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| Open AccessSwitchable supramolecular helices for asymmetric stereodivergent catalysis
Controlling multiple stereogenic centers in a single molecular scaffold represents a challenge for current switchable asymmetric catalysts. Here, the authors achieve asymmetric stereodivergency by means of a switchable supramolecular helical catalyst allowing all stereoisomers to be obtained with high and similar enantioselectivities.
- Ran Chen
- , Ahmad Hammoud
- & Matthieu Raynal
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Article
| Open AccessMechanically controlled multifaceted dynamic transformations in twisted organic crystal waveguides
Crystals with mechanical responses are of interest, but often only one or two dynamic motions can be achieved with one crystal. Here, the authors report a combination of dynamic movements in naturally twisted optical waveguiding microcrystals.
- Mehdi Rohullah
- , Vuppu Vinay Pradeep
- & Rajadurai Chandrasekar
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Article
| Open AccessVitrification-enabled enhancement of proton conductivity in hydrogen-bonded organic frameworks
Proton conduction is one of the interesting applications of hydrogen-bonded organic frameworks. Here, the authors report hydrogen-bonded organic framework that can be transformed into glassy state, effectively mitigating grain boundary effects, and significantly enhancing proton conduction performance.
- Feng-Fan Yang
- , Xiao-Lu Wang
- & Linfeng Liang
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Article
| Open AccessNested non-covalent interactions expand the functions of supramolecular polymer networks
Supramolecular polymer networks have unique and useful properties due to the reversible nature of their cross-links. Here, the authors show that when two distinct supramolecular interaction classes exist within a single cross-link, new functions can result.
- David J. Lundberg
- , Christopher M. Brown
- & Jeremiah A. Johnson
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Article
| Open AccessBulk transparent supramolecular glass enabled by host–guest molecular recognition
Strategies to produce supramolecular glass and the study of its intrinsic structure and mechanical properties remains largely unexplored. Here, the authors prepare a supramolecular glass via the host–guest recognition between methyl-β-cyclodextrin and para-hydroxybenzoic acid with recyclability, compatibility, and thermal processability.
- Changyong Cai
- , Shuanggen Wu
- & Shengyi Dong
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Article
| Open AccessCoordination cages integrated into swelling poly(ionic liquid)s for guest encapsulation and separation
The efficient encapsulation of guests by coordination cages in the solid state is prevented by their flexibility, dynamicity, and metal-ligand bond reversibility. Here, the authors report coordination cages integrated into poly(ionic liquid)s to control swelling and mechanical properties of the gels and develop efficient and regenerable supramolecular separation materials.
- Xiang Zhang
- , Dawei Zhang
- & Mingyuan He
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Article
| Open AccessCell-penetrating protein-recognizing polymeric nanoparticles through dynamic covalent chemistry and double imprinting
Molecular recognition of proteins is essential for achieving their biological functions but it is challenging to prepare selective protein-binding materials. Here the authors report a method that combines dynamic covalent chemistry and double molecular imprinting to construct protein-recognizing nanoparticles capable of specific inhibition of protein–protein interactions.
- Avijit Ghosh
- , Mansi Sharma
- & Yan Zhao
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Article
| Open AccessIsostructural doping for organic persistent mechanoluminescence
Organic mechanoluminescent materials have potential in a range of applications, but it can be challenging to achieve long-lived emission. Here, the authors report isostructural doping as a strategy to achieve multicolour and high efficiency organic mechanoluminescence, applied in stress sensing.
- Zongliang Xie
- , Yufeng Xue
- & Bin Liu
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Article
| Open AccessNoncovalent synthesis of homo and hetero-architectures of supramolecular polymers via secondary nucleation
Synthesis of supramolecular polymers with controlled architecture is desirable but challenging. Here, the authors use a secondary nucleation event to prepare a range of supramolecular polymer architectures.
- Srinu Kotha
- , Rahul Sahu
- & Kotagiri Venkata Rao
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Article
| Open AccessIn situ enzymatic control of colloidal phoresis and catalysis through hydrolysis of ATP
The design of synthetic systems that can sense chemical gradients and respond with directional motility and chemical activity is of interest. Here, the authors realize and control such behaviors in a synthetic system by tailoring multivalent interactions of adenosine nucleotides with catalytic microbeads.
- Ekta Shandilya
- , Bhargav Rallabandi
- & Subhabrata Maiti
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Article
| Open AccessHighly efficient in crystallo energy transduction of light to work
Crystals are known to have a range of responses to light, but multiple responses in the same material are rare. Here, the authors report different mechanical effects in response to light across three polymorphs as a result of a dimerization reaction.
- Jiawei Lin
- , Jianmin Zhou
- & Junbo Gong
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Article
| Open AccessProbing the surface charge of condensates using microelectrophoresis
The surface charge and ζ-potential of biomolecular condensates is key to their interactions with membranes and proteins. Here, the authors developed a method to determine the ζ-potential of condensates using microelectrophoresis and single-droplet tracking.
- Merlijn H. I. van Haren
- , Brent S. Visser
- & Evan Spruijt
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Article
| Open AccessSelenium catalysis enables negative feedback organic oscillators
Multiple autocatalytic reactions producing thiols are known, but negative feedback loop motifs are unavailable for thiol chemistry. Here, the authors develop a negative feedback loop based on the selenocarbonates, in which thiols induce the release of aromatic selenols that catalyze the oxidation of thiols by organic peroxides.
- Xiuxiu Li
- , Polina Fomitskaya
- & Sergey N. Semenov
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Article
| Open AccessAssembly of short amphiphilic peptoids into nanohelices with controllable supramolecular chirality
Helical protein assemblies are an important biological structure, but are challenging to mimic with synthetic materials. Here, the authors report the use of peptoids to form nanohelix structures with controllable supramolecular chirality.
- Renyu Zheng
- , Mingfei Zhao
- & Chun-Long Chen
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Article
| Open AccessHighly robust supramolecular polymer networks crosslinked by a tiny amount of metallacycles
Supramolecular polymeric materials have exhibited attractive features such as self-healing, reversibility and stimuli-responsiveness but because of the weak bonding nature of most noncovalent interactions, constructing supramolecular polymer materials with high robustness remains challenging. Here, the authors describe the construction of highly robust stimuli-responsive supramolecular polymer networks by using only a tiny amount of metallacycles as the supramolecular crosslinkers.
- Lang He
- , Yu Jiang
- & Shijun Li
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Article
| Open AccessConvoluted micellar morphological transitions driven by tailorable mesogenic ordering effect from discotic mesogen-containing block copolymer
Assembly of block copolymers can be controlled to give varying morphologies and functionalities, but there are still aspects of the process that are not well understood. Here, the authors report convoluted self-assembly behaviours of block copolymers with discotic liquid crystalline moieties.
- Huanzhi Yang
- , Yunjun Luo
- & Xiaoyu Li
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Article
| Open AccessSupramolecular polynuclear clusters sustained cubic hydrogen bonded frameworks with octahedral cages for reversible photochromism
The development of supramolecular porous crystalline frameworks with architectures from secondary building units remains challenging. Here, the authors report ammonium node-assembled clusters as supramolecular secondary building units to sustain a body centered cubic hydrogenbonded framework with octahedral cages for haloform encapsulation and reversible photochromism.
- Xiaojun Ding
- , Jing Chen
- & Gang Ye
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Article
| Open AccessChiral BINOL-phosphate assembled single hexagonal nanotube in aqueous solution for confined rearrangement acceleration
Supramolecular confined catalysis aims to mimic the active pocket of an enzyme to enhance the efficiency and selectivity of catalytic reactions. Here, the authors describe the formation of chiral nanotubes stable in aqueous solution employing a chiral BINOL-phosphate which can accelerate the 3-aza-Cope rearrangement by a nanotubular interior confinement effect.
- Kang Li
- , Wei-Min Qin
- & Yue-Peng Cai
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Article
| Open AccessDeveloping a machine learning model for accurate nucleoside hydrogels prediction based on descriptors
Supramolecular nucleoside-based hydrogels have potential in biomedical applications, but there is no model to predict what nucleoside derivatives will form hydrogels. Here, the authors report a machine learning model to predict the ability of nucleoside derivatives to form hydrogels.
- Weiqi Li
- , Yinghui Wen
- & Hang Zhao
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| Open AccessStructurally diverse macrocycle co-crystals for solid-state luminescence modulation
Organic co-crystals are useful in the fabrication of functional materials, but it is challenging to achieve structural diversity of co-crystals. Here, the authors report nine sets of macrocycle cocrystals with diverse structures and stoichiometric ratios giving different luminescence properties.
- Bin Li
- , Lingling Liu
- & Chunju Li
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Article
| Open AccessSqueezing formaldehyde into C60 fullerene
The interconversion of the two spin isomers of formaldehyd has been studied in the gas phase but has never been observed experimentally in the condensed phase. Here the authors report the encapsulation of formaldehyde inside C60 cages and observe spin-isomer conversion of the formaldehyde guest molecules in the cryogenic solid state.
- Vijyesh K. Vyas
- , George R. Bacanu
- & Richard J. Whitby
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Article
| Open AccessA molecular T-pentomino for separating BTEX hydrocarbons
Globally important BTEX hydrocarbons are separated using a T-shaped host with the shape and crystal tiling characteristics of a pentomino. A strategy based on designing and applying crystalline molecular ominos to perform separations of hydrocarbons and other environmentally-relevant compounds is outlined.
- Christopher J. Hartwick
- , Eric W. Reinheimer
- & Leonard R. MacGillivray
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| Open AccessDynamic mechanostereochemical switching of a co-conformationally flexible [2]catenane controlled by specific ionic guests
By virtue of the rotational motions of interlocked macrocycles, the authors describe a chameleon-like catenane host that can adjust its co-conformation for selective binding to copper(I) or sulfate ion. While the cationic copper(I) complex is achiral, the interlocked rings in the catenane host rotate and re-orient into a chiral co-conformation upon forming the anionic sulfate complex.
- Yueliang Yao
- , Yuen Cheong Tse
- & Ho Yu Au-Yeung
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Article
| Open AccessDynamic control of DNA condensation
Artificial biomolecular condensates are valuable tools to study the design principles of phase separation. Here, the authors demonstrate and characterize a model system of artificial DNA condensates whose kinetic formation and dissolution depends on DNA inputs that activate or deactivate the phase separating DNA subunits.
- Siddharth Agarwal
- , Dino Osmanovic
- & Elisa Franco
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Article
| Open AccessScalable production of structurally colored composite films by shearing supramolecular composites of polymers and colloids
Structurally coloured composite films are flexible optical materials with potential in a range of applications, but their production is impacted by long time-frames and limited materials. Here, the authors report a method for the production of large scale films by shearing supramolecular composites.
- Miaomiao Li
- , Bolun Peng
- & Jintao Zhu
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Article
| Open AccessMechanically interlocked [c2]daisy chain backbone enabling advanced shape-memory polymeric materials
Mechanically interlocked structures in polymer backbones can give interesting functionality, but can be challenging to prepare and control. Here, the authors report the development of polymers with a daisy chain unit in the backbone that are capable of shape memory behaviour.
- Shang-Wu Zhou
- , Danlei Zhou
- & Da-Hui Qu
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Article
| Open AccessSmart touchless human–machine interaction based on crystalline porous cages
Smart sensors are important components in the development of touchless human-machine interaction systems. Here, the authors describe a smart 3D porous crystalline organic cage-based system that exhibits remarkable responsiveness to fingertip humidity, contributing to the advancement of touchless human-machine interaction technology.
- Jinrong Wang
- , Weibin Lin
- & Niveen M. Khashab
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Article
| Open AccessComplexation-driven assembly of imine-linked helical receptors showing adaptive folding and temperature-dependent guest selection
The development of synthetic receptors capable of selectively binding monosaccharides is highly challenging. Here, authors present the efficient synthesis of these receptors based on foldamers, achieved through complexation-induced equilibrium shifting.
- Geunmoo Song
- , Seungwon Lee
- & Kyu-Sung Jeong
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Article
| Open AccessA general supramolecular strategy for fabricating full-color-tunable thermally activated delayed fluorescence materials
Thermally activated delayed fluorescence materials with full-colour tunability are desirable but challenging to prepare. Here, the authors report a method for preparing such materials through the design of host-guest cocrystals with through-space charge transfer.
- Nan Xue
- , He-Ye Zhou
- & Chuan-Feng Chen
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Article
| Open AccessCross-catenation between position-isomeric metallacages
The study of cross-catenated metallacages could provide facile insights into achieving more precise control over low-symmetry/high-complexity hierarchical assembly systems but is currently lacking. Here, the authors report a cross-catenane formed between two position-isomeric Pt(II) metallacages in the solid state.
- Yiliang Wang
- , Taotao Liu
- & Jun Li
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Article
| Open AccessSeparation of benzene and toluene associated with vapochromic behaviors by hybrid[4]arene-based co-crystals
Cocrystal engineering combined with macrocycle chemistry has allowed the development of materials with vapochromic characteristics. Here, the authors report the development of a macrocycle cocrystal for the separation of trace solvents.
- Jingyu Chen
- , Wenjie Zhang
- & Jiong Zhou
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Article
| Open AccessWater-stable boroxine structure with dynamic covalent bonds
Despite the structural significance of boroxines in different classes of materials, their applicability in aqueous media is limited by their hydrolytic instability. Here, the authors discovered a water-stable boroxine structure with excellent pH stability and water-compatible dynamic covalent bonds.
- Xiaopei Li
- , Yongjie Zhang
- & Guangyan Qing
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Article
| Open AccessVisualizing the interfacial-layer-based epitaxial growth process toward organic core-shell architectures
Organic heterostructures with controlled geometry on the micro and nanoscale are important in nanotechnology, but epitaxial growth processes with high lattice mismatching are challenging to achieve. Here, the authors report a visualisation process for morphology evolution on epitaxial growth.
- Ming-Peng Zhuo
- , Xiao Wei
- & Liang-Sheng Liao
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| Open AccessLight-responsive MXenegel via interfacial host-guest supramolecular bridging
Multifunctional composite hydrogels are promising candidates to develop smart and recyclable electronic components. Here, the authors report a reversible on-demand liquefication and solidification conductive gel formed by the self-assembly of photoresponsive host-guest complexes and MXene nanosheets which can be integrated into traditional solid-state circuits.
- Yu-Liang Lin
- , Sheng Zheng
- & Jiun-Tai Chen
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Article
| Open AccessBioinspired polymeric supramolecular columns as efficient yet controllable artificial light-harvesting platform
The formation of artificial light-harvesting systems with high donor/acceptor ratios for efficient energy transfer remains challenging. Here, the authors describe a polymeric supramolecular column-based light-harvesting system by modular columnar assembly of donor/acceptor chromophores, enabling superior light-harvesting efficiency and dynamic full-color tunable emission.
- Bin Mu
- , Xiangnan Hao
- & Wei Tian
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| Open AccessHydrogen bond unlocking-driven pore structure control for shifting multi-component gas separation function
C2H4 is one of the most important chemical raw materials. Here, the authors report that tuning of pore structure shifts the multi-component gas separation function, enabling one-step production of high-purity C2H4 in the quaternary mixture.
- Rong Yang
- , Yu Wang
- & Kai-Jie Chen
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Article
| Open AccessUncovering supramolecular chirality codes for the design of tunable biomaterials
Assembly of amyloids is important in neurodegenerative diseases, but there is limited understanding of how supramolecular chirality is controlled. Here, the authors report the design of peptide derivatives that allow chirality inversion at biologically relevant temperatures.
- Stephen J. Klawa
- , Michelle Lee
- & Ronit Freeman
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Article
| Open AccessSelf-similar chiral organic molecular cages
To enhance the utility of organic molecular cages (OMCs), the evolution of OMCs into higher-level chiral OMCs with self-similar superstructures is meaningful yet challenging. Here, the authors report a pair of higher-level 3D tri-bladed chiral helical molecular cages, displaying self-similarity in a discrete self-similar superstructure at different levels.
- Zhen Wang
- , Qing-Pu Zhang
- & Chuan-Feng Chen
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Article
| Open AccessSelf-assembled dendrimer polyamide nanofilms with enhanced effective pore area for ion separation
Membrane technology using well-defined pore structure enables high ion purity and recovery but achieving uniform pore structure and effective pore area is challenging. Here the authors introduce dendrimers that self-assemble, facilitating the formation of polyamide nanofilms with well-defined effective pore ranges and uniform pore structures.
- Bingbing Yuan
- , Yuhang Zhang
- & Q. Jason Niu
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Article
| Open AccessMultistate structures in a hydrogen-bonded polycatenation non-covalent organic framework with diverse resistive switching behaviors
Hydrogen-bonded organic frameworks as stimuli responsive multistate structures show potential in the field of resistive switching. Here, the authors report a 0D+1D hydrogen-bonded polycatenation non-covalent organic framework showing reversible transformation of multistate-structures triggered by electrical field and temperature, enabling reversibly switchable resistive random-access memory and write-once-read-many-times memory behavior.
- Shimin Chen
- , Yan Ju
- & Zhangjing Zhang
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Article
| Open AccessSelf-assembly of the smallest and tightest molecular trefoil knot
The synthesis of molecular knots remains challenging. Here, the authors report the synthesis of a chiral molecular trefoil metallaknot by self-assembly which contains only 54 atoms in the backbone.
- Zhiwen Li
- , Jingjing Zhang
- & Richard J. Puddephatt
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Article
| Open AccessAtomic-resolution structure analysis inside an adaptable porous framework
Single crystal X-ray diffraction is one of the most powerful structure elucidation tools, but it’s challenging to determine complex structures. Here the authors report a metal-organic framework for encapsulation and immobilization of various guests using highly ordered internal water network, obtaining high quality atomic-resolution data.
- Yuki Wada
- , Pavel M. Usov
- & Masaki Kawano
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Article
| Open AccessBiomimetic chiral hydrogen-bonded organic-inorganic frameworks
Assembly is an interesting strategy to build chiral hierarchies with premade properties and functionalities. Here, the authors present assembled chiral hydrogen-bonded organic-inorganic frameworks with dynamical chiroptical activities and employ them as powerful and recoverable platforms for enantioselective recognition of chiral aliphatic substrates.
- Jun Guo
- , Yulong Duan
- & Yi Liu
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Article
| Open AccessStoichiometry validation of supramolecular complexes with a hydrocarbon cage host by van ’t Hoff analyses
“van ’t Hoff, the first Nobel laureate, invented a double-arrow formalism to define equilibria in 1884. Here, the authors apply his accompanying method, the van ’t Hoff plot, to a modern problem to decide the stoichiometry of supramolecular complexes.”
- Toshiya M. Fukunaga
- , Yuzuka Onaka
- & Hiroyuki Isobe
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Article
| Open AccessSelective amide bond formation in redox-active coacervate protocells
Coacervate droplets are promising protocells that sequester nutrients, but how new peptides could be synthesized inside coacervates remains a mystery. Here, the authors develop redox-active coacervates that facilitate the formation of new peptide bonds.
- Jiahua Wang
- , Manzar Abbas
- & Evan Spruijt
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Article
| Open AccessSolvent-pair surfactants enabled assembly of clusters and copolymers towards programmed mesoporous metal oxides
A solvent-pair surfactants enabled assembly method is developed to achieve a general and programmable synthesis of mesoporous metal oxides via the association of POMs with block copolymers through indirect interaction.
- Wenhe Xie
- , Yuan Ren
- & Yonghui Deng
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Article
| Open AccessSite-selective chemical reactions by on-water surface sequential assembly
Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, the authors demonstrate the assembly of amino-substituted porphyrins on a water surface into J-aggregate structures in the presence of charged surfactants.
- Anupam Prasoon
- , Xiaoqing Yu
- & Xinliang Feng
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Article
| Open AccessThermally-induced atropisomerism promotes metal-organic cage construction
While heat modification is ubiquitous in biologic systems, it remains a significant challenge in artificial systems. Here the authors demonstrate thermal regulation of conversion between different rigid macrocycle atropisomers and related self-assemblies.
- Jiaqi Liang
- , Shuai Lu
- & Han-Yuan Gong
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Article
| Open AccessAnti-Kasha triplet energy transfer and excitation wavelength dependent persistent luminescence from host-guest doping systems
Anti-Kasha processes have potential in organic luminogens, but design of materials with these characteristics is challenging. Here, the authors report the development of a host-guest system with anti-Kasha behaviour and triplet energy transfer.
- Weiwei Xie
- , Wenbin Huang
- & Ben Zhong Tang