Self-assembly articles within Nature Chemistry

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  • Article |

    The construction of analogues of natural gap junctions would provide a bottom–up strategy for building intercellular communication pathways for synthetic cells. Now artificial intercellular gap junctions have been prepared from unimolecular tubular channels by mimicking the hydrophobic–hydrophilic–hydrophobic triblock structure of natural junction channels.

    • Yong-Hong Fu
    • , Yi-Fei Hu
    •  & Jun-Li Hou

  • Article
    | Open Access

    Advances in the development of cytoskeletal-like materials with modular structures and mechanics are pivotal for the engineering of synthetic cells. Now actin-mimetic supramolecular peptide networks have been designed using programmable peptide–DNA crosslinkers, giving rise to tunable tactoid-shaped bundles and mechanical properties that control spatial localization, the diffusion of payloads and shape changes within artificial cells.

    • Margaret L. Daly
    • , Kengo Nishi
    •  & Ronit Freeman

  • Article
    | Open Access

    Carbon capture, utilization and storage is key for climate change mitigation and developing more environmentally friendly technologies. Now it has been shown that CO2 capture in single-component water-lean solvents is accompanied by the self-assembly of reverse-micelle-like tetrameric clusters in solution that enable the formation of various CO2-containing compounds.

    • Julien Leclaire
    • , David J. Heldebrant
    •  & Jaelynne King

  • Article |

    Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H2 evolution.

    • Isaac N. Cloward
    • , Tianfei Liu
    •  & Alexander J. M. Miller

  • Article |

    Chromophore supramolecular assemblies have long been studied for their exotic photophysical properties arising from their local geometry and long-range sensitive excitonic couplings. Now a high-resolution structure of a model nanotubular system has revealed a uniform brick-layer molecular arrangement and a non-biological supramolecular motif—interlocking sulfonates—enabling clear understanding of supramolecular structure–excitonic property relationships.

    • Arundhati P. Deshmukh
    • , Weili Zheng
    •  & Justin R. Caram

  • Article |

    Metal-mediated self-assembly of organic building blocks is a powerful strategy to generate complex supramolecular objects. The non-statistical combination of multiple different components, however, has been a major challenge. Now integrative self-sorting of low-symmetry multicomponent cages has been achieved by combining shape complementarity and selective backbone interactions under thermodynamic control.

    • Kai Wu
    • , Elie Benchimol
    •  & Guido H. Clever

  • Perspective |

    The self-assembly of stimuli-responsive building blocks yields functional nano-systems and smart materials. This Perspective discusses how the integration of photoswitches into discrete coordination cages enables control over their assembly, guest binding and systems behaviour. Four scenarios are drawn to highlight the relationship between the photoswitching and dynamic assembly equilibria.

    • Elie Benchimol
    • , Jacopo Tessarolo
    •  & Guido H. Clever

  • Article |

    Bottom-up assembly of protocells into networking superstructures represents a further key step towards rudimentary formation of life. Now it has been shown that a pool of biomolecules can self-organize into an interactive binary population of protocell coacervates with a self-sorting chain-like configuration, allowing for biomolecular extraction, translocation and macroscale separation.

    • Wenjing Mu
    • , Liyan Jia
    •  & Yan Qiao

  • News & Views |

    The intentional interweaving of two different metal–organic framework (MOF) lattices could offer a strategy for combining the disparate properties of the two frameworks within a single MOF material. Now, the rational construction of such hetero-interpenetrated MOFs has been demonstrated.

    • Tendai Gadzikwa

  • Article |

    The kinetics of liquid–liquid phase separation (LLPS) in cell-like confinements remains poorly understood. Now it has been shown that it involves complex interplay between the incipient phases and the membrane boundary, which arrests phase coarsening, deforms the membrane and couples LLPS with lipid phase separation.

    • Wan-Chih Su
    • , James C. S. Ho
    •  & Atul N. Parikh

  • News & Views |

    The concepts of multistep processes and regioselectivity — fundamental in covalent synthesis — have now been applied to the non-covalent synthesis of sequence-controlled multiblock supramolecular polymers.

    • Ghislaine Vantomme

  • In Your Element |

    Rajeev K. Dubey and Frank Würthner discuss the colourful character of perylene bisimides and the impact of aggregation on their functional properties.

    • Rajeev K. Dubey
    •  & Frank Würthner

  • Article |

    Supramolecular structures are typically formed by the one-step self-assembly of building blocks. Now, a greater level of control has been achieved using stepwise non-covalent reactions under kinetic control. Two-dimensional block supramolecular polymers with tailored compositions and sequences were synthesized, and a site selectivity that is reminiscent of regioselectivity in covalent synthesis was observed.

    • Norihiko Sasaki
    • , Jun Kikkawa
    •  & Kazunori Sugiyasu

  • Article |

    Clathrates—open crystals with a hierarchy of polyhedral cages—are mostly found in atomic and molecular systems. Now, it has been shown through Monte Carlo simulations that the formation of colloidal host–guest clathrates can be driven by entropy alone, through entropy compartmentalization.

    • Sangmin Lee
    • , Thi Vo
    •  & Sharon C. Glotzer

  • News & Views |

    Systems that feature long-range order but no translational periodicity are intriguing. Now, a T-shaped molecule consisting of three non-miscible components has been devised that self-assembles into a columnar liquid quasicrystal.

    • Marianne Impéror-Clerc

  • Article |

    Quasicrystals are intriguing structures that exhibit long-range positional correlations but no periodicity in real space. Now, T-shaped amphiphilic molecules featuring rigid cores have been found to self-assemble into a columnar liquid quasicrystal with dodecagonal symmetry. The honeycomb structure observed arises from a strictly quasiperiodic tessellation of square, triangular and trapezoidal tiles, rather than from random tiling.

    • Xiangbing Zeng
    • , Benjamin Glettner
    •  & Carsten Tschierske

  • Article |

    The advantages and disadvantages of building a nanosystem using one, two or more molecular components are poorly understood. Now, using structural and catalytic DNA-based nanosystems and theoretical simulations, it has been shown that the assembly of trimeric nanosystems displays much higher levels of programmability and functionality than the monomeric or dimeric counterparts.

    • D. Lauzon
    •  & A. Vallée-Bélisle

  • Article |

    The enantioselective functionalization of C60 is highly challenging, typically requiring complex chiral tethers or demanding chromatography. Fullerenes have now been shown to undergo Diels–Alder reactions in a chemo-, regio- and enantio-selective fashion through confinement within an enantiopure metal–organic cage functionalized with a chiral formylpyridine group.

    • Zifei Lu
    • , Tanya K. Ronson
    •  & Jonathan R. Nitschke

  • Article
    | Open Access

    Modulation of surface properties and functions can be achieved through covalent and non-covalent molecular binding, but the lack of responsiveness and requirement for specific binding groups makes spatiotemporal control challenging. Now, it has been shown that adaptive insertion of a hydrophobic anchor into a poly(ethylene glycol) host is an effective non-covalent binding strategy for programmable surface functionalization.

    • Shaohua Zhang
    • , Wei Li
    •  & Daniela A. Wilson

  • Article |

    Identifying and quantifying the biodistribution of synthetic polymeric nanoparticles in biological milieu is crucial for biomedical applications. Now, it has been shown that encoded polymeric amphiphiles with discrete molar masses undergo sequence- and length-dependent self-assembly into precise digital micelles that can be used in direct sequence reading and ex vivo label-free quantification assays.

    • Qiangqiang Shi
    • , Hao Yin
    •  & Shiyong Liu

  • Article |

    The properties of chiral conjugated molecules, such as the absorption and/or emission of circularly polarized light or electron transport, are highly anisotropic. Now it has been shown that templating layers can control the orientation and anisotropic properties of small chiral molecules in bulk thin films useful for a range of emerging technologies.

    • Jessica Wade
    • , Francesco Salerno
    •  & Matthew J. Fuchter

  • Article |

    Photoelectrochemical cells are hampered by electron–hole recombination. Now, supramolecular machinery has enabled the docking of macrocyclic electron-accepting redox mediators to a dye through pseudorotaxane formation. Upon electron transfer from the dye, the anionic redox-mediator rings are launched away from the surface, reducing charge recombination, establishing charge separation and improving the efficiency of the solar cells in which they feature.

    • T. Bouwens
    • , T. M. A. Bakker
    •  & J. N. H. Reek

  • Article |

    Meso–meso linked porphyrin arrays have been described as rod-like photonic wires. Now it has been shown that they can be bent into rings using template-directed synthesis. These rings of porphyrins mimic the light-harvesting arrays of chlorophyll molecules responsible for photosynthesis.

    • Henrik Gotfredsen
    • , Jie-Ren Deng
    •  & Harry L. Anderson

  • News & Views |

    The rational synthesis of advanced porous materials that mimic the behaviours of biological proteins remains challenging. Now, a distinct type of crystalline porous peptide framework has been prepared through bioinspired noncovalent assembly, enabling chemical tuning of the properties and functions of the pore environments.

    • Jinqiao Dong
    •  & Dan Zhao

  • Article |

    Proton wires in enzyme active sites enable stereoselective reactions under mild conditions by facilitating dual activation of a nucleophile and an electrophile through reciprocal proton transfer. Now it has been shown that such an activation mode can be mimicked inside a supramolecular capsule, enabling a general approach to β-glycosides.

    • Tian-Ren Li
    • , Fabian Huck
    •  & Konrad Tiefenbacher

  • Article |

    Oscillations are widespread throughout the natural world and a number of fascinating inorganic oscillating reactions are known—but the formation and control of oscillating, self-replicating synthetic systems has remained challenging. Now, it has been shown that chemically fuelled oscillations within a network of organic replicators can drive supramolecular assembly and disassembly.

    • Michael G. Howlett
    • , Anthonius H. J. Engwerda
    •  & Stephen P. Fletcher

  • News & Views |

    The rational synthesis of organic nanotubes and their hierarchical architectures has remained challenging. Now, one-dimensional hollow covalent organic frameworks have been prepared that can further assemble into toroid-shaped materials.

    • Gabrielle A. Leith
    •  & Natalia B. Shustova

  • Article |

    A wide variety of covalent organic cages and two- and three-dimensional covalent organic frameworks have been obtained through dynamic covalent chemistry, yet the synthesis of their one-dimensional counterparts has remained challenging. Porous covalent organic nanotubes have now been prepared through reversible aldehyde–amine condensation and it has been shown that these can further assemble into toroidal architectures.

    • Kalipada Koner
    • , Shayan Karak
    •  & Rahul Banerjee

  • News & Views |

    Why do bulky anions solubilize macromolecules in water but precipitate out the corresponding monomers? The answer lies in the differences in local water structure. Polymers have now been shown to disrupt water structure more than their monomers, leading to an accumulation of anions near the polymers that increases their solubility.

    • Aniket U. Thosar
    •  & Amish J. Patel

  • Article |

    DNA-encoded libraries facilitate the discovery of ligands that interact with biomolecules but such technologies do not take full advantage of the principles of Darwinian selection. Now, libraries of conformationally constrained peptides (Dsuprabodies) have been assembled using a strategy that allows for iterative cycles of selection, amplification and diversification. This method was validated with selections against streptavidin and PD-L1.

    • Balayeshwanth R. Vummidi
    • , Lluc Farrera-Soler
    •  & Nicolas Winssinger

  • Article |

    In biological systems, controlled molecular motion along a particular path is realized by protein motors that travel along microtubule filaments. Now, control of motion with light has been achieved in a synthetic supramolecular system, in which anionic porphyrin molecules move along the fibres of a bis-imidazolium gel upon irradiation.

    • Mario Samperi
    • , Bilel Bdiri
    •  & David B. Amabilino

  • Article |

    Liquid–liquid phase separation plays an important role in creating cellular compartments and protocells, but designing small-molecule models remains difficult. A peptide-based synthon for liquid–liquid phase separation consisting of two stickers and a flexible, polar spacer has now been presented. Condensates formed by these synthons can concentrate biomolecules and catalyse anabolic reactions.

    • Manzar Abbas
    • , Wojciech P. Lipiński
    •  & Evan Spruijt

  • Article |

    Coulombic interactions can be used to assemble charged nanoparticles into higher-order structures, but this process typically requires similarly sized oppositely charged partners. Now, small anions or cations with as few as three charges have been shown to induce attractive interactions between oppositely charged nanoparticles in water, guiding the assembly of colloidal crystals.

    • Tong Bian
    • , Andrea Gardin
    •  & Rafal Klajn

  • News & Views |

    A new class of interwoven metal–organic containers, including one with a cubic architecture, twelve crossing points and a large internal volume, has now been reported. Interconversion between different self-assembled structures can be triggered by simply exchanging the associated anions.

    • Andrew W. Heard
    • , Natasha M. A. Speakman
    •  & Jonathan R. Nitschke

  • Article |

    Although many systems that involve protocell–protocell interactions have been developed, there are fewer reports of protocell–environment interactive systems. Now, helical hydrogel filaments—in which enzyme-containing proteinosomes are immobilized—have been shown to contract and expand as the local chemical environment changes. Enzyme processing regulates the chemomechanical responses to generate different modes of actuation in the soft microstructures.

    • Ning Gao
    • , Mei Li
    •  & Stephen Mann

  • Article |

    In atomic solids, substitutional doping is a powerful approach to modulating materials properties. Now, three substitutional mixtures of {Co6Se8} and {Cr6Te8} clusters in a crystal lattice with C60 fullerenes have been prepared. At two Co:Cr mixing ratios, the solid solutions showed particularly high electrical conductivities and low activation barriers for electron transport, owing to their structural heterogeneity.

    • Jingjing Yang
    • , Jake C. Russell
    •  & Colin Nuckolls

  • Article |

    Collagen-like peptides can self-assemble into hundreds of closely related triple helices. Now, an algorithm has been developed that predicts the most stable helix and the extent to which it will assemble to the exclusion of the competing helices. This information can help improve the understanding of triple helix design and assembly.

    • Douglas R. Walker
    • , Sarah A. H. Hulgan
    •  & Jeffrey D. Hartgerink

  • News & Views |

    The synthesis of molecular knots has been a major achievement in the field of chemical topology, but only a few relatively simple ones have been made so far. A route based on a weaving approach has now been used to make a seven-crossing knot and could offer a route to more complicated structures.

    • Dan Preston
    •  & Paul E. Kruger

  • Article |

    A combination of metal- and anion-template synthesis directs the weaving of molecular weft and warp strands in the assembly of a 3 × 3 interwoven grid. Connection of the ligand strands by alkene metathesis produces the topology of a seven-crossing endless knot, an important cultural and religious symbol.

    • David A. Leigh
    • , Jonathan J. Danon
    •  & Steffen L. Woltering

  • News & Views |

    Artificial photosynthesis represents a promising method of generating hydrogen for our clean and sustainable energy needs. Now, photocatalytic nanofibres have been developed that incorporate photosensitizers and catalysts into well-defined self-assembled structures for efficient hydrogen production.

    • Gregory I. Peterson
    • , Sanghee Yang
    •  & Tae-Lim Choi

  • Article |

    The majority of discrete structures obtained by self-assembly possess high symmetry, and thus low complexity: all subunits relate to their neighbours in a similar manner. Now, the spontaneous formation of complex low-symmetry assemblies produced from a single building block has been demonstrated using a systems chemistry approach. The single building block oligomerizes to form specific homomeric cyclic macromolecules that adopt a folded conformation.

    • Charalampos G. Pappas
    • , Pradeep K. Mandal
    •  & Sijbren Otto

  • Article |

    Nature successfully uses supramolecular assemblies for efficient and robust solar energy harvesting; however, mimicking such material systems for applications in optoelectronic devices has been hampered by stability issues such as the fragility of the supramolecular structures used and the delicate nature of Frenkel excitons. Now, enabled by tunable cage-like scaffolds, stable supramolecular light-harvesting nanotubes have been composed that are robust even under heat stress.

    • Kara Ng
    • , Megan Webster
    •  & Dorthe M. Eisele

  • News & Views |

    After years of speculation on the origins of symmetry-making and -breaking during crystallization, time-resolved in situ scanning probe microscopy and all-atom molecular dynamics simulations have shown that the formation of olanzapine crystals largely occurs by the incorporation of centrosymmetric dimers into growth sites.

    • Susan M. Reutzel-Edens

  • Article |

    Crystal symmetry is notoriously uncorrelated to the symmetry of the constituent molecules that make up a crystal. Symmetry breaking is typically thought to occur during nucleation and growth, but a symmetry element of olanzapine crystals—an inversion centre—has now been shown to emerge in centrosymmetric dimers extant in solution prior to crystallization.

    • Monika Warzecha
    • , Lakshmanji Verma
    •  & Peter G. Vekilov

  • Article |

    A six-helix bundle DNA structure called meta-DNA has now been assembled and shown to possess some structural properties similar to those of single-stranded DNA. Two meta-DNAs containing complementary ‘meta-base pairs’ are shown to form double helices. Meta-DNA building blocks are also used to construct a series of DNA architectures and to perform a hierarchical strand-displacement reaction.

    • Guangbao Yao
    • , Fei Zhang
    •  & Hao Yan

  • News & Views |

    Controlling the formation of ordered and predictable patterns in dissipative reaction–diffusion processes is challenging. Now, liquid vibrations induced by audible sound have been shown to direct the formation of spatiotemporal patterns in switchable chemical systems and assemblies.

    • Charalampos G. Pappas

  • Article |

    Patterns formed by artificial out-of-equilibrium chemical oscillating networks (such as the Belousov–Zhabotinsky reaction) are difficult to control with any precision. Now, it has been shown that low-intensity audible sound can be used to generate spatiotemporal patterns with a programmable distribution of redox- and pH-responsive chemical systems and supramolecular assemblies in solution.

    • Ilha Hwang
    • , Rahul Dev Mukhopadhyay
    •  & Kimoon Kim

  • Article |

    Reversible nanoscale knotting and unknotting of a molecular strand can be used to control the handedness of helical organizations at macroscopic length scales. Dopant knotted and unknotted strands induce supramolecular helical structures of opposite handedness in achiral liquid crystals, and the left- and right-handed forms can be switched in situ.

    • Nathalie Katsonis
    • , Federico Lancia
    •  & Fredrik Schaufelberger

  • News & Views |

    It’s not known how life’s essential properties of replication, metabolism and compartmentalization were first integrated. Two recent articles now shed light on how metabolic characteristics may be incorporated into replicating systems, harnessing an external energy source to increase their rate of replication and acquiring catalytic activity.

    • Pablo Solís-Muñana
    •  & Jack L. Y. Chen

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