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| Open AccessArray of nanosheets render ultrafast and high-capacity Na-ion storage by tunable pseudocapacitance
Sodium ion batteries are a promising alternative to lithium ion technology, however their sluggish sodiation kinetics currently hinder performance. Here the authors fabricate ultrathin layered tin(II) sulfide nanostructures displaying a pseudocapacitance contribution for high capacity sodium ion anodes.
- Dongliang Chao
- , Changrong Zhu
- & Ze Xiang Shen
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| Open AccessWater-mediated cation intercalation of open-framework indium hexacyanoferrate with high voltage and fast kinetics
Rechargeable aqueous metal-ion batteries are promising for large-scale applications, but performance and stability issues still remain. Here the authors utilize open-framework indium hexacyanoferrate cathodes to improve performance, showing that water-mediated cation intercalation occurs at the cathode.
- Liang Chen
- , Hezhu Shao
- & Zhaoping Liu
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| Open AccessVisualizing non-equilibrium lithiation of spinel oxide via in situ transmission electron microscopy
Non-equilibrium intercalation reactions may determine the performance of lithium-ion battery materials undergoing lithiation, but it is difficult to probe in real time. Here, the authors use in situelectron microscopy to identify kinetically-driven phase evolution in magnetite single nanoparticles.
- Kai He
- , Sen Zhang
- & Dong Su
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| Open AccessPhotoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics
Aerosol droplets have significant effects on atmospheric photochemistry, however measuring absorption from single droplets is a challenge. Here, the authors report a method to measure absorption of nanodroplets with attolitre sensitivity, showing rate enhancements for light focusing in photolysis reactions.
- Johannes W. Cremer
- , Klemens M. Thaler
- & Ruth Signorell
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| Open AccessEvidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis
The excitation of metal nanoparticles with light can lead to localized surface plasmon resonances, capable of driving chemical reactions in bound species. Here, the authors elucidate this mechanism and suggest that future plasmonic catalysts may be able to selectively activate specific chemical bonds.
- Calvin Boerigter
- , Robert Campana
- & Suljo Linic
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| Open AccessNew insights into photoactivated volume generation boost surface morphing in liquid crystal coatings
The photomechanical surface modulation of liquid crystal polymer networks can be amplified with a small amount of azobenzene, but its mechanism is not yet fully understood. Here, Liu and Broer propose that the continuously oscillating trans-to-cisisomerization of azobenzene plays the dominating role.
- Danqing Liu
- & Dirk J. Broer
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| Open AccessAtomically resolved real-space imaging of hot electron dynamics
Hot electrons—electrons with very high kinetic energies—are important in many processes but difficult to observe due to their short lifetimes. Here, the authors analyse STM based nonlocal manipulation of organic molecules on a surface, showing that the measurements probe hot electron dynamics in real space.
- D. Lock
- , K. R. Rusimova
- & P. A. Sloan
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| Open AccessLow surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal
Surface recombination velocity can have a major impact on solar cell performance. Here, Yanget al. measure surface recombination dynamics in perovskite single crystals using broadband transient reflectance spectroscopy. Grain size is crucial to avoid the effects of surface recombination on carrier lifetime.
- Ye Yang
- , Yong Yan
- & Matthew C. Beard
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| Open AccessKinetics and fracture resistance of lithiated silicon nanostructure pairs controlled by their mechanical interaction
It is imperative to understand how individual Si nanostructures interact in battery operations. Here, the authors design well-defined crystalline Si nanopillars and show how mechanical interactions of neighbouring Si structures affect their reaction kinetics and fracture resistance during electrochemical lithiation.
- Seok Woo Lee
- , Hyun-Wook Lee
- & Yi Cui
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| Open AccessStrain induced fragility transition in metallic glass
The equivalency of stress and temperature as driving force for the relaxation in metallic glasses is widely accepted. Here, Yu et al.examine this assumption in simulations and find that stress induces a fragile-to-strong transition in addition to accelerated relaxation dynamics as temperature does.
- Hai-Bin Yu
- , Ranko Richert
- & Konrad Samwer
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Direct mechanochemical cleavage of functional groups from graphene
Breaking chemical bonds with mechanical force can be a useful route to modify chemical species, but studying the process in detail can be challenging. Here, the authors use atomic force microscopy to apply pressure and monitor bond cleavage on chemically modified graphene.
- Jonathan R. Felts
- , Andrew J. Oyer
- & Paul E. Sheehan
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Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects
Electrochemical devices based on oxide materials, such as batteries or fuel cells, rely on the transport of ions through the crystal lattice. Here, the authors model ion diffusion through CeO2and observe that edge dislocations slow down ion diffusion, contrary to similar processes in metals.
- Lixin Sun
- , Dario Marrocchelli
- & Bilge Yildiz
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Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics
Molecular core levels are localized around a single atomic site, but for indistinguishable atoms, photoionised core-holes can either be seen as localized or delocalized. Using a prototypical symmetric system, CS2, Guillemin et al. show that these states can be disentangled by fragmentation dynamics.
- R. Guillemin
- , P. Decleva
- & M. Simon
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Exciton dynamics reveal aggregates with intermolecular order at hidden interfaces in solution-cast organic semiconducting films
Grain boundaries between crystalline domains in solution-processed organic semiconductor thin films are believed to inhibit charge transport, but their structure is invisible to conventional characterization techniques. Wong et al. show the existence of nano-crystalline aggregates at domain interfaces.
- Cathy Y. Wong
- , Benjamin L. Cotts
- & Naomi S. Ginsberg
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| Open AccessUnravelling the multilayer growth of the fullerene C60 in real time
Despite the technological relevance of molecular thin films, there is limited understanding of their growth on a molecular level. Here, the authors characterize the relevant processes in real time and determine energy parameters using a combination of X-ray techniques and kinetic Monte Carlo simulations.
- S. Bommel
- , N. Kleppmann
- & S. Kowarik
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Water-induced correlation between single ions imaged at the solid–liquid interface
The organization of ions at solid–liquid interfaces is of interest in many fields, but little information at the nanoscale is available. Here, the authors report atomic-level observations of ordering of ions at surfaces in solutions, which is driven by water instead of the conventional electrostatic correlations.
- Maria Ricci
- , Peter Spijker
- & Kislon Voïtchovsky
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Single-molecule chemical reaction reveals molecular reaction kinetics and dynamics
Chemical reactions are typically composed of a number of elementary steps, but elucidating these steps is a challenge, particularly in the condensed phase. Here, the authors use quantum chemical calculations and single-molecule spectroscopy to unravel the details of a reversible redox process.
- Yuwei Zhang
- , Ping Song
- & Weilin Xu
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| Open AccessEncapsulation kinetics and dynamics of carbon monoxide in clathrate hydrate
Carbon monoxide clathrate hydrate has been widely studied and although the structure-II gas hydrate is predicted to be thermodynamically favourable, it is the structure-I hydrate that has been observed. Here, the authors synthesize the structure-II carbon monoxide hydrate and probe its structure and formation.
- Jinlong Zhu
- , Shiyu Du
- & Yusheng Zhao
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Extreme surface propensity of halide ions in water
The surface chemistry of aqueous solutions plays a ubiquitous role in many chemical and biological processes. Here, the authors probe the surfaces of sodium halide solutions with surface-specific femtosecond vibrational spectroscopy, and observe surface concentrations of halide ions several times greater than in the bulk.
- Lukasz Piatkowski
- , Zhen Zhang
- & Mischa Bonn
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Desorption kinetics from a surface derived from direct imaging of the adsorbate layer
Desorption kinetics cannot be simply described by the standard method, the temperature-programmed desorption. Here, Günther et al.use low-energy electron microscopy to image an adsorbate layer during desorption, and propose a model that quantitatively explains the complex desorption process.
- S. Günther
- , T. O. Menteş
- & J. Wintterlin
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Multistep kinetic self-assembly of DNA-coated colloids
The final state of self-assembled systems is determined by both their thermodynamic and kinetic pathways. Di Michele et al.develop a strategy to realize predesigned amorphous structures of complex DNA colloidal mixtures by selectively activating local inter- or intra-species interactions upon freezing.
- Lorenzo Di Michele
- , Francesco Varrato
- & Erika Eiser
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| Open AccessReactivity mapping with electrochemical gradients for monitoring reactivity at surfaces in space and time
Liquid chemical reactions on surfaces are important, but conventional characterization techniques for solutions cannot be directly applied. This study shows a high-throughput method to control and monitor chemical reactivity on surfaces via an electrochemically produced pH gradient in solutions.
- Sven O. Krabbenborg
- , Carlo Nicosia
- & Jurriaan Huskens
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The lifetime of the deviations from bulk behaviour in polymers confined at the nanoscale
Monitoring the impact of annealing on nanometre-thick polymer layers provides new insight into the changes in the performance of macromolecular materials. Here, the authors present results showing a correlation between the deviations from bulk behaviour and the growth of an irreversibly adsorbed layer.
- Simone Napolitano
- & Michael Wübbenhorst
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Vibrational dynamics and surface structure of amorphous selenium
Defining the structure of amorphous solids is a challenge because of their lack of structural order. In this study, the authors combine experiment and theory to analyse the surface of amorphous selenium, and show that the differences between surface and bulk are attributable to a particular type of coordination defect.
- T. Scopigno
- , W. Steurer
- & T. Wagner