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| Open AccessAccelerating the discovery of insensitive high-energy-density materials by a materials genome approach
The synthesis of explosive materials that are stable, highly dense, and have low sensitivity to external stimuli is a challenge. Here, the authors use a genomic approach to accelerate the discovery of insensitive high explosive molecules with good detonation and low sensitivity properties.
- Yi Wang
- , Yuji Liu
- & Yong Tian
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Article
| Open AccessSystematic design of superaerophobic nanotube-array electrode comprised of transition-metal sulfides for overall water splitting
Water splitting by nanostructured, abundant catalysts provides a renewable means to make carbon neutral fuels, but the ideal material morphology and composition remain uncertain. Here, the authors prepare superaerophobic, multi-metallic sulfide nanotube arrays as bifunctional water splitting catalysts.
- Haoyi Li
- , Shuangming Chen
- & Xun Wang
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Article
| Open AccessTailoring exciton and excimer emission in an exfoliated ultrathin 2D metal-organic framework
Two dimensional (2D) metal-organic frameworks have demonstrated unique photophysical properties compared to their bulk analogs. Here, the authors demonstrate that exfoliation of 2D MOFs can suppress interlayer exciton-related emission, allowing for modulation of the overall emission color and switching of optical memory states.
- Wei-Ming Liao
- , Jian-Hua Zhang
- & Cheng-Yong Su
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Article
| Open AccessOut-of-equilibrium microcompartments for the bottom-up integration of metabolic functions
Generating artificial cells able to carry out metabolic activities out-of-equilibrium is a current challenge in synthetic biology. Here the authors use a microfluidic platform for integration and analysis of minimal metabolic reactions in artificial microcompartments formed of water-in-oil droplets.
- Thomas Beneyton
- , Dorothee Krafft
- & Jean-Christophe Baret
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Article
| Open AccessRecipes for improper ferroelectricity in molecular perovskites
In layered inorganic materials lattice distortions can couple to break inversion symmetry and drive improper ferroelectricity, but in perovskites, symmetry prohibits such an effect. Here, the authors use group-theoretical analysis to provide crystal engineering design principles for improper ferroelectricity in molecular perovskites.
- Hanna L. B. Boström
- , Mark S. Senn
- & Andrew L. Goodwin
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Article
| Open AccessLiquid phase blending of metal-organic frameworks
The recently introduced glass and liquid states of metal–organic frameworks (MOFs) provide opportunities to design and explore new properties for this class of material. Here, the authors show that a MOF liquid can be blended with another MOF component to produce domain-structured MOF glasses with single, tailorable glass transitions.
- Louis Longley
- , Sean M. Collins
- & Thomas D. Bennett
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Article
| Open AccessOn-surface synthesis of poly(p-phenylene ethynylene) molecular wires via in situ formation of carbon-carbon triple bond
Incorporating carbon-carbon triple bonds into conjugated chains typically requires acetylenic precursors. Here, the authors synthesize poly(p-phenylene ethynylene) molecular wires on Cu(111) by directly coupling trichloromethyl-containing precursors, forming C-C triple bonds in situ
- Chen-Hui Shu
- , Meng-Xi Liu
- & Pei-Nian Liu
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Article
| Open AccessControlled synthesis of highly-branched plasmonic gold nanoparticles through peptoid engineering
Peptoids are promising crystallization agents, as they offer the molecular recognition capabilities of proteins and peptides but with higher stability and synthetic tunability. Here, the authors show that sequence-defined peptoids can controllably template the formation and shape evolution of gold nanostructures with defined morphologies.
- Feng Yan
- , Lili Liu
- & Chun-Long Chen
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Article
| Open AccessTopologically frustrated dynamics of crowded charged macromolecules in charged hydrogels
Diffusion of molecules in crowded environment is important for various living systems, but the dynamics of charged molecules in charged matrices remains still unexplored. Here the authors report a dynamics of DNA and polyelectrolytes in a charged hydrogel where the guest molecules do not diffuse but experience topologically frustrated dynamics.
- Di Jia
- & Murugappan Muthukumar
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Article
| Open AccessCrosslinking of fibrous hydrogels
Unlike synthetic hydrogels, biological gels are made of fibrous networks which give rise to unique properties, such as high porosity and mechanical responsiveness. Here the authors use polyisocyanide-based gels and selectively crosslink inside the bundles to lock the fibrous network and thus control the architecture and the mechanics.
- Daniël C. Schoenmakers
- , Alan E. Rowan
- & Paul H. J. Kouwer
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Article
| Open AccessTransient modes of zeolite surface growth from 3D gel-like islands to 2D single layers
While zeolites are industrially relevant as molecular sieves and catalysts, their growth mechanisms remain widely debated. Here, Rimer and colleagues probe the crystallization pathway of zeolite LTA with spatiotemporal resolution, identifying a distinctive nonclassical pathway, and demonstrating that growth is highly dependent on synthetic conditions.
- Manjesh Kumar
- , Madhuresh K. Choudhary
- & Jeffrey D. Rimer
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Article
| Open AccessCross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites
Two-dimensional, organic-inorganic hybrid perovskites have sustained research interest due to attractive optoelectronic and excitonic properties. Here, Guo et al. systematically investigate coherent acoustic phonon transport versus layer thickness in these materials with strong acoustic impedance mismatch
- Peijun Guo
- , Constantinos C. Stoumpos
- & Richard D. Schaller
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Article
| Open AccessNanoparticle-templated nanofiltration membranes for ultrahigh performance desalination
Nanofiltration membranes are important for water desalination technologies, but designing membranes that achieve both high permeance and high salt rejection remains challenging. Here, the authors use sacrificial nanoparticles in the membrane fabrication process, leading to crumpled structures with ultrahigh permeance.
- Zhenyi Wang
- , Zhangxin Wang
- & Jian Jin
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Article
| Open AccessHigh-resolution AFM structure of DNA G-wires in aqueous solution
DNA and RNA G-quadruplexes can stack to form higher-order structures called G-wires. Here the authors report high-resolution AFM images of higher-order DNA G-quadruplexes in aqueous solution that could impact the design of G-wire based nanodevices and the understanding of G-wires in biology.
- Krishnashish Bose
- , Christopher J. Lech
- & Anh Tuân Phan
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Article
| Open AccessRevealing isoelectronic size conversion dynamics of metal nanoclusters by a noncrystallization approach
How metal nanoclusters evolve in size is poorly understood, particularly at the atomic level. Here, the authors use mass spectrometry to study the size conversion dynamics between two isoelectronic gold nanoclusters with atomic resolution, revealing that the growth reaction proceeds through a distinct balanced equation.
- Qiaofeng Yao
- , Victor Fung
- & Jianping Xie
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Article
| Open AccessHollow organic capsules assemble into cellular semiconductors
Perylene diimide-bithiophene macrocycles are electroactive and shape-persistent hosts. Here, the authors describe their self-assembly into a cellular organic semiconducting film whose voids are electrically sensitive to different guests, and which can function as the active layer in a field-effect transistor device.
- Boyuan Zhang
- , Raúl Hernández Sánchez
- & Colin Nuckolls
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Article
| Open AccessNanographenes as electron-deficient cores of donor-acceptor systems
Nanographenes in donor-acceptor π-systems generally serve as electron-donating moieties but the reversed structures are hardly reported. Here, the authors present a facile synthetic protocol towards reversed donor-acceptor nanographenes by amination and demonstrate fine property tuning by varying the donating ability of the aniline groups.
- Yu-Min Liu
- , Hao Hou
- & Klaus Müllen
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Article
| Open AccessEmergent superconductivity in an iron-based honeycomb lattice initiated by pressure-driven spin-crossover
Up to now, all iron-based high-Tc superconductors contain a square iron lattice. Here, Wang et al. report the observation of superconductivity in an iron honeycomb lattice accompanied with pressure-driven spin-crossover, in-plane lattice collapse and insulator-metal transition.
- Yonggang Wang
- , Jianjun Ying
- & Ho-kwang Mao
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Article
| Open AccessSelf-organizing layers from complex molecular anions
Using ions of one polarity to form functional layers on surfaces is usually challenging because of counter ions which are inevitably present in the condensed phase. Here the authors demonstrate accumulation of mass-selected anions and neutral molecules from the gas phase to form a self-organizing liquid-like layer on a surface.
- Jonas Warneke
- , Martin E. McBriarty
- & Julia Laskin
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| Open AccessSculpting and fusing biomimetic vesicle networks using optical tweezers
Assembly of higher-order artificial vesicles can unlock new applications. Here, the authors use optical tweezers to construct user-defined 2D and 3D architectures of chemically distinct vesicles and demonstrate inter-vesicle communication and light-enabled compartment merging.
- Guido Bolognesi
- , Mark S. Friddin
- & Yuval Elani
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Article
| Open AccessLight-driven transformable optical agent with adaptive functions for boosting cancer surgery outcomes
The combination of imaging techniques in cancer treatment often involves a trade-off in properties due to the opposite working mechanisms. Here, the authors report on a material that avoids the trade-off by switching from photoacoustic imaging to fluorescence imaging upon an external light trigger
- Ji Qi
- , Chao Chen
- & Ben Zhong Tang
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Article
| Open AccessSupramolecular Kandinsky circles with high antibacterial activity
Nested structures are common throughout nature and art, yet remain challenging synthetic targets in supramolecular chemistry. Here, the authors design multitopic terpyridine ligands that coordinate into nested concentric hexagons, and show that these discrete supramolecules display potent antimicrobial activity.
- Heng Wang
- , Xiaomin Qian
- & Xiaopeng Li
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Article
| Open AccessA self-destructive nanosweeper that captures and clears amyloid β-peptides
Cerebral amyloid β-peptide accumulation is a causative factor in Alzheimer’s Disease. Here the authors design a 'nanosweeper' that binds amyloid β-peptide and induces autophagy to clear the accumulated plagues.
- Qiang Luo
- , Yao-Xin Lin
- & Hao Wang
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| Open AccessIn-situ visualization of solute-driven phase coexistence within individual nanorods
Compared to thin films and other geometries, nanorods can exhibit particularly high performance in solute-intercalation-based energy and information storage devices. Here, the authors use in situ electron microscopy and spectroscopy to study the hydrogenation of palladium nanorods, revealing relationships between nanorod structure and device cyclability and capacity.
- Fariah Hayee
- , Tarun C. Narayan
- & Jennifer A. Dionne
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Article
| Open AccessTopologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers
The separation of C6 alkane isomers is crucial to the petroleum refining industry, but the distillation methods in place are energy intensive. Here, the authors design a series of topologically-guided zirconium-based metal-organic frameworks with optimized pore structures for efficient C6 alkane isomer separations.
- Hao Wang
- , Xinglong Dong
- & Jing Li
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Article
| Open AccessA modular synthetic approach for band-gap engineering of armchair graphene nanoribbons
Effective band-gap engineering of armchair graphene nanoribbons calls for control over both width and edge structure. Here, the authors report a modular synthesis of narrow N = 6 armchair graphene nanoribbons whose edges can be unsymmetrically modified with heteroarenes, introducing a simple way to tune band gap.
- Gang Li
- , Ki-Young Yoon
- & Guangbin Dong
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Article
| Open AccessChemical diversity in a metal–organic framework revealed by fluorescence lifetime imaging
Metal-organic frameworks are typically characterized by a variety of techniques, but most only provide information on properties as an average of a bulk sample. Here, Wuttke and colleagues demonstrate that fluorescence imaging and lifetime analysis allows access to local information on defects and functional groups.
- Waldemar Schrimpf
- , Juncong Jiang
- & Stefan Wuttke
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Article
| Open AccessA phase transformable ultrastable titanium-carboxylate framework for photoconduction
Porous TiO2 materials are attractive for energy-related applications owing to their accessible active sites, but suffer from poor stability. Here the authors synthesize a highly stable and porous metal–organic framework containing polymeric 1D Ti–O subunits, which displays a high condensation degree and high photoconductivity.
- Sujing Wang
- , Takashi Kitao
- & Christian Serre
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Article
| Open AccessBio-inspired nano-traps for uranium extraction from seawater and recovery from nuclear waste
Uranium extraction is important for both uranium recovery and nuclear waste management. Here, inspired by the high sensitivity of proteins towards specific metal ions, Ma and colleagues demonstrate that introducing secondary coordination spheres into amidoxime-functionalized porous polymers can enhance their uranyl chelating abilities.
- Qi Sun
- , Briana Aguila
- & Shengqian Ma
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Article
| Open AccessThe effect of crystallite size on pressure amplification in switchable porous solids
Pressure amplification phenomena have recently been observed in ordered mesoporous solids, but little is understood about this counter-intuitive behaviour. Here, Kaskel and colleagues demonstrate that crystal size can play an important role in modulating pressure amplification in metal-organic frameworks.
- Simon Krause
- , Volodymyr Bon
- & Stefan Kaskel
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Article
| Open AccessSpontaneous formation of gold nanostructures in aqueous microdroplets
Reactions in aqueous microdroplets can significantly differ from those in bulk. Here, the authors report microdroplets that not only accelerate gold nanoparticle formation by several orders of magnitude but also promote spontaneous nanostructure formation with no reducing agents or template.
- Jae Kyoo Lee
- , Devleena Samanta
- & Richard N. Zare
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Article
| Open AccessUnderstanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling
Understanding host–guest interactions and structural changes within porous materials is crucial for enhancing gas storage properties. Here, the authors combine cryogenic loading of gases with high pressure crystallography and computational techniques to obtain atomistic detail of adsorption-induced structural and energetic changes in ZIF-8.
- Claire L. Hobday
- , Christopher H. Woodall
- & Stephen A. Moggach
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Article
| Open AccessComputer-aided discovery of a metal–organic framework with superior oxygen uptake
The emergence of thousands of metal–organic frameworks (MOFs) has created the challenge of finding promising structures for particular applications. Here, the authors present a tool for computer-aided material discovery where a large number of MOFs are screened, with the top-ranked structure synthesized for oxygen storage applications.
- Peyman Z. Moghadam
- , Timur Islamoglu
- & David Fairen-Jimenez
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Article
| Open AccessChirality-controlled crystallization via screw dislocations
Understanding why and how molecules transfer their chirality into helical superstructures, including crystals, remains a challenge. Here, the authors show that topological defects not only promote the growth, but also control the helical morphology of crystals formed by chiral rod-shaped particles.
- Baeckkyoung Sung
- , Alexis de la Cotte
- & Eric Grelet
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Article
| Open AccessMetal-organic frameworks for precise inclusion of single-stranded DNA and transfection in immune cells
Non-viral vectors are important for transfection but can be limited in the uptake, protection and release of ssDNA. Here, the authors report on the design of metal-organic-framework vectors with precisely controlled pore geometry and demonstrate the vector in the transfection of immune cells.
- Shuang Peng
- , Binglin Bie
- & Xiang Zhou
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Article
| Open AccessChemical tunnel-splitting-engineering in a dysprosium-based molecular nanomagnet
Suppression of quantum tunneling in molecular magnets is key for their magnetic behaviours to be exploitable. Here, the authors show that tuning the geometry of lanthanide single-ion magnets leads to a suppression of the quantum tunneling, finding a three-fold reduction of the tunnel splitting upon changing the crystal field symmetry.
- Mikkel A. Sørensen
- , Ursula B. Hansen
- & Jesper Bendix
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Article
| Open AccessAdsorption-based atmospheric water harvesting device for arid climates
Harvesting water from the atmosphere is an important solution to water scarcity, but doing so in arid climates is highly challenging. Here, the authors develop a metal-organic framework-based water harvesting device that can deliver over 0.25 L of water per kg of adsorbent over a single cycle at relative humidities of 10–40% and at subzero dew points.
- Hyunho Kim
- , Sameer R. Rao
- & Evelyn N. Wang
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Article
| Open AccessElementary steps in electrical doping of organic semiconductors
Molecular doping is routinely used in organic semiconductor devices nowadays, but the physics at play remains unclarified. Tietze et al. describe it as a two-step process and show it costs little, energetically, to dissociate charge transfer complexes due to energetic disorder of organic semiconductors.
- Max L. Tietze
- , Johannes Benduhn
- & Karl Leo
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Article
| Open AccessExplosive dissolution and trapping of block copolymer seed crystallites
The study of the dissolution of polymer crystals is a challenging task. Here the authors use crystallization-driven self-assembly of coil-crystalline block copolymers as a trapping technique to track the change in length of 1D seed crystallites during annealing.
- Gerald Guerin
- , Paul A. Rupar
- & Mitchell A. Winnik
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Article
| Open AccessBiomimetic artificial organelles with in vitro and in vivo activity triggered by reduction in microenvironment
The efficacy of stimuli-responsive enzyme delivery systems is usually limited to in vitro applications. Here the authors form artificial organelles by inserting stimuli-responsive protein gates in membranes of polymersomes loaded with enzymes and obtain a triggered functionality both in vitro and in vivo.
- T. Einfalt
- , D. Witzigmann
- & C. G. Palivan
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Article
| Open AccessPlasma dye coating as straightforward and widely applicable procedure for dye immobilization on polymeric materials
Dye coating techniques for colored materials are often cost intensive or cause degradation of the material during processing. Here the authors demonstrate a fast, scalable and cost efficient plasma dye coating procedure, which allows for covalent immobilization of dye molecules on different polymer surfaces.
- Lieselot De Smet
- , Gertjan Vancoillie
- & Richard Hoogenboom
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Article
| Open AccessSpin-liquid-like state in a spin-1/2 square-lattice antiferromagnet perovskite induced by d10–d0 cation mixing
Quantum spin liquids are predicted to form in frustrated square lattice magnets but this has been difficult to verify experimentally. Here the authors show that cation mixing in the square perovskite Sr2Cu(Te0.5W0.5)O6 can be used to tune it into the spin liquid regime.
- O. Mustonen
- , S. Vasala
- & M. Karppinen
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Article
| Open AccessSurface plasmon resonance extension through two-block metal-conducting polymer nanorods
Localized surface plasmon resonance can be exploited for a range of applications, but remains difficult to tailor in metal-organic nanostructures. Here the authors synthesize gold-polypyrrole nanorods and observe a unique extended surface plasmon resonance, which they find to be tunable through doping.
- Insub Jung
- , Minkyung Kim
- & Sungho Park
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Article
| Open AccessCation vacancy stabilization of single-atomic-site Pt1/Ni(OH)x catalyst for diboration of alkynes and alkenes
Development of single-atomic-site catalysts with high metal loading remains a challenge. Here, the authors report a nickel hydroxide nanoboard with abundant Ni2+ vacancy defects serving as the support to achieve high platinum loading by simple wet impregnation.
- Jian Zhang
- , Xi Wu
- & Yadong Li
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Article
| Open AccessUltra-thin enzymatic liquid membrane for CO2 separation and capture
Porous membranes show great promise for CO2 separation and capture, but are currently limited by a trade-off between permeance and selectivity. Here, the authors fabricate a bio-inspired, ultra-thin enzymatic liquid membrane that displays exceptional CO2 permeability and selectivity under ambient conditions.
- Yaqin Fu
- , Ying-Bing Jiang
- & C. Jeffrey Brinker
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Article
| Open AccessThe role of confined collagen geometry in decreasing nucleation energy barriers to intrafibrillar mineralization
Nucleation in highly confined gaps shows distinctly different behavior from nucleation in extrafibrillar spaces. Here, using in situ X-ray scattering and classical nucleation theory, the authors show how confined geometry reduces energy barriers to intrafibrillar mineralization of collagen.
- Doyoon Kim
- , Byeongdu Lee
- & Young-Shin Jun
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Article
| Open AccessHighly stretchable carbon aerogels
Improved compressive elasticity was lately demonstrated for carbon aerogels but the problem of reversible stretchability remained a challenge. Here the authors use a hierarchical structure design and synergistic effects between carbon nanotubes and graphene to achieve high stretchability in carbon aerogels.
- Fan Guo
- , Yanqiu Jiang
- & Chao Gao
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Article
| Open AccessEffect of friction on oxidative graphite intercalation and high-quality graphene formation
Scalable graphene production from graphite via an intercalation-oxidation-reduction process is still hampered by low reproducibility and many lattice defects. Here, the authors show that reducing molecular friction by using highly crystalline graphite and mild oxidizing conditions is the key to high quality graphene.
- Steffen Seiler
- , Christian E. Halbig
- & Siegfried Eigler
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Article
| Open AccessQuantum and electrochemical interplays in hydrogenated graphene
Electrochemically-gated graphene field-effect transistors show promise for sensing of charged species in real time. Here, the authors leverage the interplay between electrical in-plane transport and electrochemical activity to explore the sensing performance of hydrogenated graphene.
- Lin Jiang
- , Wangyang Fu
- & Grégory F. Schneider