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Article
| Open AccessConstructing chemical stable 4-carboxyl-quinoline linked covalent organic frameworks via Doebner reaction for nanofiltration
Covalent linkages are the key component of covalent organic frameworks (COFs) and the development of stable and functional linkages is essential to broaden their application prospects. Here, the authors report the synthesis of crystalline and ultrastable 4-carboxyl-quinoline linked COFs via Doebner reactions in both one-pot and post-synthetic modification methods and demonstrate application of the COFs in nanofiltration.
- Yongliang Yang
- , Ling Yu
- & Yaqi Cai
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Article
| Open AccessOrigin of high thermal conductivity in disentangled ultra-high molecular weight polyethylene films: ballistic phonons within enlarged crystals
Oriented polymers may exhibit high thermal conductivity, but the upper limits remain unclear. Here, the authors show that heat-carrying phonons scatter primarily from crystalline domain boundaries in disentangled polyethylene films.
- Taeyong Kim
- , Stavros X. Drakopoulos
- & Austin J. Minnich
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Article
| Open AccessRemote and precise control over morphology and motion of organic crystals by using magnetic field
Elastic organic crystals are the materials foundation of future lightweight flexible electronic, optical and sensing devices, yet precise control over their deformation has not been accomplished. Here, the authors demonstrate rapid remote bending of organic crystals which are coupled to magnetic nanoparticles using magnetic field.
- Xuesong Yang
- , Linfeng Lan
- & Hongyu Zhang
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Article
| Open AccessMultiple yet switchable hydrogen-bonded organic frameworks with white-light emission
Switchable hydrogen-bonded frameworks have potential applications in the development of smart materials. Herein, the authors report eleven hydrogen-bonded organic frameworks and two non-porous structures that can undergo reversible structural and fluorescence switching; white-light emission is enabled.
- Yadong Shi
- , Shuodong Wang
- & Ben Zhong Tang
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Article
| Open AccessFully conjugated azacorannulene dimer as large diaza[80]fullerene fragment
Heterofullerenes are an important synthetic target for organic chemists. Here, the authors demonstrate a fully conjugated azacorannulene dimer starting from a bifunctional polycyclic aromatic azomethine ylide, providing a powerful method for the bottom-up synthesis of large multiazafullerene fragments
- Weifan Wang
- , Fiona Hanindita
- & Shingo Ito
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Article
| Open AccessHalogen hydrogen-bonded organic framework (XHOF) constructed by singlet open-shell diradical for efficient photoreduction of U(VI)
While hydrogen bonded organic frameworks are well covered in the scientific literature, halogen hydrogen-bonded organic framework (XHOF) remain less explored. Here, the authors demonstrate a highly stable diradical-based XHOF and demonstrate photoreduction of uranyl ions and high capacity of uranyl immobilization.
- Lijuan Feng
- , Yihui Yuan
- & Ning Wang
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Article
| Open AccessAnisotropic fluid with phototunable dielectric permittivity
Light stimuli are widely used to control material properties, yet it remains challenging to reversibly photocontrol the dielectric permittivity. Nishikawa et al. achieve this goal in an anisotropic fluid via its liquid crystal phase transition induced by isomerization of an azobenzene-tethered phototrigger.
- Hiroya Nishikawa
- , Koki Sano
- & Fumito Araoka
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Article
| Open AccessPushing detectability and sensitivity for subtle force to new limits with shrinkable nanochannel structured aerogel
The fabrication of pressure sensors with both ultralow detection limits and ultrahigh sensitivity is still challenging. Here, the authors propose a design strategy for fabricating a soft polysiloxane crosslinked MXene aerogel with multilevel nanochannels inside its cellular walls for ultrasensitive pressure detection.
- Xinlei Shi
- , Xiangqian Fan
- & Jiajie Liang
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Article
| Open AccessElectro-mechanically switchable hydrocarbons based on [8]annulenes
Pure hydrocarbons with properties that can be switched by external stimuli are interesting for the design and development of new responsive materials. Here, the authors develop an oligomeric [8]annulene-based material that combines topological switching upon redox changes with structural simplicity, stability, and straightforward synthesis.
- Magdalena Tasić
- , Jakov Ivković
- & Daniel Strand
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Article
| Open AccessSingle-component color-tunable circularly polarized organic afterglow through chiral clusterization
Circularly polarized organic afterglow (CPOA) with both long-lived room-temperature phosphorescence and circularly polarized luminescence is attracting great interest, but the development of multicolor-tunable CPOA in a single-component material remains challenging. Here, the authors report a strategy to achieve multicolor CPOA through chiral clusterization by inserting a chirality center into a non-conjugated organic cluster.
- Hui Li
- , Jie Gu
- & Runfeng Chen
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Article
| Open AccessBridging pico-to-nanonewtons with a ratiometric force probe for monitoring nanoscale polymer physics before damage
Understanding the transmission of nanoscale forces is important in polymer physics but physical approaches have limitations in analyzing the local force distribution in condensed environments. Here, the authors report a conformation flexible dual-fluorescent force probe and realize ratiometric analysis of the distribution of local forces in a stretched polymer chain network.
- Ryota Kotani
- , Soichi Yokoyama
- & Shohei Saito
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Article
| Open AccessPatterned crystal growth and heat wave generation in hydrogels
The crystallization of metastable liquid phase change materials releases stored energy upon nucleation. Here, the authors demonstrate area-selective activation of thermoresponsive processes by exothermic crystallization of sodium acetate into trihydrate crystals within a patterned polyacrylamide hydrogel.
- Thomas B. H. Schroeder
- & Joanna Aizenberg
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Article
| Open AccessSolid-state cooling by elastocaloric polymer with uniform chain-lengths
The elastocaloric effect was originally found in natural rubber, but the development of polymer based elastocaloric cooling still remains underdeveloped. Herein, the authors demonstrate that polymer elastomers with uniform molecular chain-lengths exhibit enormous elastocaloric effects through reversible conformational changes.
- Shixian Zhang
- , Quanling Yang
- & Qing Wang
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Article
| Open AccessSize compatibility and concentration dependent supramolecular host–guest interactions at interfaces
Quantification of supramolecular host–guest interactions is important for modulating supramolecular systems but accurately evaluating the adhesion energies of host–guest pairs remains challenging. Here, the authors directly quantify the interaction energies between cyclodextrin modified surfaces and ditopic adamantane using a surface force apparatus.
- Jintae Park
- , Jinwoo Park
- & Dong Woog Lee
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Article
| Open AccessSupramolecular tessellations by the exo-wall interactions of pagoda[4]arene
Supramolecular tessellation has gained increasing interest in supramolecular chemistry for its structural aesthetics and potential applications in optics, magnetics and catalysis. Here, the authors expand the examples of molecular building blocks for supramolecular tessellation and fabricate supramolecular tessellations using the exo-wall interactions of pagoda[4]arene.
- Xiao-Ni Han
- , Ying Han
- & Chuan-Feng Chen
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Article
| Open AccessA chemosensor-based chiral coassembly with switchable circularly polarized luminescence
‘Fluorescent chemisensors with fast response time and pronounced luminescence variation are important but have not been well investigated for self-assembled chiral systems. Here, the authors present a coassembled multiple component system that responds to SO2 derivatives, giving rise to dynamic aggregation behaviors and switchable luminescence as well as circularly polarized luminescence.
- Qiuhong Cheng
- , Aiyou Hao
- & Pengyao Xing
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Article
| Open AccessBottom-up modular synthesis of well-defined oligo(arylfuran)s
Oligofurans have attracted great attention because of their strong fluorescence, charge delocalization, and increased solubility. Here the authors show a bottom-up modular construction of chemically and structurally well-defined oligo(arylfuran)s by de novo synthesis of α,β′-bifuran monomers and late-stage bromination, stannylation and subsequent coupling reaction.
- Yang Chen
- , Pingchuan Shen
- & Shifa Zhu
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Article
| Open AccessEnabling three-dimensional porous architectures via carbonyl functionalization and molecular-specific organic-SERS platforms
Nanostructured films of organic semiconductors with low lying LUMO orbitals can enhance Raman signals via a chemical enhancement mechanism but currently the material choice is limited to fluorinated oligothiophenes. Here, the authors investigate the growth of a porous thienoacene film enabled by carbonyls and demonstrate molecular specific organic-SERS platforms.
- Ibrahim Deneme
- , Gorkem Liman
- & Hakan Usta
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Matters Arising
| Open AccessThe mechanism of bending in co-crystals of caffeine and 4-chloro-3-nitrobenzoic acid
- Amy J. Thompson
- , Jason R. Price
- & Jack K. Clegg
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Article
| Open AccessGenerating circularly polarized luminescence from clusterization‐triggered emission using solid phase molecular self-assembly
Organic cluster-triggered emission (CTE) displays promising application in bioimaging, chemical sensing, and multicolor luminescence but circular polarize luminescence derived from CTE remains less studied. Here, the authors demonstrate CTE based CPL emission from a supramolecular film derived from solid phase molecular self-assembly.
- Peilong Liao
- , Shihao Zang
- & Yun Yan
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Article
| Open AccessMechanochemical transformation of planar polyarenes to curved fused-ring systems
The transformation of planar aromatic molecules into non-planar structures is a challenging task and has not been realized by mechanochemistry before. Here, the authors demonstrate that mechanochemical forces can transform a planar polyarene into a curved geometry by creating new C-C bonds along the rim of the molecular structure.
- Teoh Yong
- , Gábor Báti
- & Mihaiela C. Stuparu
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Article
| Open AccessTempering of cocoa butter and chocolate using minor lipidic components
In chocolate production, a complicated tempering process is used to guide the crystallization of cocoa butter towards its most desirable polymorph, which gives the chocolate proper melting behavior, gloss, and snap—hallmarks of good quality chocolate. Here, the authors find that simply adding a specific phospholipid also directs crystallization towards this polymorph, producing chocolate with comparable microstructure and properties to tempered chocolate.
- Jay Chen
- , Saeed M. Ghazani
- & Alejandro G. Marangoni
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Article
| Open AccessA general design approach toward covalent organic frameworks for highly efficient electrochemiluminescence
Electrochemiluminescence (ECL) plays a key role in analysis and sensing but its application is limited by a lack of highly tunable luminophores. Here, the authors demonstrate the design of high efficient ECL luminophores of covalent organic frameworks (COFs) in aqueous media by simultaneously restricting the donor and acceptor to the COFs’ electron configurations and constructing charge transport networks through olefin linkages.
- Ya-Jie Li
- , Wei-Rong Cui
- & Jian-Ding Qiu
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Article
| Open AccessMolecular insertion regulates the donor-acceptor interactions in cocrystals for the design of piezochromic luminescent materials
The design of piezochromic luminescent materials with desirable stimuliresponsive properties remains challenging. Here, the authors report the insertion of a non-emissive molecule into a donor and acceptor binary cocrystal and realize desirable piezochromic luminescent properties by manipulation of intermolecular interactions between the donor and acceptor molecules.
- Chunguang Zhai
- , Xiu Yin
- & Bingbing Liu
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Article
| Open AccessBicyclo[2.2.0]hexene derivatives as a proaromatic platform for group transfer and chemical sensing
Cyclohexadienes have been widely explored as proaromatic surrogates for group transfer reactions but limited storage stability and difficult accessibility of these compounds limits the application range. Here, the authors present a class of proaromatic bicyclo[2.2.0]hexene derivatives and demonstrate their application in alkyl transfer reactions and sensing applications.
- Bin Wu
- , Jianing Wang
- & Rong Zhu
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Review Article
| Open AccessProtein nanofibrils for next generation sustainable water purification
Water scarcity is a rapidly spreading global challenge but water purification technologies are often not sustainable. Here, the authors review the research on water purification technologies based on protein nanofibrils as a green and affordable solution to alleviate a water crisis.
- Mohammad Peydayesh
- & Raffaele Mezzenga
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Article
| Open AccessBarrier-free reverse-intersystem crossing in organic molecules by strong light-matter coupling
Strong coupling of organic materials with optical cavities allows to manipulate the rate of energy transfer between their internal states. Here, the authors show a hybrid state of singlet character with energy lower than the triplet state, and a flow of energy from the triplet to the hybrid state.
- Yi Yu
- , Suman Mallick
- & Karl Börjesson
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Article
| Open AccessHierarchical communication of chirality for aromatic oligoamide sequences
Communication of chirality at a molecular level is the fundamental for transmitting chirality information but one-step communication modes in many artificial systems limits further processing the chirality information. Here, the authors report chirality communication of aromatic oligoamide sequences within interpenetrated helicate architecture in a hierarchical manner.
- Jiajia Zhang
- , Dan Luo
- & Quan Gan
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Article
| Open AccessOvertemperature-protection intelligent molecular chiroptical photoswitches
Realizing overtemperature protection with a molecular device is challenging. Here, the authors demonstrate an overtemperature protection function by integrating thermo- and photoresponsive functions into a pillar[6]arene based pseudocatanene.
- Jiabin Yao
- , Wanhua Wu
- & Cheng Yang
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Article
| Open AccessActive discovery of organic semiconductors
Existing methods for organic semiconductor computational screening are limited by the computational demand of the process, leading to the identification of non-optimal material candidates. Here, the authors report machine learning method to guide the discovery of organic semiconductors.
- Christian Kunkel
- , Johannes T. Margraf
- & Karsten Reuter
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Article
| Open AccessJ-aggregates of meso-[2.2]paracyclophanyl-BODIPY dye for NIR-II imaging
J-aggregation has been proved to be an efficient strategy for the development of fluorescent imaging agents in the NIR-II spectral region but the design of appropriate J-aggregates is challenging. Here, the authors demonstrate J-aggregation of a BODIPY dye with NIR-II emission and demonstrate lymph node imaging for fluorescence guided surgery.
- Kang Li
- , Xingchen Duan
- & Zhipeng Liu
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Article
| Open AccessUnexpected organic hydrate luminogens in the solid state
Developing organic photoluminescent materials with high emission efficiencies in the solid state under a water atmosphere is important for practical applications. Here, the authors report the formation of intra- and intermolecular hydrogen bonds in a tautomerizable Schiff base and intercalation of water in the crystal lattice leading to a luminescent organic hydrate.
- Feng Zhou
- , Peiyang Gu
- & Jianmei Lu
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Article
| Open AccessPredicting wavelength-dependent photochemical reactivity and selectivity
Predicting the conversion and selectivity of a photochemical reactions is challenging. Here, the authors introduce a framework for the quantitative prediction of the time-dependent progress of a photoligation reaction and predict LED-light induced conversion through a wavelength-resolved numerical simulation.
- Jan P. Menzel
- , Benjamin B. Noble
- & Christopher Barner-Kowollik
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Article
| Open AccessNear quantitative synthesis of urea macrocycles enabled by bulky N-substituent
Macrocycles are molecular structures extensively used in the design of catalysts, therapeutics and supramolecular assemblies but synthesis procedures that can produce macrocycles in high yield under high reaction concentrations are rare. Here the authors report the use of dynamic hindered urea bond for the construction of urea macrocycles with high efficiency.
- Yingfeng Yang
- , Hanze Ying
- & Jianjun Cheng
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Article
| Open AccessUltrastable liquid crystalline blue phase from molecular synergistic self-assembly
Blue phases are spatially ordered yet fragile liquid crystalline structures, bearing applications in optoelectronics and photonics. Hu et al. show that self-assembly within a mixture of different mesogens may significantly broaden the temperature range over which they are stable.
- Wei Hu
- , Ling Wang
- & Huai Yang
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Article
| Open AccessSelf-powered multifunctional sensing based on super-elastic fibers by soluble-core thermal drawing
Though thermal drawing methods are attractive for fabricating fiber-based sensor devices, existing methods allow limited access to low viscosity and low modulus materials. Here, the authors demonstrate a two-step soluble-core fiber fabrication method with wide applicability to soft polymer materials.
- Mengxiao Chen
- , Zhe Wang
- & Lei Wei
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Article
| Open AccessThermochromic aggregation-induced dual phosphorescence via temperature-dependent sp3-linked donor-acceptor electronic coupling
Aggregation-induced emission (AIE) has proven to be a viable strategy to achieve highly efficient room temperature phosphorescence (RTP) in bulk by restricting molecular motions. Here, the authors present an RTP design strategy by combining the concept of AIE and donor-acceptor motif and demonstrate unusual thermochromic dual phosphorescence.
- Tao Wang
- , Zhubin Hu
- & Guoqing Zhang
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Article
| Open AccessMolecular cannibalism: Sacrificial materials as precursors for hollow and multidomain single crystals
The coexistence of single-crystallinity with a multidomain morphology is a paradoxical crystallographic phenomenon. Here, the authors introduce a crystallographic morphology never reported before. The single-crystals with a curved and hollow morphology offer opportunities to generate a class of synthetic multidomain crystals.
- Maria Chiara di Gregorio
- , Merna Elsousou
- & Milko E. van der Boom
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Article
| Open AccessLighting up solid states using a rubber
Changes in molecular properties due to stimuli response are critically important for the development of new materials. However, most processes are slow or inefficient in the solid state. Here the authors demonstrate property switching in the solid state using a rubbing-induced tautomerism in multiple hydrogen-bonded donor-acceptor couples.
- Zhongyu Li
- , Yanjie Wang
- & Liangliang Zhu
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Article
| Open AccessFerroelectric columnar assemblies from the bowl-to-bowl inversion of aromatic cores
Organic ferroelectrics are of potential use in state-of-the-art ferroelectric devices but mechanistic insight in generating ferroelectricity remains limited. Here, the authors demonstrate that a bowl-to-bowl inversion of a bowl shaped organic molecule generates ferroelectric dipole relaxation, extending the concept of ferroelectricity in small organic molecules.
- Shunsuke Furukawa
- , Jianyun Wu
- & Tomoyuki Akutagawa
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Article
| Open AccessThe role of spin in the degradation of organic photovoltaics
The commercialisation of organic photovoltaic technology calls for research on material degradation mechanisms. Ramirez et al. show that triplet excitons produced by back charge transfer can significantly impact the photo-stability of fullerene-based devices even in the absence of water and oxygen.
- Ivan Ramirez
- , Alberto Privitera
- & Moritz Riede
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Article
| Open AccessThe coupling and competition of crystallization and phase separation, correlating thermodynamics and kinetics in OPV morphology and performances
Designing efficient blue perovskite LEDs by using mixed halides perovskite is still a challenge, limited mainly by the phase segregation issue. Here, the authors demonstrate in situ fabrication of quasi-2D CsPbClBr2 nanocrystal films with mixed ligands to overcome the constraint.
- Zaiyu Wang
- , Ke Gao
- & Feng Liu
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Article
| Open AccessElectrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces
N-heterocyclic carbenes (NHCs) have been widely used for the formation of monolayers but self-assembly methods come with drawbacks such as need for dry environment or using specifically-synthesized precursors. Here, the authors demonstrate an approach for surface-anchoring of NHCs which overcomes these limitations by using electrochemically-assisted deprotonation.
- Einav Amit
- , Linoy Dery
- & Elad Gross
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Article
| Open AccessSequentially amplified circularly polarized ultraviolet luminescence for enantioselective photopolymerization
Chiral functional materials with circularly polarized luminescence can be used in various applications but rarely reported. Here the authors show, a complex system, which show intense circularly polarized ultraviolet luminescence with large glum value, enabling a chiral UV light triggered enantioselective polymerization.
- Dongxue Han
- , Xuefeng Yang
- & Pengfei Duan
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Article
| Open AccessCharge-generating mid-gap trap states define the thermodynamic limit of organic photovoltaic devices
The inability to accurately measure the charge-generating energy states in organic solar cells makes elucidating the photovoltaic effect in these devices difficult. Here, the authors report charge-generating mid-gap trap states in organic solar cells via ultra-sensitive photovoltaic measurements.
- Nasim Zarrabi
- , Oskar J. Sandberg
- & Ardalan Armin
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Article
| Open AccessDesign of highly efficient deep-blue organic afterglow through guest sensitization and matrices rigidification
Though realizing organic materials with deep blue emission is attractive for next-generation display technologies, achieving this emission in afterglow molecules remains a challenge. Here, the authors report blue organic afterglow via a strategy involving guest sensitization and matrix rigidification.
- Shen Xu
- , Wu Wang
- & Wei Huang
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Article
| Open AccessPorous cage-derived nanomaterial inks for direct and internal three-dimensional printing
3D printing of nanomaterials generates opportunities to create advanced materials but printing of nanoparticles with intrinsic porosity has gained only little attention. Here, the authors demonstrate printing of silica nanocages using digital light processing to fabricate hierarchically porous parts with tunable internal structure and complex shapes.
- Tangi Aubert
- , Jen-Yu Huang
- & Ulrich Wiesner
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Article
| Open AccessGeometric pinning and antimixing in scaffolded lipid vesicles
Lipid bilayers feature an intricate interplay between membrane geometry and its chemical composition but lack of a model system with simultaneous control over membrane shape and composition prevented a fundamental understanding of curvature-induced effects. Here the authors demonstrate that the local substrate geometry and global chemical composition of the bilayer determine both the spatial arrangement and the sorting of lipid domains.
- Melissa Rinaldin
- , Piermarco Fonda
- & Daniela J. Kraft
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Article
| Open AccessOn demand shape memory polymer via light regulated topological defects in a dynamic covalent network
Stimuli-responsive soft materials are of interest for a range of applications. Here, the authors report on the use of light triggered catalysts to control topological defect driven isomerization of polymer networks and demonstrate application in shape memory polymers.
- Wusha Miao
- , Weike Zou
- & Tao Xie