates.
- Daniel Görl
- , Xin Zhang
- & Frank Würthner
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Induction and control of supramolecular chirality by light in self-assembled helical nanostructures
There is significant interest in the evolution of supramolecular chirality via self-assembly of achiral building blocks. Here, the authors report a system where the supramolecular chirality can be selectively and reversibly controlled and arrested by visible and ultraviolet circularly polarized light.
- Jisung Kim
- , Jinhee Lee
- & Sang Youl Kim
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| Open AccessTunable solid-state fluorescent materials for supramolecular encryption
Solid-state fluorescent materials show promise for potential applications in security and anti-counterfeiting technologies. Here, the authors report a heterorotaxane which has found application in security inks with highly tunable solid-state fluorescence through supramolecular encapsulation.
- Xisen Hou
- , Chenfeng Ke
- & J. Fraser Stoddart
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| Open AccessSupramolecular gels with high strength by tuning of calix[4]arene-derived networks
The physical properties of gel materials makes them attractive options in various applications, but supramolecular gels typically lack mechanical strength. Here, the authors present a calix[4]arene-based supramoleculer gel tuned to possess high tensile strength.
- Ji Ha Lee
- , Jaehyeon Park
- & Jong Hwa Jung
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Chiral recognition and selection during the self-assembly process of protein-mimic macroanions
Certain chiral macroions have previously been shown to self-assemble into spherical structures. Here, the authors observe self-sorting of racemic macroions into enantiomeric ‘blackberry’-shaped structures, and furthermore show that the addition of chiral co-anions allows the formation of a single enantiomer.
- Panchao Yin
- , Zhi-Ming Zhang
- & Tianbo Liu
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Optically switchable transistors by simple incorporation of photochromic systems into small-molecule semiconducting matrices
Organic thin-film transistors can be photomodulated by incorporating photochromic molecules, but the state-of-the-art suffers from poor charge transport. Here, the authors improve charge mobility by three orders of magnitude by blending small conjugated molecules into diarylethene.
- Mirella El Gemayel
- , Karl Börjesson
- & Paolo Samorì
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Interfacial assembly of dendritic microcapsules with host–guest chemistry
Self-assembly is an attractive route to the formation of functional materials. Here the authors report a droplet-based microfluidic method to assemble supramolecular polymer capsules composed of two different layered shells, capable of orthogonal storage of both hydrophilic and hydrophobic guests.
- Yu Zheng
- , Ziyi Yu
- & Oren A. Scherman
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| Open AccessThree-dimensional periodic supramolecular organic framework ion sponge in water and microcrystals
The construction of soluble periodic supramolecular three-dimensional networks is challenging. Here, the authors use an encapsulated dimerization strategy to direct the assembly of a periodic three-dimensional supramolecular organic framework and evaluate its absorption properties.
- Jia Tian
- , Tian-You Zhou
- & Zhan-Ting Li
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Sponge-like molecular cage for purification of fullerenes
Mixtures of various size fullerenes are available as a component of fullerene soot, but isolating pure fullerenes is a challenging task. Here, the authors use a porphyrin-based supramolecular cage that encapsulates fullerenes with high selectivity and releases C60by a simple washing technique.
- Cristina García-Simón
- , Marc Garcia-Borràs
- & Xavi Ribas
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Ostwald’s rule of stages governs structural transitions and morphology of dipeptide supramolecular polymers
Suparmolecular polymers are built by monomers via non-covalent bonds, whilst the pathway of their nucleation processes is not yet clear. Here, Levin et al.show that the self-assembly of monomers proceeds through a series of metastable states, which are energetically governed by Ostwald’s rule of stages.
- Aviad Levin
- , Thomas O. Mason
- & Ehud Gazit
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Phosphorescent dye-based supramolecules for high-efficiency organic light-emitting diodes
The limit external quantum efficiency of organic LEDs based on isotropically oriented iridium complexes is believed to be around 30%. But Kim et al. show that the emission from these complexes is in fact anisotropic, enabling them to increase the external quantum efficiency of these devices to 36%.
- Kwon-Hyeon Kim
- , Sunghun Lee
- & Jang-Joo Kim
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Protein crystalline frameworks with controllable interpenetration directed by dual supramolecular interactions
Proteins are particularly desirable building blocks for self-assembled biomimetic materials. Here, the authors present crystalline frameworks based on concanavalin A with controllable levels of interpenetration via dual supramolecular interactions.
- Fuji Sakai
- , Guang Yang
- & Ming Jiang
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The surface barrier phenomenon at the loading of metal-organic frameworks
Metal-organic frameworks are well studied for mass transfer applications, although rates of mass transfer for similar systems are shown to vary widely, attributed to surface barriers. Here, the authors quantitatively study this phenomenon and demonstrate that surface barriers are not intrinsic to the materials.
- Lars Heinke
- , Zhigang Gu
- & Christof Wöll
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Correlating interfacial octahedral rotations with magnetism in (LaMnO3+δ)N/(SrTiO3)N superlattices
Layered oxide heterostructures are widely studied because of the new quantum states that can arise at the interface between the oxide materials used. Here, the authors are able to link the rotation of crystallographic oxygen octahedra at the interface to a modified ferromagnetic state in such heterostructures.
- Xiaofang Zhai
- , Long Cheng
- & Changgan Zeng
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Rapid fabrication of hierarchically structured supramolecular nanocomposite thin films in one minute
There is significant research into fabrication methods for the rapid, scalable preparation of composite nanomaterials. Here, the authors probe the assembly of supramolecular nanocomposites in thin films and are able to optimize parameters to produce hierarchically structured thin films in one minute.
- Joseph Kao
- , Kari Thorkelsson
- & Ting Xu
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Crystal structure of an amphiphilic foldamer reveals a 48-mer assembly comprising a hollow truncated octahedron
Foldamers are small molecules or oligomers that can adopt secondary and tertiary structures due to noncovalent interactions. Here, the authors show that an amphiphilic foldamer can adopt a hollow truncated octahedron crystal structure comprising of 48 individual foldamer units.
- Vincenzo Pavone
- , Shao-Qing Zhang
- & William F. DeGrado
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Size evolution of highly amphiphilic macromolecular solution assemblies via a distinct bimodal pathway
Micelles find applications in areas such as drug delivery systems, and as such, the kinetic stability of these structures is of high interest. Here the authors show that individual block copolymer micelles can continue to evolve after transfer to a selective solvent.
- Elizabeth G. Kelley
- , Ryan P. Murphy
- & Thomas H. Epps
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Strongly underestimated dispersion energy in cryptophanes and their complexes
Cryptophanes are common host molecules, capable of binding neutral guests strongly. Here the authors show that, contrary to popular belief, solvents commonly used for these studies can be enclosed by the host and hence affect the calculated binding constants.
- Gebhard Haberhauer
- , Sascha Woitschetzki
- & Heinz Bandmann
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Polystyrene sulphonic acid resins with enhanced acid strength via macromolecular self-assembly within confined nanospace
Solid acid catalysts allow easy separation and reduction in waste not easily achievable with mineral acids. Here the authors report polystyrene sulphonic acid resins whose acid strength and catalytic performance can be tuned by changing their morphology within a confined nanospace.
- Xiaomin Zhang
- , Yaopeng Zhao
- & Qihua Yang
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Article
| Open AccessComplex self-assembly of pyrimido[4,5-d]pyrimidine nucleoside supramolecular structures
Supramolecular self-assembly is a fundamentally important process in fields ranging from structural biology to materials chemistry. Here, the authors report the supramolecular assembly of complex nanostructures from simple nucleosides, and probe the formation process using various in situtechniques.
- Hang Zhao
- , Xiurong Guo
- & Qianming Chen
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Supramolecular high-aspect ratio assemblies with strong antifungal activity
Efficient and pathogen-specific antifungal agents are required to mitigate drug resistance problems. Here the authors present a series of cationic small molecules, which are easy to isolate and characterize, and which can self-assemble to give polymer-like antifungal activity and specificity.
- Kazuki Fukushima
- , Shaoqiong Liu
- & James L. Hedrick
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Macromolecular semi-rigid nanocavities for cooperative recognition of specific large molecular shapes
Large molecular shape-consistent host molecules are required for molecular recognition applications and the development of artificial enzymes. Here, the authors synthesize semi-rigid dendritic molecules with cavities capable of tunable discrimination between a range of large guest molecules.
- Takane Imaoka
- , Yuki Kawana
- & Kimihisa Yamamoto
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Direct visualization of a guest-triggered crystal deformation based on a flexible ultramicroporous framework
Host–guest materials open up the possibility of tuning physical properties based on the addition of appropriate guests. Here, a flexible, porous coordination polymer is reported, in which the addition of guest molecules significantly alters the thermal expansion properties as well as deforming the crystal lattice.
- Hao-Long Zhou
- , Rui-Biao Lin
- & Xiao-Ming Chen
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DNA-directed self-assembly of shape-controlled hydrogels
The development of a series of orthogonal binding interactions to direct the controlled self-assembly of mesoscale objects is desirable. Here, the authors use DNA as a sequence-specific glue to assemble hydrogel cuboids into a diverse series of structures in the micro- to millimeter length scale.
- Hao Qi
- , Majid Ghodousi
- & Ali Khademhosseini
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| Open AccessSelective isolation of gold facilitated by second-sphere coordination with α-cyclodextrin
Currently, gold recovery from waste materials requires inorganic cyanides and more environmentally benign methods are required. Here, the authors report that host–guest interactions between α-cyclodextrin and gold lead to the precipitation of one-dimensional superstructures, offering a selective and green alternative.
- Zhichang Liu
- , Marco Frasconi
- & J. Fraser Stoddart
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Stepwise self-assembly of C60 mediated by atomic scale moiré magnifiers
A promising route towards molecular devices is the self-assembly of atoms or molecules on a surface. Here, Gruznev et al. show that the synthesis of unique geometries of C60molecules on gold–indium-covered crystalline silicon is governed by moiré interference.
- D.V. Gruznev
- , A.V. Matetskiy
- & Y.L. Wang