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| Open AccessA catalytically active oscillator made from small organic molecules
We report a small-organic-molecule oscillator that catalyses an independent chemical reaction in situ without impairing its oscillating properties, allowing the construction of complex systems enhancing applications in automated synthesis and systems and polymerization chemistry.
- Matthijs ter Harmsel
- , Oliver R. Maguire
- & Syuzanna R. Harutyunyan
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Article
| Open AccessFemtosecond proton transfer in urea solutions probed by X-ray spectroscopy
The potential of water-window X-ray absorption spectroscopy for disentangling individual aspects of the respective electronic and structural dynamics in ultrafast non-adiabatic dynamics of molecular systems in a liquid environment is established.
- Zhong Yin
- , Yi-Ping Chang
- & Hans Jakob Wörner
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Tracking cubic ice at molecular resolution
Tracking the formation of cubic ice (ice Ic) using transmission electron microscopy and low-dose imaging shows preferential nucleation of ice Ic at low-temperature interfaces and two types of stacking disorder.
- Xudan Huang
- , Lifen Wang
- & Xuedong Bai
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Tunnelling measured in a very slow ion–molecule reaction
The proton-transfer tunnelling reaction rate between H2 and D– has been measured as about 1 out of 1011 collisions, making it the slowest rate constant ever measured for an ion–molecule reaction in the gas phase.
- Robert Wild
- , Markus Nötzold
- & Roland Wester
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Article
| Open AccessCondensed-phase isomerization through tunnelling gateways
Measurements of isomerization rates of CO isotopologues on an NaCl surface show a nonmonotonic mass dependence that arises from resonantly enhanced cross-barrier coupling, or ‘tunnelling gateways’, which are intrinsic to condensed-phase tunnelling.
- Arnab Choudhury
- , Jessalyn A. DeVine
- & Alec M. Wodtke
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Article |
Precision test of statistical dynamics with state-to-state ultracold chemistry
The chemical reaction 2KRb → K2 + Rb2 is studied under ultralow temperatures at the quantum state-to-state level, allowing unprecedented details of the reaction dynamics to be observed.
- Yu Liu
- , Ming-Guang Hu
- & Kang-Kuen Ni
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Article |
Sub-cycle atomic-scale forces coherently control a single-molecule switch
The near field of a terahertz wave confined to a scanning probe tip provides femtosecond atomic-scale forces that coherently modulate the switching probability of a molecule between two stable adsorption geometries.
- Dominik Peller
- , Lukas Z. Kastner
- & Jascha Repp
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Article |
Coherent control of a surface structural phase transition
A structural phase transition from metal to insulator on a solid surface is controlled by an ultrafast sequence of optical pulses.
- Jan Gerrit Horstmann
- , Hannes Böckmann
- & Claus Ropers
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Mapping the emergence of molecular vibrations mediating bond formation
Femtosecond X-ray liquidography is used to track the vibrational wavepacket trajectories of gold atoms in solution, enabling time-resolved observations of the emergence of vibrations and the evolution of the formation of covalent bonds.
- Jong Goo Kim
- , Shunsuke Nozawa
- & Hyotcherl Ihee
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Article |
Atomic imaging of the edge structure and growth of a two-dimensional hexagonal ice
Real-space imaging of the edge structures and growth of a two-dimensional ice on a gold substrate is achieved using noncontact atomic-force microscopy with a carbon monoxide tip.
- Runze Ma
- , Duanyun Cao
- & Ying Jiang
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Article |
Metal-free directed sp2-C–H borylation
A method for the site-selective C–H borylation of arenes and heteroarenes is described, in which BBr3 acts as both a reagent and a catalyst.
- Jiahang Lv
- , Xiangyang Chen
- & Zhuangzhi Shi
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Letter |
Velocity-resolved kinetics of site-specific carbon monoxide oxidation on platinum surfaces
The catalytic oxidation of carbon monoxide over platinum proceeds through two distinct channels: it is dominated at low temperatures by the more active step sites and at high temperatures by the more abundant terrace sites of the platinum surface.
- Jannis Neugebohren
- , Dmitriy Borodin
- & Theofanis N. Kitsopoulos
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Letter |
Potential enthalpic energy of water in oils exploited to control supramolecular structure
Less than 0.01 per cent by weight of water in an alkane solvent is sufficient to interact with co-dissolved supramolecular polymeric chains by hydrogen bonding and modulate the structure of the assembly.
- Nathan J. Van Zee
- , Beatrice Adelizzi
- & E. W. Meijer
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Letter |
Role of stacking disorder in ice nucleation
Stacking-disordered ice crystallites are shown to have an ice nucleation rate much higher than predicted by classical nucleation theory, which needs to be taken into account in cloud modelling.
- Laura Lupi
- , Arpa Hudait
- & Valeria Molinero
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Letter |
Autocatalytic, bistable, oscillatory networks of biologically relevant organic reactions
A few-component network of biologically relevant, organic reactions displays bistability and oscillations, without an enzymatic catalyst.
- Sergey N. Semenov
- , Lewis J. Kraft
- & George M. Whitesides
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Article |
Synergistic, ultrafast mass storage and removal in artificial mixed conductors
An artificial composite of the super-ionic conductor RbAg4I5 and the electronic conductor graphite exhibits extremely fast diffusion of silver ions at the interface between the two materials, generating both silver-excess and silver-deficient sites.
- Chia-Chin Chen
- , Lijun Fu
- & Joachim Maier
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Letter |
Tracking excited-state charge and spin dynamics in iron coordination complexes
Femtosecond resolution X-ray fluorescence spectroscopy is shown to track the charge and spin dynamics triggered when an iron coordination complex is excited by light, and establishes the critical role of intermediate spin states in the de-excitation process.
- Wenkai Zhang
- , Roberto Alonso-Mori
- & Kelly J. Gaffney
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Letter |
Single-molecule fluorescence probes dynamics of barrier crossing
Here the Kramers diffusion coefficient and free-energy barrier are characterized for the first time through single-molecule fluorescence measurements of the temperature- and viscosity-dependence of the transition path time for protein folding.
- Hoi Sung Chung
- & William A. Eaton
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Letter |
Snapshots of cooperative atomic motions in the optical suppression of charge density waves
The development of table-top femtosecond electron diffraction sources in recent years has opened up a new way to observe atomic motions in crystalline materials undergoing structural changes. Here, the technique is used to study the charge density wave material 1T-TaS2, where a modulation of the electron density is accompanied by a periodic lattice distortion. In this femtosecond electron diffraction experiment, where atomic motions are observed in response to a 140 femtosecond optical pulse, the periodic lattice distortion is found to collapse on an exceptionally fast timescale (about 250 femtoseconds), indicative of an electronically driven process involving a highly cooperative process.
- Maximilian Eichberger
- , Hanjo Schäfer
- & R. J. Dwayne Miller
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News & Views |
Surprise in the strong regime
The finding that the normal phase of an ultracold gas of fermionic atoms in the strongly interacting regime is close to a Fermi liquid isn't quite what theorists expected for these systems.
- Yong-il Shin
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Letter |
TCR–peptide–MHC interactions in situ show accelerated kinetics and increased affinity
T lymphocytes, which are an integral part of most adaptive immune responses, recognize foreign antigens through the binding of antigenic peptide–major histocompatibility complex (pMHC) molecules on other cells to specific T-cell antigen receptors (TCRs). Using single-molecule microscopy and fluorescence resonance energy transfer, the kinetics of TCR–pMHC binding are now measured in situ, revealing accelerated kinetics and increased affinity when compared with solution measurements.
- Johannes B. Huppa
- , Markus Axmann
- & Mark M. Davis
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Letter |
Experimental evidence for a frustrated energy landscape in a three-helix-bundle protein family
The primary sequence of a protein defines its free-energy landscape and thus determines the rate constants of folding and unfolding, with theory suggesting that roughness in the energy landscape leads to slower folding. However, obtaining experimental descriptions of this landscape is challenging. Landscape roughness is now shown to be responsible for the slower folding and unfolding times observed in the R16 and R17 domains of α-spectrin relative to the similar R15 domain.
- Beth G. Wensley
- , Sarah Batey
- & Jane Clarke