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| Open AccessNon-solvent post-modifications with volatile reagents for remarkably porous ketone functionalized polymers of intrinsic microporosity
Chemical modification of porous materials is important for realising advanced applications, but often has a negative impact on other properties. Here, the authors report a method for the modification of polymers of intrinsic porosity to introduce a range of functional groups.
- Sirinapa Wongwilawan
- , Thien S. Nguyen
- & Cafer T. Yavuz
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Article
| Open AccessRealizing efficient blue and deep-blue delayed fluorescence materials with record-beating electroluminescence efficiencies of 43.4%
Thermally activated delayed fluorescence materials are important for the development of OLED materials but the development of robust blue emitting materials remains challenging. Here, the authors report three highly efficient blue and deepblue delayed fluorescence materials demonstrating excellent electroluminescence performance.
- Yan Fu
- , Hao Liu
- & Zujin Zhao
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| Open AccessAnomalous deep-red luminescence of perylene black analogues with strong π-π interactions
Perylene bisimide dyes are high-performance pigments that have red, maroon or black colors, but with typically only weak fluorescence in the solid state. Here, the authors report a series of π-stacked PBI derivatives that show highly efficient deep-red fluorescence in the solid state.
- Ningning Tang
- , Jiadong Zhou
- & Zengqi Xie
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Article
| Open AccessIn situ orderly self-assembly strategy affording NIR-II-J-aggregates for in vivo imaging and surgical navigation
J-aggregation, is an effective strategy to extend the wavelength of organic NIR-II fluorescence dyes but weak intermolecular interactions often lead to decomposition of the aggregates in biological environment. Here, the authors demonstrate a series of activatable quinazoline derivatives which can self-assemble in vivo into highly stable NIR-IIJ-aggregates.
- Zhe Li
- , Ping-Zhao Liang
- & Xiao-Bing Zhang
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| Open AccessAmyloid-polysaccharide interfacial coacervates as therapeutic materials
Liquid-liquid phase separation offer a strategy for targeting biomaterial scaffolds, but controlling assembly to form functional materials is challenging. Here, the authors transform native proteins into amyloid fibres for assembly, and use the materials as a gastric ulcer protective agent.
- Mohammad Peydayesh
- , Sabrina Kistler
- & Raffaele Mezzenga
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| Open AccessUnraveling two distinct polymorph transition mechanisms in one n-type single crystal for dynamic electronics
Cooperative transitions have acquired much attention for low transition barriers, ultrafast kinetics, and structural reversibility but cooperative transitions are rare in molecular crystals and their origin is poorly understood. Here the authors show that reorientation of the alkyl side chains in a 2-dimensional quinoidal terthiophene triggers cooperative behavior, and establish alkyl chain engineering to control the polymorphic behavior.
- Daniel William Davies
- , Bumjoon Seo
- & Ying Diao
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Article
| Open AccessObservation of Chiral-selective room-temperature phosphorescence enhancement via chirality-dependent energy transfer
Despite increasing interest in organic room temperature phosphorescence, it can still be challenging to determine mechanism and develop practical applications. Here, the authors report room temperature phosphorescent systems from chiral components, with strong phosphorescence observed only when both host and guest had the same chirality.
- Biao Chen
- , Wenhuan Huang
- & Guoqing Zhang
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Article
| Open AccessTwo-photon fluorescence imaging and specifically biosensing of norepinephrine on a 100-ms timescale
Norepinephrine (NE) is a key neurotransmitter in the central nervous system of organisms however specifically tracking the transient NE dynamics with high spatiotemporal resolution in living systems remains a great challenge. Herein, the authors developed a small molecular fluorescent probe that can precisely anchor on neuronal cytomembranes and specifically respond to NE on a 100-ms timescale.
- Leiwen Mao
- , Yujie Han
- & Yang Tian
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Article
| Open AccessMagnetically boosted 1D photoactive microswarm for COVID-19 face mask disruption
Most single-use face masks are made of synthetic plastics, thus their disposal poses a direct threat to wildlife as well as potential ecotoxicological effects in the form of microplastics. Here, the authors introduce a 1D magnetic photoactive microswarm capable of actively navigating, adhering to, and accelerating the degradation of the polypropylene microfiber of single-use face masks.
- Jeonghyo Kim
- , Carmen C. Mayorga-Martinez
- & Martin Pumera
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Article
| Open AccessPhotothermal bleaching of nickel dithiolene for bright multi-colored 3D printed parts
Most NIR radiation absorbers used in multi jet fusion 3D printing have an intrinsic dark color which prevents printing parts with variable colors. Here, the authors design an activating fusing agent containing a strong NIR absorbing dye that turns colorless after harvesting irradiation energy during the 3D printing process and provide a bright colored part when working with other color agents.
- Adekunle Olubummo
- , Lihua Zhao
- & Kyle Wycoff
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Article
| Open AccessMacromolecular sheets direct the morphology and orientation of plate-like biogenic guanine crystals
Animals precisely control the morphology and assembly of guanine crystals to produce diverse optical phenomena but little is known about how organisms regulate crystallization to produce optically useful morphologies. Here, the authors demonstrate that pre-assembled, fibrillar sheets in developing scallop eyes template nucleation and direct the growth and orientation of plate-like guanine crystals showing a striking resemblance to melanosome morphogenesis.
- Avital Wagner
- , Alexander Upcher
- & Benjamin A. Palmer
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Article
| Open AccessTautomerism unveils a self-inhibition mechanism of crystallization
Modifiers of diverse materials exhibit structures or compositions that differ from a solute molecule but often contain similar functional motifs that facilitate molecular recognition for modifier binding to crystal surfaces. Here the authors examine the intrinsic capability of tautomers, or structural isomers, to operate as crystal growth inhibitors.’
- Weiwei Tang
- , Taimin Yang
- & Jeffrey D. Rimer
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Article
| Open AccessMolecular-level enhanced clusterization-triggered emission of nonconventional luminophores in dilute aqueous solution
Luminophores based on clustering-triggered emission have drawn emerging attention in recent years but they tend to be nonluminescent in dilute solution. Here, the authors design novel clusteroluminogens through modification of cyclodextrin (CD) with amino acids to enable clusterization of chromophores in CD-based confined space and realize blue to cyan fluorescence even in the dilute solution.
- Qiuju Li
- , Xingyi Wang
- & Shun Mao
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Article
| Open AccessMicroporous organic nanotube assisted design of high performance nanofiltration membranes
Microporous organic nanotubes (MONs) hold considerable promise for designing molecular-sieving membranes because of high microporosity, customizable chemical functionalities, and favorable polymer affinity. Here, the authors report the usage of MONs derived from covalent organic frameworks to engineer 15-nm-thick microporous membranes via interfacial polymerization.
- Shuangqiao Han
- , Junyong Zhu
- & Menachem Elimelech
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Article
| Open AccessGuest-adaptive molecular sensing in a dynamic 3D covalent organic framework
Organic macrocycles and cages have been well-developed as porous solids for gas detection but balancing adaptability and robustness in these materials remains challenging. Here, the authors report a dynamic 3D covalent organic framework that can undergo concerted and adaptive structural transitions upon adsorption of gas and vapours.
- Lei Wei
- , Tu Sun
- & Yue-Biao Zhang
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| Open AccessElectrically conductive hybrid organic crystals as flexible optical waveguides
The poor conductivity of organic crystals hinders their potential on applications in flexible electronics, wearable devices, and soft robotics. Here, Naumov et al. develop a hybrid organic crystal that shows enhanced electrical conductivity and fast mechanical deformation due to temperature change.
- Xuesong Yang
- , Linfeng Lan
- & Hongyu Zhang
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Article
| Open AccessSwitchable Na+ and K+ selectivity in an amino acid functionalized 2D covalent organic framework membrane
Biological cell membranes can efficiently switch Na+/K+ selectivity in response to external stimuli but achieving analogous functions in a single artificial membrane is challenging. Here, the authors report highly crystalline covalent organic framework membranes with well-defined nanochannels and coordinative sites that act as ion-selective switches to manipulate Na+ and K+ transport.
- Li Cao
- , I-Chun Chen
- & Zhiping Lai
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| Open AccessPhotoprogrammable circularly polarized phosphorescence switching of chiral helical polyacetylene thin films
‘Pure organic room-temperature phosphorescence (RTP) materials with circularly polarized luminescence (CPL) gained increasing interest. Here, the authors propose a photoinduced circularly polarized RTP material by homogeneously dispersing phosphorescent chiral polyacetylenes into a processable polymer matrix.
- Zizhao Huang
- , Zhenyi He
- & Xiang Ma
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| Open AccessConstructing high-efficiency orange-red thermally activated delayed fluorescence emitters by three-dimension molecular engineering
The design of high-efficiency solution-processable orange-red thermally activated delayed fluorescence (TADF) emitters remains to be a challenge. Here, the authors synthesize a series of emitters consisting of a trinaphtho[3,3,3]propellane core with highly efficient emission in the orange-red region of the spectrum.
- Lei Hua
- , Yuchao Liu
- & Zhongjie Ren
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Article
| Open AccessUltrafast, autonomous self-healable iontronic skin exhibiting piezo-ionic dynamics
Sensing properties of the human skin are inspiring for the design of stretchable iontronics but achieving self-healing properties, elasticity and effective control of ion dynamics at the same time is challenging. Here, the Authors report a Cl-functionalized iontronic pressure sensitive material and realize good self-healing properties and mechanosensitive piezo-ionic dynamics.
- Elvis K. Boahen
- , Baohai Pan
- & Do Hwan Kim
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| Open AccessAn ionic vinylene-linked three-dimensional covalent organic framework for selective and efficient trapping of ReO4− or 99TcO4−
The synthesis of ionic olefin linked threedimensional covalent organic frameworks (3D COFs) is challenging because of the difficulties in forming stable carbon-carbon double bonds. Here, the authors report a general synthesis of an ionic sp2 carbon linked COFs and demonstrate selective capture of ReO4− ions.
- Cheng-Rong Zhang
- , Wei-Rong Cui
- & Jian-Ding Qiu
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| Open AccessA dish-like molecular architecture for dynamic ultralong room-temperature phosphorescence through reversible guest accommodation
Developing dynamic organic ultralong roomtemperature phosphorescence (URTP) remains challenging due to the difficulty in manipulating aggregate structures. Herein, the authors report a dish-like molecular architecture featuring guest responsive dynamic URTP.
- Wenlang Li
- , Qiuyi Huang
- & Zhenguo Chi
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Article
| Open AccessContinuous resin refilling and hydrogen bond synergistically assisted 3D structural color printing
3D photonic crystals (PCs) attract attention due to their unique optical properties but printing of colloidal particles is limited by lack of control over the assembly. Here, the authors demonstrate a continuous digital light processing 3D printing strategy using hydrogen bond assisted colloidal inks for fabricating well-assembled 3D PC structures.
- Yu Zhang
- , Lidian Zhang
- & Yanlin Song
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| Open AccessCovalent organic framework membranes for efficient separation of monovalent cations
Membrane technology holds great promise in separating monovalent cations but the sub-nanometer ion size and the small difference in ion size makes separation of monovalent cations a challenging task. Here, the authors demonstrate the efficient separation of monovalent cations using a COF membrane.
- Hongjian Wang
- , Yeming Zhai
- & Zhongyi Jiang
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Article
| Open AccessAmplification of integrated microscopic motions of high-density [2]rotaxanes in mechanically interlocked networks
Amplifying molecular motion to macroscopic material property is attractive but challenging. Here, the authors report mechanically interlocked networks with dense rotaxane backbones whose microscopic motion is integrated into decent mechanical properties of bulk materials.
- Xue Yang
- , Lin Cheng
- & Xuzhou Yan
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| Open AccessPhotodimerization induced hierarchical and asymmetric iontronic micropatterns
Hierarchical surface micro/nanopatterns enable iontronic materials to show performance enhancement in piezoionic mechanoreception and skin-interfaced coupling electrode adhesion. Here, the author proposes a facile and robust method to fabricate hierarchical and asymmetrical iontronic micropatterns through programmed regulation of the internal stress distribution and local ionic migration.
- Zehong Wang
- , Tiantian Li
- & Xuesong Jiang
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Article
| Open AccessEctopic expression of sericin enables efficient production of ancient silk with structural changes in silkworm
Transgenic modification of silkworms has the potential to engineer new silks with a wider range of properties. Here, the authors engineered the expression of the outer layer sericin SER3 in the inner fibroin layer generating a new silk with higher production efficiency and resistance to alkaline conditions.
- Xuedong Chen
- , Yongfeng Wang
- & Shiqing Xu
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Article
| Open AccessAmbipolar blend-based organic electrochemical transistors and inverters
Ambipolar organic electrochemical transistors simplify bioelectronics circuitry but are challenging due to complicated material design and synthesis. Here, the authors demonstrate that p- and n-type blends offer a simple and tuneable approach for the fabrication of ambipolar devices and circuits.
- Eyal Stein
- , Oded Nahor
- & Gitti L. Frey
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| Open AccessFluorescence-based thermal sensing with elastic organic crystals
A mechanically compliant and robust sensing material is essential for accurate and reliable thermal sensing. Here, the authors report the use of elastic organic crystals as fluorescence-based thermal sensors that cover a wide range of temperatures with complete retention of the sensor’s elasticity.
- Qi Di
- , Liang Li
- & Hongyu Zhang
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| Open AccessSmall-molecule ionic liquid-based adhesive with strong room-temperature adhesion promoted by electrostatic interaction
Low-molecular-weight adhesives (LMWAs) possess many unique features compared to polymer adhesives but fabrication of LMWAs with adhesion strengths higher exceeding those of polymeric materials is a significant challenge. Here, the authors propose an ionic liquid based thin coating adhesive with high adhesion strength.
- Jun Zhang
- , Wenxiang Wang
- & Shiguo Zhang
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| Open AccessMicrospheres from light—a sustainable materials platform
Photopolymerization provides a safe and mild fabrication pathway towards polymeric particles but the implementation of photochemistry from solution to dispersed media to produce particles is far from trivial. Here, the authors demonstrate an additive-free step-growth photopolymerization with sunlight, exploiting the photoinduced Diels-Alder to fabricate micrometer sized polymeric particles.
- Laura Delafresnaye
- , Florian Feist
- & Christopher Barner-Kowollik
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Article
| Open AccessDynamically stable and amplified circularly polarized excimer emission regulated by solvation of chiral co-assembly process
Chiral supramolecular assembly is an important strategy for the development of excellent circularly polarized luminescent (CPL)-active materials, but often they suffer from low quantum yield and luminescence dissymmetry factor. Herein, the authors we report a chiral coassembly process of achiral pyrene-based dyes leading to chiral excimers emitting with a high dissymmetry factor.
- Yuxia Zhang
- , Hang Li
- & Yixiang Cheng
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| Open AccessUltralong organic phosphorescence from isolated molecules with repulsive interactions for multifunctional applications
Despite great success in generation of ultralong organic phosphorescence (UOP) by suppressing non-radiative transitions through attractive interactions, consideration of repulsive interactions on UOP remains largely unexplored. Here, the authors introduce carboxyl groups into organic phosphors, enabling formation of the intense repulsive interactions between the isolated molecules and the matrix in rigid environment.
- Xiaokang Yao
- , Huili Ma
- & Zhongfu An
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| Open Access3D printing colloidal crystal microstructures via sacrificial-scaffold-mediated two-photon lithography
Colloidal crystals are widely applied in the fabrication of optoelectronic devices, but realizing freedom of design, such as in 3D printing, in colloidal crystal fabrication remains challenging. Here, the authors demonstrate a sacrificial-scaffold-mediated two-photon lithography strategy that enables the fabrication of complex 3D colloidal crystal microstructures with orderly arranged nanoparticles in the bulk.
- Keliang Liu
- , Haibo Ding
- & Zhongze Gu
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Article
| Open AccessTailoring thermal insulation architectures from additive manufacturing
Nanoscale porous building blocks hold great promise for a range of thermal management technologies but often porous nanoparticle assemblies are intrinsically brittle. Here, the authors report 3D printing of porous silica voxels with polymeric additives to enable the coupling between additive manufacturing and hierarchical assembly for superior machinability and structural controllability.
- Lu An
- , Zipeng Guo
- & Shenqiang Ren
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Article
| Open AccessFluorescence turn on amine detection in a cationic covalent organic framework
Ionic covalent organic frameworks (iCOFs) are new examples of porous materials and show great potential for various applications. Here, the authors demonstrate functionalization of an iCOFs with suitable emission sites and application as chemosensor for amine detection with high sensitivity which can be used to monitor meat spoilage.
- Gobinda Das
- , Bikash Garai
- & Ali Trabolsi
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| Open AccessPhoto-thermo-induced room-temperature phosphorescence through solid-state molecular motion
The development of non-invasive, rapid responsive phosphorescence is highly desirable but has rarely been described. Herein, the authors designed and prepare a series of molecular rotors containing a room temperature phosphorescence active triazine core and three bromobiphenyl units acting as rotors and demonstrate light stimulus triggered phosphorescence.
- Xing Wang Liu
- , Weijun Zhao
- & Ben Zhong Tang
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Article
| Open AccessLight-intensity-dependent photoresponse time of organic photodetectors and its molecular origin
Understanding the charge trapping mechanism in organic semiconductors is crucial to design molecules for high-performance organic photodetectors. Labanti et al. systematically investigate the impact of donor molecular structure on the energetic disorder that affects both shallow and deep trap formation.
- Chiara Labanti
- , Jiaying Wu
- & Ji-Seon Kim
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Article
| Open AccessSecondary through-space interactions facilitated single-molecule white-light emission from clusteroluminogens
Although mature and systematic theories of molecular photophysics have been developed, it is still challenging to endow clusteroluminogens (CLgens) with designed photophysical properties by manipulating through-space interactions. Here, the authors design three CLgens that show multiple emissions and white-light emission in the crystalline state, and emphasize the important role of secondary through-space interactions between the acceptor and non-conjugated donor units.
- Jianyu Zhang
- , Parvej Alam
- & Ben Zhong Tang
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Article
| Open AccessLight-activated photodeformable supramolecular dissipative self-assemblies
Dissipative self-assembly can serve as a controllable platform to exhibit temporal processes for various non-stimulus responsive properties but construction of light-fueled dissipative self-assembly structures with transformable morphology to modulate non-photoresponsive properties remains a challenge. Here, the authors report a light-activated photodeformable dissipative self-assembly system in aqueous solution as metastable fluorescent platform.
- Xu-Man Chen
- , Wei-Jie Feng
- & Quan Li
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Article
| Open AccessDynamic self-stabilization in the electronic and nanomechanical properties of an organic polymer semiconductor
Organic polymer nanomechanics has been explored through precise nanometre-scale stiffness measurements in a high-mobility semiconducting polymer. Higher eigen-mode atomic force microscopy is used to measure nanomechnical variations in the film texture, as well as the nanoscale order in the material.
- Illia Dobryden
- , Vladimir V. Korolkov
- & Deepak Venkateshvaran
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Article
| Open AccessTwo-colour light activated covalent bond formation
Dual-wavelength photochemical systems open up new avenues for novel lithographic techniques but currently only few wavelength-orthogonal photoreactive compounds undergoing reversible photoreaction are known. Here, the authors exploit cis/trans photoisomerization of azobenzenes and demonstrate photoligation of the cis state with a photochemically generated ketene.
- Sarah L. Walden
- , Leona L. Rodrigues
- & Christopher Barner-Kowollik
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| Open AccessSeeing structural evolution of organic molecular nano-crystallites using 4D scanning confocal electron diffraction (4D-SCED)
Studying organic molecular nanocrystals with electron microscopy has been challenging due to complex structures and radiation sensitivity. Here, the authors present 4D-scanning confocal electron diffraction, and demonstrate direct in situ observation of structural evolution of bulk heterojunction thin films.
- Mingjian Wu
- , Christina Harreiß
- & Erdmann Spiecker
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Article
| Open AccessSynthesis and macrocyclization-induced emission enhancement of benzothiadiazole-based macrocycle
Organic luminescent materials attract attention due to their wide application range, but many organic luminogens suffer from severe quenching effect in the aggregate state. Here, the authors demonstrate a macrocyclization induced emission enhancement by linking luminophores through methylene bridges to give a macrocycle.
- Shuo Li
- , Kun Liu
- & Chunju Li
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Article
| Open AccessControllable multiple-step configuration transformations in a thermal/photoinduced reaction
Solid-state photochemical reactions of olefinic compounds provide access to organic cyclic molecules with specific configurations but the precise control of the stereochemistry in these reactions remains challenging. Here, the authors demonstrate control of the regiospecific configurations of C=C groups and the intermediates by varying temperatures in multi-step thermal and photoinduced ring opening and closing reactions using a single-crystal coordination polymer platform.
- Meng-Fan Wang
- , Yan Mi
- & Jian-Ping Lang
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Article
| Open AccessExceptionally high work density of a ferroelectric dynamic organic crystal around room temperature
Organic electronics requires dynamic materials, however, most of them have small strokes and operate at high temperatures. Here, the authors describe organic crystal that repeatedly expands and contracts nearly half its length around room temperature.
- Durga Prasad Karothu
- , Rodrigo Ferreira
- & Panče Naumov
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Article
| Open AccessIntegrating charge mobility, stability and stretchability within conjugated polymer films for stretchable multifunctional sensors
Conjugated polymers are promising semiconductors for stretchable electronic devices but combining important properties such as high charge mobility, stability and stretchability remains challenging. Here, the authors demonstrate the synthesis of a thiophene based semiconducting polymer with cleavable side chains which shows significant improvement of charge mobility, stability and stretchability.
- Sung Yun Son
- , Giwon Lee
- & Wei You
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Article
| Open AccessClustering and halogen effects enabled red/near-infrared room temperature phosphorescence from aliphatic cyclic imides
Pure organic room temperature phosphorescence (RTP) materials become increasingly important but achieving red and near-infrared (NIR) RTP remains challenging. Here, the authors demonstrate that succinimide derived cyclic imides can emit RTP in the red and NIR spectral range with outstanding efficiencies of up to 9.2%.
- Tianwen Zhu
- , Tianjia Yang
- & Wang Zhang Yuan
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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