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| Open AccessImaging how thermal capillary waves and anisotropic interfacial stiffness shape nanoparticle supracrystals
Interfacial fluctuations at the nanoscale, such as shape evolution of a growing crystal, are prohibitively difficult to study experimentally. Here, the authors are able to map the kinetic and thermodynamic parameters involved in shaping of nanoparticle supracrystals by directly imaging the fluctuating crystal surface by liquid-phase TEM, and analyzing it in the context of capillary wave theory.
- Zihao Ou
- , Lehan Yao
- & Qian Chen
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Article
| Open AccessSpontaneous creation and annihilation dynamics and strain-limited stability of magnetic skyrmions
Skyrmions are spin textures which have integer topological charge. Typically they are very stable. Here, the authors observe the spontaneous creation and annihilation of skyrmions in regions of high exchange energy density, suggesting a limit to skyrmion stability.
- Frederic Rendell-Bhatti
- , Raymond J. Lamb
- & Damien McGrouther
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Article
| Open AccessImaging electrochemically synthesized Cu2O cubes and their morphological evolution under conditions relevant to CO2 electroreduction
Catalytic selectivity during carbon dioxide electroreduction can be tuned by using geometric copper-based catalysts. Here, the authors use liquid cell transmission electron microscopy to study the in situ synthesis and morphological evolution Cu2O cubes under carbon dioxide electroreduction conditions.
- Rosa M. Arán-Ais
- , Rubén Rizo
- & Beatriz Roldan Cuenya
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Article
| Open AccessReconstruction of evolving nanostructures in ultrathin films with X-ray waveguide fluorescence holography
The authors introduce X-ray waveguide fluorescence holography based on the waveguiding properties of thin films. Combined with model-independent reconstruction algorithms, they show that the method can be used for real-time nanostructure kinetic studies.
- Zhang Jiang
- , Joseph W. Strzalka
- & Jin Wang
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Article
| Open AccessImaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells
Rational design of multicomponent nanocrystals requires atomic-level understanding of reaction kinetics. Here, the authors apply single-particle liquid-cell electron microscopy imaging coupled with atomistic simulations to understand pathways and rates of bimetallic core-shell nanocubes undergoing oxidative dissolution.
- Lei Chen
- , Alberto Leonardi
- & Xingchen Ye
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Article
| Open AccessSpectral cross-cumulants for multicolor super-resolved SOFI imaging
Here, the authors generalize cumulant analysis by extending it into the spectral domain to allow multicolour super-resolution optical fluctuation imaging. The simultaneous acquisition of two spectral channels followed by spectral cross-cumulant analysis and unmixing allows denser spectral and spatial sampling of the super-resolved image.
- K. S. Grußmayer
- , S. Geissbuehler
- & T. Lasser
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Article
| Open AccessTransient lensing from a photoemitted electron gas imaged by ultrafast electron microscopy
Excited charge carriers, such as photoelectrons, play an important role in fundamental and technological fields. Here the authors employ an ultrafast electron microscope to directly visualize the cyclotron oscillations and oblate-to-prolate shape change of a photoemitted electron gas from a laser-excited copper surface.
- Omid Zandi
- , Allan E. Sykes
- & Renske M. van der Veen
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Article
| Open AccessMixed-state electron ptychography enables sub-angstrom resolution imaging with picometer precision at low dose
With conventional scanning transmission electron microscopy, some sensitive materials are difficult to image with atomic resolution. The authors present a method of mixed-state electron ptychography that enables picometer precision with fast acquisition and low dosage.
- Zhen Chen
- , Michal Odstrcil
- & David A. Muller
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Article
| Open AccessTuning the activities of cuprous oxide nanostructures via the oxide-metal interaction
The design of oxide-metal interface for heterogeneous catalysis has been hampered by the limited fundamental understanding. Here, the authors demonstrate that the activities of cuprous oxide nanostructures for CO oxidation can be tuned via the oxide-metal (Cu2O/M, M = Pt, Ag, Au) interaction.
- Wugen Huang
- , Qingfei Liu
- & Fan Yang
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Article
| Open AccessMachine-learning-revealed statistics of the particle-carbon/binder detachment in lithium-ion battery cathodes
Developing understanding of degradation phenomena in nickel rich cathodes is under intense investigation. Here the authors use learning-assisted statistical analysis and experiment-informed mathematical modelling to resolve the microstructure of a Ni-rich NMC composite cathode.
- Zhisen Jiang
- , Jizhou Li
- & Yijin Liu
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Article
| Open AccessStructural changes in noble metal nanoparticles during CO oxidation and their impact on catalyst activity
How nanoparticle (NP) catalysts re-structure under reaction conditions and how these changes associate with catalytic activity remains poorly understood. Here, the authors present operando TEM studies of Pd NPs during CO oxidation, which show reversible changes in both structure and activity with temperature.
- See Wee Chee
- , Juan Manuel Arce-Ramos
- & Utkur Mirsaidov
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Article
| Open AccessObservation of the molecular response to light upon photoexcitation
Photoabsorption is a fundamental process that leads to changes in the electron density in matter. Here, the authors show a direct measurement of the distribution of electron density when a cyclohexadine molecule is excited by pulsed UV radiation and probed by a time delayed X-ray pulse generated at LCLS.
- Haiwang Yong
- , Nikola Zotev
- & Peter M. Weber
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Article
| Open AccessSingle-shot ultrafast imaging attaining 70 trillion frames per second
Ultrafast imaging has been limited by the speed of electronic sensors. Here, the authors demonstrate single-shot compressed ultrafast spectral photography, which combines spectral encoding, pulse splitting, temporal shearing, and compressed sensing in order to achieve real-time imaging at 70 trillion frames per second.
- Peng Wang
- , Jinyang Liang
- & Lihong V. Wang
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Article
| Open Access3D microstructure design of lithium-ion battery electrodes assisted by X-ray nano-computed tomography and modelling
The 3D microstructure of the electrode predominantly determines the electrochemical performance of Li-ion batteries. Here, the authors show that the microstructural heterogeneities lead to non-uniform Li insertion and current distribution while graded-microstructures improve the performance.
- Xuekun Lu
- , Antonio Bertei
- & Paul R. Shearing
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Article
| Open AccessPhasor field diffraction based reconstruction for fast non-line-of-sight imaging systems
Current implementations of non-line-of-sight imaging use reconstruction algorithms that are difficult to implement fast enough for real-time application using light efficient equipment. The authors present an algorithm for non-line-of-sight imaging that is low complexity and allows fast and efficient reconstruction on a standard computer.
- Xiaochun Liu
- , Sebastian Bauer
- & Andreas Velten
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Article
| Open AccessExfoliated near infrared fluorescent silicate nanosheets for (bio)photonics
Near-infrared (NIR) fluorophores have attracted interest for bioimaging; yet availability, biocompatibility and application can be an issue. Here, the authors report on the development of Egyptian Blue nanosheets with high NIR fluorescence and photostability demonstrating bioimaging applications in vivo.
- Gabriele Selvaggio
- , Alexey Chizhik
- & Sebastian Kruss
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Article
| Open AccessMegahertz-rate shock-wave distortion cancellation via phase conjugate digital in-line holography
Shock-waves in explosive, supersonic or ionizing environments impart phase distortions to holographic imaging. Here, the authors report an ultra-high-speed phase conjugate digital in-line holography technique where a laser passes through the shock-wave and is reflected back through the phase distortion, thus correcting phase delays.
- Yi Chen Mazumdar
- , Michael E. Smyser
- & Daniel R. Guildenbecher
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Article
| Open AccessDictionary learning in Fourier-transform scanning tunneling spectroscopy
Aperiodic structure imaging suffers limitations when utilizing Fourier analysis. The authors report an algorithm that quantitatively overcomes these limitations based on nonconvex optimization, demonstrated by studying aperiodic structures via the phase sensitive interference in STM images.
- Sky C. Cheung
- , John Y. Shin
- & Abhay N. Pasupathy
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Article
| Open AccessPhase protection of Fano-Feshbach resonances
The lifetime of decaying quantum states has been thought to depend on the strength of the coupling causing the decay. Here the authors demonstrate that quantum mechanical interference can dominate this process, observing Fano-Feshbach resonance lifetimes covering several orders of magnitude.
- Alexander Blech
- , Yuval Shagam
- & Christiane P. Koch
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Article
| Open AccessSerial protein crystallography in an electron microscope
For conventional three-dimensional microcrystal electron diffraction (3D ED/MicroED), a crystal is slowly rotated under an electron beam, leading to inevitable accumulation of radiation damage during data collection. In this work, the authors present a serial electron diffraction method, where still diffraction patterns from many protein nanocrystals are rapidly recorded and merged, which minimises radiation damage and only requires a slightly modified standard scanning transmission electron microscope.
- Robert Bücker
- , Pascal Hogan-Lamarre
- & R. J. Dwayne Miller
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Article
| Open AccessDeep tissue space-gated microscopy via acousto-optic interaction
In ideal diffraction-limited optical microscopy imaging depth is limited by the multiply scattered wave. Here, the authors present a space gating method, based on an acoustic focus in the object plane and reconstruction using only the acousto-optically modulated ballistic wave, and demonstrate increased imaging depth in scattering samples.
- Mooseok Jang
- , Hakseok Ko
- & Wonshik Choi
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Article
| Open AccessThe role of transient resonances for ultra-fast imaging of single sucrose nanoclusters
X-ray free electron lasers provide high photon flux to explore single particle diffraction imaging of biological samples. Here the authors present dynamic electronic structure calculations and benchmark them to single-particle XFEL diffraction data of sucrose clusters to predict optimal single-shot imaging conditions.
- Phay J. Ho
- , Benedikt J. Daurer
- & Christoph Bostedt
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Article
| Open AccessRatiometric upconversion nanothermometry with dual emission at the same wavelength decoded via a time-resolved technique
Traditional ratiometric temperature monitoring is challenging due to the variation in tissue absorption and scattering of different wavelengths. Here, the authors show improved accuracy by using emission at the same wavelength, but different luminescent lifetimes decoded by a time-resolved technique.
- Xiaochen Qiu
- , Qianwen Zhou
- & Fuyou Li
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Article
| Open AccessFast and quantitative 2D and 3D orientation mapping using Raman microscopy
Although polarized Raman microscopy is sensitive to orientation changes, quantitative information has been missing. Here, the authors use simultaneous registration of multiple Raman scattering spectra obtained at different polarizations and show quantitative orientation mapping
- Oleksii Ilchenko
- , Yuriy Pilgun
- & Anja Boisen
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Article
| Open AccessPhoto-activated raster scanning thermal imaging at sub-diffraction resolution
Thermal characterization of biological tissues can traditionally provide either large fields of view or high resolution. By the development of super-resolution infrared photo-thermal imaging, the authors reconstruct temperature-based maps of absorptive centers in millimeter-sized biological samples.
- M. Bouzin
- , M. Marini
- & M. Collini
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Article
| Open AccessDiffractive small angle X-ray scattering imaging for anisotropic structures
Mesoscale investigations of material microarchitecture using small angle X-ray scattering (SAXS) methods have been limited by long measurement times. Here, the authors present an X-ray diffractive optics method which enables single shot acquisition of SAXS signals over large areas.
- Matias Kagias
- , Zhentian Wang
- & Marco Stampanoni
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Article
| Open AccessReal-time 3D reconstruction from single-photon lidar data using plug-and-play point cloud denoisers
The use of single-photon data has been limited by time-consuming reconstruction algorithms. Here, the authors combine statistical models and computational tools known from computer graphics and show real-time reconstruction of moving scenes.
- Julián Tachella
- , Yoann Altmann
- & Stephen McLaughlin
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Article
| Open AccessHow to control single-molecule rotation
The orientation of a molecule on a surface affects many processes, so the ability to control single-molecule rotation could be powerful. Here, the authors use the electric field from a scanning tunneling microscope tip to precisely induce unidirectional rotation of a polar molecule, allowing visualization of the molecule’s internal dipole moment.
- Grant J. Simpson
- , Víctor García-López
- & Leonhard Grill
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Article
| Open AccessComplex vectorial optics through gradient index lens cascades
The manufacturing process for GRIN lenses causes a symmetric birefringence variation which is considered a deficiency. Here, the authors show how this birefringence can generate vector vortex beams and form the basis of a Müller matrix polarimeter with potential for endoscopic label-free cancer diagnostics.
- Chao He
- , Jintao Chang
- & Martin J. Booth
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Article
| Open AccessUltrabright gap-enhanced Raman tags for high-speed bioimaging
The speed of surface-enhanced Raman spectroscopy (SERS) imaging is generally limited due to low Raman signals. Here, the authors develop bright gap-enhanced Raman tags with external hot spots and demonstrate their use in fast near-infrared bioimaging.
- Yuqing Zhang
- , Yuqing Gu
- & Jian Ye
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Article
| Open AccessVisualization and quantification of inhomogeneous and anisotropic magnetic fields by polarized neutron grating interferometry
The magnetic field imaging on microscopic scale is of great importance to fundamental research as well industrial applications. Here the authors show the capability to visualize and characterize the magnetic properties with 100-micrometer resolution in macroscopic samples using a cold polarized neutron beam in neutron grating interferometry.
- Jacopo Valsecchi
- , Ralph P. Harti
- & Christian Grünzweig
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Article
| Open AccessUsing X-ray tomoscopy to explore the dynamics of foaming metal
Understanding fast phenomena that happen in hot and opaque environments, such as during metal foaming, remains a challenge. Here, the authors use ultra-fast imaging of more than 200 three-dimensional volumes per second to explore bubble coalescence in an aluminium alloy.
- Francisco García-Moreno
- , Paul Hans Kamm
- & John Banhart
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Article
| Open AccessBand-collision gel electrophoresis
Electrophoretic mobility shift assays are widely used in gel electrophoresis to study binding interactions between different molecular species, but these assays access only a subset of reaction possibilities. Here, the authors develop a band-collision gel electrophoresis (BCGE) approach that demonstrates a much wider variety of reaction types.
- Dimitri A. Bikos
- & Thomas G. Mason
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Article
| Open AccessThree-dimensional character of the deformation twin in magnesium
Imaging deformation twins in three dimensions is difficult and they are usually viewed as two-dimensional ellipsoids. Here, the authors statistically analyze more than two hundred deformation twins in magnesium observed in three different views and show lateral twin expansion is faster than forward propagation.
- Y. Liu
- , P. Z. Tang
- & C. N. Tomé
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Article
| Open AccessDirect observation and impact of co-segregated atoms in magnesium having multiple alloying elements
Commercial alloys contain trace solutes that segregate at grain boundaries but have been difficult to directly image due to electron beam damage. Here, the authors use atomic-resolution energy dispersive X-ray spectroscopy at lower electron voltage to image segregation at magnesium alloy twin boundaries.
- Xiaojun Zhao
- , Houwen Chen
- & Jian-Feng Nie
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Article
| Open AccessIn-operando high-speed microscopy and thermometry of reaction propagation and sintering in a nanocomposite
Imaging highly exothermic reactions in high spatial and temporal resolution to understand their underlying reaction mechanisms is challenging. Here, the authors develop a high-speed microscopy/pyrometry imaging system to successfully observe reactive sintering in a nanothermite reaction in-operando.
- Haiyang Wang
- , Dylan J. Kline
- & Michael R. Zachariah
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Article
| Open AccessAb initio nonrigid X-ray nanotomography
Radiation induced sample deformation can be a limiting factor for X-ray imaging resolution at the nanoscale. The authors report a tomographic model that estimates and accounts for morphological changes during data acquisition and enables reconstruction of a high-resolution image ab initio.
- Michal Odstrcil
- , Mirko Holler
- & Manuel Guizar-Sicairos
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Article
| Open AccessDirect measurement of nanostructural change during in situ deformation of a bulk metallic glass
Observing defect formation during bulk metallic glass deformation remains challenging. Here, the authors combine in situ nanobeam electron diffraction and large-scale molecular dynamics simulations to directly link changes to the local atomic ordering with shear band formation in a metallic glass.
- Thomas C. Pekin
- , Jun Ding
- & Andrew M. Minor
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Article
| Open AccessDirect observation of picosecond melting and disintegration of metallic nanoparticles
Laser-matter interaction has been intensively studied in equilibrium states, but irreversible processes in a highly nonequilibrium state at nanoscales remains elusive due to experimental challenges. Here, Ihm et al. image heterogeneous melting of gold nanoparticles with nanometer and picosecond resolution.
- Yungok Ihm
- , Do Hyung Cho
- & Changyong Song
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Article
| Open AccessA monolithic immersion metalens for imaging solid-state quantum emitters
Photon collection from quantum emitters is difficult, and their scale requires the use of free-space optical measurement setups which prevent packaging of quantum devices. Here, the authors design and fabricate a metasurface that acts as an immersion lens to collect and collimate the emission of an individual emitter.
- Tzu-Yung Huang
- , Richard R. Grote
- & Lee C. Bassett
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Article
| Open AccessAtomic resolution electron microscopy in a magnetic field free environment
Electron microscopy typically requires strong magnetic lenses in order to reach atomic resolution, prohibiting the possibility to measure magnetic materials. The authors here present a lens design that enables atomic-resolution electron microscopy of magnetic materials by providing a field-free sample region.
- N. Shibata
- , Y. Kohno
- & Y. Ikuhara
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Article
| Open AccessImaging gigahertz zero-group-velocity Lamb waves
Zero-group-velocity Lamb waves, which are surface waves with reduced losses and high Q factor, have many potential applications. The authors image such waves in 2 dimensions, and in the GHz range, with a bilayer using a time-resolved imaging technique with an ultra-short-pulse laser.
- Qingnan Xie
- , Sylvain Mezil
- & Oliver B. Wright
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Article
| Open AccessTransmission of natural scene images through a multimode fibre
The optical transmission of images through a multimode fibre remains an outstanding challenge. Here, the authors implement a method that statistically reconstructs the inverse transformation matrix for a fibre and demonstrate real-time imaging of natural scenes in full colour, high resolution and high frame rate.
- Piergiorgio Caramazza
- , Oisín Moran
- & Daniele Faccio
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Article
| Open AccessInformation-rich localization microscopy through machine learning
Single-molecule methods often rely on point spread functions that are tailored to interpret specific information. Here the authors use a neural network to extract complex PSF information from experimental images, and demonstrate this by classifying color and axial positions of emitters.
- Taehwan Kim
- , Seonah Moon
- & Ke Xu
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Article
| Open AccessDynamics of pore formation during laser powder bed fusion additive manufacturing
Laser-matter interactions during laser powder bed fusion additive manufacturing remain poorly understood. Here, the authors combine in situ X-ray imaging and finite element simulations to show how detrimental pores form under printing conditions and develop a strategy to suppress them.
- Aiden A. Martin
- , Nicholas P. Calta
- & Manyalibo J. Matthews
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Review Article
| Open AccessPiezoresponse force microscopy and nanoferroic phenomena
- Alexei Gruverman
- , Marin Alexe
- & Dennis Meier
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Article
| Open AccessGeometric imaging of borophene polymorphs with functionalized probes
Borophene, or 2D boron, is highly polymorphic with many predicted lattice arrangements, complicating the identification of its atomic structure. Here, the authors use functionalized-tip scanning probe microscopy to directly resolve the atomic lattice structures of several borophene polymorphs.
- Xiaolong Liu
- , Luqing Wang
- & Mark C. Hersam
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Article
| Open AccessUltra-high resolution imaging of thin films and single strands of polythiophene using atomic force microscopy
Semiconducting polymers are widely used in optoelectronic devices, in which their microstructure informs function. Here, the authors are able to resolve the molecular and sub-molecular ordering of polythiophene strands and thin films using atomic force microscopy, a significant step towards correlating polymer structure with device performance.
- Vladimir V. Korolkov
- , Alex Summerfield
- & Peter H. Beton
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Article
| Open AccessPartially coherent radar unties range resolution from bandwidth limitations
Distinguishing between closely situated targets depends inversely on the bandwidth of the transmitted radar signal. Here, the authors demonstrate a type of ranging system which is not limited by bandwidth. They show an improvement of two orders of magnitude, compared to standard coherent radars with the same bandwidth.
- Rony Komissarov
- , Vitali Kozlov
- & Pavel Ginzburg