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| Open AccessObservation of a promethium complex in solution
Stable chelation of the 147Pm radionuclide in aqueous solution by the newly synthesized organic diglycolamide ligand is demonstrated and the resulting complex studied, showing accelerated shortening of bonds at the beginning of the lanthanide series.
- Darren M. Driscoll
- , Frankie D. White
- & Alexander S. Ivanov
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Interchain-expanded extra-large-pore zeolites
We report a strategy that yields thermally and hydrothermally stable silicates by expansion of a one-dimensional silicate chain with an intercalated silylating agent that separates and connects the chains.
- Zihao Rei Gao
- , Huajian Yu
- & Miguel A. Camblor
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Article
| Open AccessCapturing the generation and structural transformations of molecular ions
The use of mega-electronvolt ultrafast electron diffraction combined with resonance-enhanced multiphoton ionization yields data that can reveal the formation and subsequent structural relaxation of a molecular ion on an ultrafast timescale.
- Jun Heo
- , Doyeong Kim
- & Hyotcherl Ihee
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Article
| Open AccessOperando probing of the surface chemistry during the Haber–Bosch process
Using X-ray photoelectron spectroscopy, the surface composition of iron and ruthenium catalysts during ammonia synthesis at pressures up to 1 bar and temperatures as high as 723 K can be revealed.
- Christopher M. Goodwin
- , Patrick Lömker
- & Anders Nilsson
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On-surface synthesis of aromatic cyclo[10]carbon and cyclo[14]carbon
We provide a modified strategy for the on-surface synthesis of cyclocarbons with 10 or 14 carbon atoms that provides a route for characterizing annular carbon allotropes.
- Luye Sun
- , Wei Zheng
- & Wei Xu
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Observing the primary steps of ion solvation in helium droplets
The initial steps of the ion solvation process are observed for the solvation of a single sodium ion in liquid helium, opening possibilities for benchmarking theoretical descriptions of ion solvation.
- Simon H. Albrechtsen
- , Constant A. Schouder
- & Henrik Stapelfeldt
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Adsorbate motors for unidirectional translation and transport
An adsorbate motor that moves unidirectionally on a copper surface is achieved by inducing intramolecular hydrogen transfer in a single molecule.
- Grant J. Simpson
- , Mats Persson
- & Leonhard Grill
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Structure evolution at the gate-tunable suspended graphene–water interface
Using centimetre-sized substrate-free monolayer graphene suspended on aqueous electrolyte surface, the structural evolution versus gate voltage at the graphene–water interface is shown, demonstrating minimal influence of extrinsic factors.
- Ying Xu
- , You-Bo Ma
- & Chuan-Shan Tian
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Article
| Open AccessProton transport through nanoscale corrugations in two-dimensional crystals
A study using high-resolution scanning electrochemical cell microscopy attributes proton permeation through defect-free graphene and hexagonal boron nitride to transport across areas of the structure that are under strain.
- O. J. Wahab
- , E. Daviddi
- & P. R. Unwin
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Article
| Open AccessReversible spin-optical interface in luminescent organic radicals
We report organic molecules showing both efficient luminescence and near-unity generation yield of excited states with high spin multiplicity, simultaneously supporting a high efficiency of initialization, spin manipulations and light-based readout at room temperature.
- Sebastian Gorgon
- , Kuo Lv
- & Emrys W. Evans
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Article
| Open AccessSingle molecule infrared spectroscopy in the gas phase
Using tagging spectroscopy, the infrared spectrum of a single organic molecule in the gas phase has been successfully measured.
- Aaron Calvin
- , Scott Eierman
- & David Patterson
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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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Characterization of just one atom using synchrotron X-rays
Using a specialized tip as a detector, the fingerprints of a single atom of iron and terbium are observed in synchrotron X-ray absorption spectra, allowing elemental and chemical characterization one atom at a time.
- Tolulope M. Ajayi
- , Nozomi Shirato
- & Saw-Wai Hla
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Separating single- from multi-particle dynamics in nonlinear spectroscopy
Transient absorption with N prescribed excitation intensities allows isolation of N increasingly nonlinear responses, enabling separation of single- and multiple-exciton dynamics.
- Pavel Malý
- , Julian Lüttig
- & Tobias Brixner
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Article
| Open AccessField-linked resonances of polar molecules
A type of universal scattering resonance between ultracold microwave-dressed polar molecules associated with field-linked tetramer bound states in the long-range potential well is observed, providing a general strategy for resonant scattering between ultracold polar molecules.
- Xing-Yan Chen
- , Andreas Schindewolf
- & Xin-Yu Luo
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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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The first-principles phase diagram of monolayer nanoconfined water
Monolayer water exhibits rich and diverse phase behaviour that is highly sensitive to temperature and the van der Waals pressure acting within the nanochannel.
- Venkat Kapil
- , Christoph Schran
- & Angelos Michaelides
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Magneto-optical trapping and sub-Doppler cooling of a polyatomic molecule
The polyatomic molecule calcium monohydroxide is magneto-optically trapped and cooled below the Doppler cooling limit, making it a candidate for applications in quantum simulation and computation.
- Nathaniel B. Vilas
- , Christian Hallas
- & John M. Doyle
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Article
| Open AccessMaterials synthesis at terapascal static pressures
Pressures of up to 900 gigapascals (9 million atmospheres) are achieved in a laser-heated double-stage diamond cell, enabling the synthesis of Re7N3, and materials characterization is performed in situ using single-crystal X-ray diffraction.
- Leonid Dubrovinsky
- , Saiana Khandarkhaeva
- & Natalia Dubrovinskaia
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Article
| Open AccessUnbiasing fermionic quantum Monte Carlo with a quantum computer
A hybrid quantum-classical algorithm for solving many-electron problems is developed, enabling the simulation, with the aid of 16 qubits on a quantum processor, of chemical systems with up to 120 orbitals.
- William J. Huggins
- , Bryan A. O’Gorman
- & Joonho Lee
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Evidence for the association of triatomic molecules in ultracold 23Na40K + 40K mixtures
Evidence is presented for the association of triatomic molecules near the Feshbach resonance in an ultracold gas comprising a mixture of 23Na40K molecules and 40K atoms, along with an estimation of the binding energy of the triatomic molecules.
- Huan Yang
- , Xin-Yao Wang
- & Jian-Wei Pan
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Direct observation of ultrafast hydrogen bond strengthening in liquid water
Liquid ultrafast electron scattering measures structural responses in liquid water with femtosecond temporal and atomic spatial resolution to reveal a transient hydrogen bond contraction then thermalization preceding relaxation of the OH stretch.
- Jie Yang
- , Riccardo Dettori
- & Xijie Wang
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Direct imaging of single-molecule electrochemical reactions in solution
Optical imaging of single-molecule electrochemical reactions in aqueous solution enables super-resolution electrochemiluminescence microscopy, which can be used to monitor the adhesion dynamics of live cells with high spatiotemporal resolution.
- Jinrun Dong
- , Yuxian Lu
- & Jiandong Feng
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Spectroscopic evidence for a gold-coloured metallic water solution
Spectroscopic measurements confirm that when water is adsorbed on drops of an alkali alloy at low pressure a gold-coloured metallic layer forms as electrons rapidly move from the drop into the water.
- Philip E. Mason
- , H. Christian Schewe
- & Pavel Jungwirth
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Asymmetric response of interfacial water to applied electric fields
Experimental measurements of vibrational sum-frequency generation spectra indicate that the dielectric response of water near an electrode may be strongly asymmetric, with different responses to positive and negative electrode charge.
- Angelo Montenegro
- , Chayan Dutta
- & Alexander V. Benderskii
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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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Direct assessment of the acidity of individual surface hydroxyls
Non-contact atomic force microscopy measurements are used to probe the hydrogen bond strength of individual surface hydroxyl groups and determine their acidity with atomic precision.
- Margareta Wagner
- , Bernd Meyer
- & Ulrike Diebold
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Transporting and concentrating vibrational energy to promote isomerization
Infrared absorption by a thick CO crystal produces many vibrational quanta that can be transported and concentrated at a salt interface to drive orientational isomerization of CO molecules with enhanced efficiency.
- Jascha A. Lau
- , Li Chen
- & Alec M. Wodtke
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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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Probing the critical nucleus size for ice formation with graphene oxide nanosheets
Nucleation experiments with water droplets containing differently sized graphene oxide nanosheets provide an experimental indication of the temperature-dependent size of the critical ice nucleus.
- Guoying Bai
- , Dong Gao
- & Jianjun Wang
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Analogue quantum chemistry simulation
An analogue quantum simulator based on ultracold atoms in optical lattices and cavity quantum electrodynamics is proposed for the solution of quantum chemistry problems and tested numerically for a simple molecule.
- Javier Argüello-Luengo
- , Alejandro González-Tudela
- & J. Ignacio Cirac
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Selective triplet exciton formation in a single molecule
Recombination of excitons to produce molecular light emission is made more efficient by controlling electron spin within the molecule to produce spin-triplet excitons only, without the usual accompanying spin-singlet excitons.
- Kensuke Kimura
- , Kuniyuki Miwa
- & Yousoo Kim
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Absence of amorphous forms when ice is compressed at low temperature
Slow compression of ice at low temperature results in the sequential formation of a series of crystalline phases, challenging theories that connect amorphous ice to supercooled liquid water.
- Chris A. Tulk
- , Jamie J. Molaison
- & Dennis D. Klug
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Colossal barocaloric effects in plastic crystals
Colossal barocaloric effects are observed in the plastic crystal neopentylglycol and found to originate from the extensive molecular orientational disorder, giant compressibility and highly anharmonic lattice dynamics of the material.
- Bing Li
- , Yukinobu Kawakita
- & Zhidong Zhang
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Electronic noise due to temperature differences in atomic-scale junctions
A fundamental electronic noise—beyond electronic thermal noise and voltage-activated shot noise—that is generated by temperature differences across nanoscale conductors is demonstrated, with possible implications for thermometry and electronics.
- Ofir Shein Lumbroso
- , Lena Simine
- & Oren Tal
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Heterointerface effects in the electrointercalation of van der Waals heterostructures
The electrointercalation of lithium into van der Waals heterostructures of graphene, hexagonal boron nitride and molybdenum dichalcogenides is studied at the level of individual atomic interfaces.
- D. Kwabena Bediako
- , Mehdi Rezaee
- & Philip Kim
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The effect of hydration number on the interfacial transport of sodium ions
A sodium ion hydrated with three (rather than one, two, four or five) water molecules diffuses orders of magnitude more quickly than the other ion hydrates owing to the interfacial symmetry mismatch.
- Jinbo Peng
- , Duanyun Cao
- & Ying Jiang
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Molecular nucleation mechanisms and control strategies for crystal polymorph selection
Cryo-transmission electron microscopy reveals the initiation of glucose isomerase crystals and their growth into different crystalline or gel polymorphs, and shows that mutating specific amino acids controls which polymorph grows.
- Alexander E. S. Van Driessche
- , Nani Van Gerven
- & Mike Sleutel
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Perovskite nickelates as electric-field sensors in salt water
Application of an electric field changes the transport and optical properties of samarium nickelate submerged in water, making it a suitable passive sensor of weak electric fields in salt water.
- Zhen Zhang
- , Derek Schwanz
- & Shriram Ramanathan
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Molecular magnetic hysteresis at 60 kelvin in dysprosocenium
Magnetic hysteresis is observed in a dysprosocenium complex at temperatures of up to 60 kelvin, the origin of which is the localized metal–ligand vibrational modes unique to dysprosocenium.
- Conrad A. P. Goodwin
- , Fabrizio Ortu
- & David P. Mills
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Preparation and coherent manipulation of pure quantum states of a single molecular ion
By exploiting a co-trapped Ca+ ion, a single CaH+ ion is prepared in pure quantum states, which are coherently manipulated, using a protocol that could easily be extended to other molecular ion species.
- Chin-wen Chou
- , Christoph Kurz
- & Dietrich Leibfried
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A low-spin Fe(iii) complex with 100-ps ligand-to-metal charge transfer photoluminescence
An iron complex is described that exhibits photoluminescence at room temperature, opening the way to the use of iron-based materials as low-cost, non-toxic light emitters and photosensitizers.
- Pavel Chábera
- , Yizhu Liu
- & Kenneth Wärnmark
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Doped polymer semiconductors with ultrahigh and ultralow work functions for ohmic contacts
A general strategy for producing solution-processed doped polymers with the extreme work functions that are required to make good ohmic contacts to semiconductors is demonstrated in high-performance light-emitting diodes, transistors and solar cells.
- Cindy G. Tang
- , Mervin C. Y. Ang
- & Peter K. H. Ho
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Molecular-scale evidence of aerosol particle formation via sequential addition of HIO3
Field data from an iodine-rich, coastal environment point to the molecular steps involved in the formation of new aerosol particles from iodine vapours over coastal regions.
- Mikko Sipilä
- , Nina Sarnela
- & Colin O’Dowd
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Photodissociation of ultracold diatomic strontium molecules with quantum state control
The photodissociation of 88Sr2 molecules is examined at ultracold temperatures with a high degree of control, and a wealth of quantum effects such as barrier tunnelling, matter—wave interference of reaction products and forbidden pathways are observed
- M. McDonald
- , B. H. McGuyer
- & T. Zelevinsky
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Mean first-passage times of non-Markovian random walkers in confinement
An analytical method of determining the mean first-passage time (the time taken by a random walker in confinement to reach a target point) is presented for a Gaussian non-Markovian random walker, thus revealing the importance of memory effects in first-passage statistics.
- T. Guérin
- , N. Levernier
- & R. Voituriez
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Continuous probing of cold complex molecules with infrared frequency comb spectroscopy
Combining cavity-enhanced direct frequency comb spectroscopy with buffer gas cooling enables rapid collection of well-resolved infrared spectra for molecules such as nitromethane, naphthalene and adamantane, confirming the value of the combined approach for studying much larger and more complex molecules than have been probed so far.
- Ben Spaun
- , P. Bryan Changala
- & Jun Ye
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A lithium–oxygen battery based on lithium superoxide
Lithium–oxygen batteries allow oxygen to be reduced at the battery’s cathode when a current is drawn; in present-day batteries, this results in formation of Li2O2, but it is now shown that another high energy density material, namely LiO2, with better electronic conduction can be used instead as the discharge product, if the electrode is decorated with iridium nanoparticles.
- Jun Lu
- , Yun Jung Lee
- & Khalil Amine
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Square ice in graphene nanocapillaries
The structure of the low-dimensional water confined in hydrophobic pores is shown, using electron microscopy and supported by molecular dynamics simulations, to be ‘square ice’, which does not have the conventional tetrahedral hydrogen bonding.
- G. Algara-Siller
- , O. Lehtinen
- & I. V. Grigorieva