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| 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 AccessEnabling robust blue circularly polarized organic afterglow through self-confining isolated chiral chromophore
The preparation of systems that give blue circularly polarised organic afterglow is desirable but challenging. Here, the authors confine a chiral chromophore within a polymer matrix to limit non-radiative transitions and give blue circularly polarised organic afterglow.
- Mingjian Zeng
- , Weiguang Wang
- & Wei Huang
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Article
| Open AccessVapor-induced phase-separation-enabled versatile direct ink writing
The extrusion-based three-dimensional printing of polymers, metals, and composites requires elevated temperatures and may lead to diverse undesirable defects on printed parts. Here, the authors develop a vapor-induced phase separation printing technique to construct polymeric, metallic, and composite parts by using a polymer as a binder.
- Marc Sole-Gras
- , Bing Ren
- & Yong Huang
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Article
| Open AccessKinetically controlled metal-elastomer nanophases for environmentally resilient stretchable electronics
Metal-elastomer nanophases are critical for stretchable electronics but face mixing challenges. This study introduces a kinetic method for precise mixing, yielding gyrified nanophases with improved durability and strain-invariant conductivity, which holds promise for resilient stretchable devices.
- Soosang Chae
- , Won Jin Choi
- & Tae Il Lee
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Article
| Open AccessFine-tuning the pore environment of ultramicroporous three-dimensional covalent organic frameworks for efficient one-step ethylene purification
The construction of three-dimensional covalent organic frameworks for gas separation is challenging due to the similar physicochemical properties of the gas mixture. Here, the authors report functional three-dimensional covalent organic frameworks by fine-tunning the pore environment with pyridine units to achieve effective separation of ethane from ethylene.
- Yang Xie
- , Wenjing Wang
- & Cheng Wang
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Article
| Open AccessClosed-loop recycling of sulfur-rich polymers with tunable properties spanning thermoplastics, elastomers, and vitrimers
Sulfur-rich polymers are promising candidates for chemical recycling but lack efficient synthetic strategies for achieving diverse structures. Here, the authors report a synthesis strategy for polytrithiocarbonates which is compatible with a wide range of monomers enabling diverse structures via polycondensation of dithiols and dimethyl trithiocarbonate.
- Jin-Zhuo Zhao
- , Tian-Jun Yue
- & Wei-Min Ren
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Article
| Open AccessArtificial kagome lattices of Shockley surface states patterned by halogen hydrogen-bonded organic frameworks
By utilizing the templating effect of a halogen hydrogen-bonded organic framework, the authors show that the Shockley surface states of coinage metals can be patterned into artificial kagome lattices with high tunability.
- Ruoting Yin
- , Xiang Zhu
- & Bing Wang
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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 AccessLong lifetimes white afterglow in slightly crosslinked polymer systems
It is challenging to achieve multicolor long-lived room temperature phosphorescence in intrinsic polymers, especially for white afterglow. Here, the authors report a strategy to obtain pure white afterglow micro-crosslinked polymers by covalently coupling different conjugated chromophores with precursors through a simple and rapid one-pot reaction.
- Qingao Chen
- , Lunjun Qu
- & Chaolong Yang
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Article
| Open AccessA Janus carbaporphyrin pseudo-dimer
Carbaporphyrin dimers, known for their interesting photophysical properties and application in metal-organic chemistry, generally contain two identical subunits. Here, the authors highlight the benefits that can accrue from breaking the inherent symmetry of carbaporphyrin dimers and details a new approach to creating heterobimetallic complexes.
- Haodan He
- , Jiyeon Lee
- & Xian-Sheng Ke
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Article
| Open AccessIntegrated mechanical computing for autonomous soft machines
Many mechanical computation platforms developed till date lack a rational design strategy and have limited computational functions, such as stand-alone single logic gates, or deformation/transition behaviors. Byun at al. have reported a systematic design principle for integrated mechanical computing that enables the electronics-free design of autonomous and intelligent soft machines, which are seamlessly integrated.
- Junghwan Byun
- , Aniket Pal
- & Metin Sitti
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Article
| Open AccessDiffusion-rate sieving of propylene and propane mixtures in a cooperatively dynamic porous crystal
Porous coordination polymers (PCPs) are commonly used in gas separation processes but developing PCPs that work at high temperatures and feature both high uptake capacity and selectivity remains challenging. Here, the authors report diffusion-rate sieving of propylene/propane at 300 K by constructing a PCP whose global and local dynamics cooperatively govern the adsorption process via gate opening for propylene and diffusion regulation for propane.
- Yan Su
- , Ken-ichi Otake
- & Cheng Gu
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Article
| Open AccessA modular organic neuromorphic spiking circuit for retina-inspired sensory coding and neurotransmitter-mediated neural pathways
The distinctive interdependence in mixed ionic-electronic conductors emulates retinal pathway. Here, the authors develop a modular organic neuromorphic spiking circuit to replicate the interdependent functions of receptors, neurons and synapses that are chemically modulated by neurotransmitters.
- Giovanni Maria Matrone
- , Eveline R. W. van Doremaele
- & Yoeri van de Burgt
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Article
| Open AccessPhoto-modulated activation of organic bases enabling microencapsulation and on-demand reactivity
Oil-water emulsion techniques can be used for encapsulation of chemicals and control of reactivity, but is challenging for highly reactive materials such as acids and bases. Here, the authors report the encapsulation of bases by masking of reactivity with photo-removable protecting groups.
- Wenle Li
- , Xiaocun Lu
- & Nancy R. Sottos
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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 AccessUltrathin organosiloxane membrane for precision organic solvent nanofiltration
The use of membranes under harsh conditions, particularly involving the separation of complex organic solvents, remains challenging. Here the authors demonstrate an ultrathin organosiloxane polymer membrane using initiated chemical vapor deposition to effectively separate solutes within the molecular weight range of 150–300 g mol−1.
- Jihoon Choi
- , Keonwoo Choi
- & Dong-Yeun Koh
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Article
| Open AccessQuantitative, high-sensitivity measurement of liquid analytes using a smartphone compass
Smartphone cameras have been widely used for analysis purposes, but the use of magnetometers in smartphones is limited in this regard. In this study, the authors present a smartphone analyte sensor platform that utilizes the built in magnetometer to directly translate signals through analyte-responsive magnetic-hydrogel composites.
- Mark Ferris
- & Gary Zabow
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Article
| Open AccessCatalytic polymer self-cleavage for CO2 generation before combustion empowers materials with fire safety
Overcoming this challenge of fire hazards by carbon, hydrogen, and oxygen rich materials remains challenging. Here, the authors demonstarte that catalytic polymer auto-pyrolysis before combustion releases CO2, equipping the material with fire retardant properties.
- Wei Luo
- , Ming-Jun Chen
- & Hai-Bo Zhao
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Article
| Open AccessAnomalous anti-Kasha excited-state luminescence from symmetry-breaking heterogeneous carbon bisnanohoops
It is a long-standing scientific controversy to achieve anti-Kasha emissions by tuning structures at a molecular level. Herein, the authors constructed two symmetry-breaking heterogeneous carbon bisnanohoops with unusual anti-Kasha characteristics.
- Xinyu Zhang
- , Cheng Chen
- & Pingwu Du
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Article
| Open AccessEngineering the pore environment of antiparallel stacked covalent organic frameworks for capture of iodine pollutants
Radioiodine capture from nuclear fuel waste and contaminated water sources is of environmental importance but technically challenging. Here, the authors report covalent organic frameworks with antiparallel eclipsed stacked structures with dynamic adsorption performance for iodine pollutants under various conditions.
- Yinghui Xie
- , Qiuyu Rong
- & Xiangke Wang
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Article
| Open AccessSilk fibroin hydrogel adhesive enables sealed-tight reconstruction of meniscus tears
Suture repair is the current clinical treatment for meniscus tears, but inaccessible tears in company with re-tears susceptibility remain unresolved. Here the authors address these issues by developing a meniscus adhesive-based strategy for the seamless and dense reconstruction of torn meniscus.
- Xihao Pan
- , Rui Li
- & Hongwei Ouyang
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Article
| Open AccessDirect observation of phase transitions in truncated tetrahedral microparticles under quasi-2D confinement
Boundary conditions can give rise to new types of phases during self-assembly. Here the authors show that tetrahedral particles can form a hexagonal phase on a surface, that can transform into a quasi-diamond phase under a gravitational field.
- David Doan
- , John Kulikowski
- & X. Wendy Gu
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Article
| Open AccessProgramming mechanics in knitted materials, stitch by stitch
Knitted fabrics are prized for their stretchability, breathability, and long-wearability in everyday life. This study combines experiments and simulations to present a micromechanical approach to understanding the origin of the anisotropic elasticity of four canonical patterns of knitted fabrics.
- Krishma Singal
- , Michael S. Dimitriyev
- & Elisabetta A. Matsumoto
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Article
| Open AccessThermodynamic driving forces in contact electrification between polymeric materials
Contact electrification is a widely observed phenomenon in nature and in materials. Here, the authors use molecular dynamics simulations to show the importance of thermodynamic driving forces in contact electrification in insulating materials.
- Hang Zhang
- , Sankaran Sundaresan
- & Michael A. Webb
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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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Article
| Open AccessNucleic-acid-base photofunctional cocrystal for information security and antimicrobial applications
Cocrystal engineering is a promising strategy for constructing multifunctional materials. Here, the authors describe nucleic-acid-base cocrystal systems with different colors of phosphorescence from their monomeric counterparts and high-temperature phosphorescence with antimicrobial effects and data encryption applications.
- Wenqing Xu
- , Guanheng Huang
- & David Lee Phillips
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Article
| Open AccessHeight-renderable morphable tactile display enabled by programmable modulation of local stiffness in photothermally active polymer
The controllability of deformation height in reconfigurable touch displays currently limits their deliverable information. Hwang et al. present a light-triggered morphable tactile display enabling generation of refreshable, height-adjustable, and latchable 3D topologies with varying textures on a thin film surface.
- Inwook Hwang
- , Seongcheol Mun
- & Sungryul Yun
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Article
| 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 AccessSub-8 nm networked cage nanofilm with tunable nanofluidic channels for adaptive sieving
Drawing inspiration from biological cell membranes, here, the authors create sub-8 nm membranes with adaptive nanofluidic channels, mimicking the cell membrane properties, by interconnecting 0D nanoporous molecules at the oil/water interface.
- Si-Hua Liu
- , Jun-Hao Zhou
- & Jian-Ke Sun
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Review Article
| Open AccessLight-driven polymer recycling to monomers and small molecules
Chemical recycling of plastic enables renewed production of pristine materials, but generally comes at a high energy cost. This review focuses on light-driven approaches for chemically recycling and upcycling plastic waste, with emphasis on reduced energy consumption and selective transformations of challenging to recycle backbone structures.
- Laura Wimberger
- , Gervase Ng
- & Cyrille Boyer
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Article
| Open AccessEncoding ordered structural complexity to covalent organic frameworks
Starting from simple building blocks with specific molecular packing geometries, here, the authors synthesized structurally complex covalent organic framework COF-305 with nine different stereoisomers of its constituents showing specific sequences on topologically equivalent sites.
- Lei Wei
- , Xinyue Hai
- & Yingbo Zhao
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Article
| Open AccessLight and matter co-confined multi-photon lithography
Mask-free multi-photon lithography allows the straightforward fabrication of nanostructures, but high precision and good resolution can be challenging to achieve. Here, the authors report a combination of photo-inhibition and chemical quenchers for improved lithography performance.
- Lingling Guan
- , Chun Cao
- & Xu Liu
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Article
| Open AccessBiobased and biodegradable films exhibiting circularly polarized room temperature phosphorescence
Sustainable materials with circularly polarized room-temperature phosphorescence are desirable but challenging to design. Here, the authors report the development of thin films, based on cellulose nanocrystals and lignosulfonate, with circularly polarised room temperature phosphorescence.
- Mengnan Cao
- , Yiran Ren
- & Zhijun Chen
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Article
| Open AccessElectrothermally controlled origami fabricated by 4D printing of continuous fiber-reinforced composites
Effective active origami capable of on-demand modulation are limited by challenges such as limited load-bearing capacity and transformable states. Here, authors report fiber-reinforced composites for controlled electrothermal origami with excellent mechanical performance and spatiotemporal controllability.
- Yaohui Wang
- , Haitao Ye
- & Yi Xiong
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Article
| Open AccessSupra-biological performance of immobilized enzymes enabled by chaperone-like specific non-covalent interactions
Designing complex synthetic materials for enzyme immobilization could unlock the utility of biocatalysis in extreme environments. Here, the authors report on random copolymer brushes as dynamic immobilization supports that enable supra-biological catalytic performance of immobilized enzymes.
- Héctor Sánchez-Morán
- , Joel L. Kaar
- & Daniel K. Schwartz
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Article
| Open AccessDouble charge flips of polyamide membrane by ionic liquid-decoupled bulk and interfacial diffusion for on-demand nanofiltration
Currently polyamide membranes fabricated by interfacial polymerization are limited by inherently negative charge as well as narrow charge tailoring window restricting the application of these membranes. Here, the authors report a facile ionic liquid-decoupled bulk/interfacial diffusion strategy to fabricate polyamide membranes which can transform on-demand from inherently negative to highly positive and near-neutral charge.
- Bian-Bian Guo
- , Chang Liu
- & Zhi-Kang Xu
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Article
| Open Access3D printing by stereolithography using thermal initiators
Common stereolithography-based 3D printing relies on photopolymerization using photoinitiators. Here, the authors replace the conventional photoinitiators with low-cost, widely used thermal initiators to achieve 3D-printed objects.
- Doron Kam
- , Omri Rulf
- & Shlomo Magdassi
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Article
| Open AccessMolecular sieving of iso-butene from C4 olefins with simultaneous high 1,3-butadiene and n-butene uptakes
The efficient separation of iso-butene, an important raw material in chemical industry, remains challenging due to similar molecular properties of C4 olefins. Here, the authors report a sulfate-pillared adsorbent for the molecular sieving of iso-C4H8 from C4H6 and n-C4H8 with good benchmark uptake ratios and Henry’s selectivities.
- Junhui Liu
- , Hanting Xiong
- & Jun Wang
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Article
| Open AccessComplete separation of benzene-cyclohexene-cyclohexane mixtures via temperature-dependent molecular sieving by a flexible chain-like coordination polymer
The separation and purification of C6 cyclic hydrocarbons by thermal distillation is an energy intensive process which may be replaced by alternative energy-efficient adsorptive techniques. Here, the authors report a chain-like coordination polymer which facilitates complete separation of benzene, cyclohexene, and cyclohexane via an ideal molecular sieving mechanism.
- Feng Xie
- , Lihang Chen
- & Jing Li
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Article
| Open AccessMolecular near-infrared triplet-triplet annihilation upconversion with eigen oxygen immunity
Molecular triplet-triplet upconversion is useful in a wide range of applications, but is limited by significant oxygen quenching. Here the authors report the combination of sensitiser and annihilator that is stable in aerated environments, and suitable for in vivo sensing.
- Xinyu Wang
- , Fangwei Ding
- & Guanying Chen
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Article
| Open AccessAbnormal thermally-stimulated dynamic organic phosphorescence
In thermally stimulated phosphorescent materials a thermal stimulus inevitably quenches the emission due to intensive non radiative transition. Here, the authors report an abnormal thermally stimulated phosphorescence behavior in organic phosphors and show enhancement of phosphorescence and change of the emission color upon temperature increase.
- He Wang
- , Huili Ma
- & Zhongfu An
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Article
| Open AccessUltrafast underwater self-healing piezo-ionic elastomer via dynamic hydrophobic-hydrolytic domains
Elastomers capable of autonomous self-healing and mechanical stimulus sensing in aquatic environments are interesting for applications in underwater soft electronics. Here, the authors present a hydrophobic-hydrolytic molecularly engineered self-healing piezo-ionic elastomer with underwater self-healing properties and mechanosensitive ion channels.
- Zhengyang Kong
- , Elvis K. Boahen
- & Do Hwan Kim
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Article
| Open AccessEffect of inorganic material surface chemistry on structures and fracture behaviours of epoxy resin
The mechanisms of adhesion between polymers and inorganic materials are not fully understood. Here, authors demonstrate the clear evidence that the surface chemistry impacts the crosslinked structures of resins near the interfaces, resulting in different fracture behaviours and adhesive strengths.
- Tomohiro Miyata
- , Yohei K. Sato
- & Hiroshi Jinnai
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Article
| Open AccessWater-dispersible X-ray scintillators enabling coating and blending with polymer materials for multiple applications
Water dispersible X-ray scintillators are highly desirable for multiple application scenarios. Zhang et al report the synthesis of new X-ray scintillator nanocrystals anchored on the surface of water dispersible halloysite nanotubes, enabling radiation exposure monitoring, flexible scintillator screens, and information encryption.
- Hailei Zhang
- , Bo Zhang
- & Richard Hoogenboom
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Article
| 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 AccessSequence-dependent material properties of biomolecular condensates and their relation to dilute phase conformations
How material properties affect the functional state of biocondensates is a long-standing question. Here the authors demonstrate how such properties are encoded in a disordered protein sequence and can be predicted from dilute phase conformations.
- Dinesh Sundaravadivelu Devarajan
- , Jiahui Wang
- & Jeetain Mittal
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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 AccessIn-vivo integration of soft neural probes through high-resolution printing of liquid electronics on the cranium
Neural systems are often bulky and heavy. Here, the authors produce a conformable neural interface for mice using liquid metals directly printed on the skull that can monitor neural activities with long-term stability.
- Young-Geun Park
- , Yong Won Kwon
- & Jang-Ung Park