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| Open AccessPolar surface structure of oxide nanocrystals revealed with solid-state NMR spectroscopy
Polar-faceted nanocrystals often have complex atomic surface configurations that are very difficult to characterize. Here, the authors are able to determine detailed structural information about the polar facets of ceria nanocubes by using 17O and 1H solid-state NMR spectroscopy, in combination with density functional theory calculations.
- Junchao Chen
- , Xin-Ping Wu
- & Luming Peng
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Article
| Open AccessCombined orbital tomography study of multi-configurational molecular adsorbate systems
The shape and energy of frontier orbitals determine the reactivity of molecular systems. Combining orbital tomography based on photoelectron spectroscopy with electron diffraction and DFT, the authors investigate a complex multi-configurational adsorbate system revealing adsorptions geometries and hierarchy and geometry of molecular orbitals.
- Pavel Kliuiev
- , Giovanni Zamborlini
- & Luca Castiglioni
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Article
| Open AccessA generalized Stark effect electromodulation model for extracting excitonic properties in organic semiconductors
The development of a generalized electromodulation (EM) spectroscopy model that accurately extracts material parameters for organic electronics remains a challenge. Here, the authors report an EM model that enhances parameter extraction accuracy by accounting for optical interference effects.
- Taili Liu
- , Yishu Foo
- & Sai-Wing Tsang
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Article
| Open AccessDynamic modulation of modal coupling in microelectromechanical gyroscopic ring resonators
Micro- and nanomechanical resonators play a crucial role in sensing applications. Here, the authors demonstrate electrically tunable modal coupling in capacitive microelectromechanical gyroscopic ring resonators that allows for improving the performance micro/nano-sensors relying on precise control of the degree of modal coupling.
- Xin Zhou
- , Chun Zhao
- & Ashwin A. Seshia
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Article
| Open AccessDynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction
Monitoring catalyst structural changes under working conditions is crucial for understanding how catalysts operate. Here, authors examine single-atom Ru electrocatalyst by operando synchrotron spectroscopies to identify the catalytic mechanism during the acidic oxygen evolution reaction.
- Linlin Cao
- , Qiquan Luo
- & Tao Yao
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Article
| Open AccessIn situ analysis of catalyst composition during gold catalyzed GaAs nanowire growth
Semiconductor nanowires are promising materials for miniaturized devices, but a thorough understanding of their growth mechanism is necessary for controlled synthesis. Here, the authors use in situ spectroscopy and microscopy to measure the composition of the catalyst droplet as a function of different growth parameters during Au-seeded GaAs nanowire growth.
- Carina B. Maliakkal
- , Daniel Jacobsson
- & Kimberly A. Dick
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Article
| Open AccessA physically cryptographic warhead verification system using neutron induced nuclear resonances
Inspection and authentication of warheads is important for nuclear safety and security. Here the authors report experimental scheme for the verification of nuclear warheads using the neutron resonance transmission analysis of a reference and candidate objects while preserving the sensitive information.
- Ezra M. Engel
- & Areg Danagoulian
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Article
| Open AccessQuantification of porosity in extensively nanoporous thin films in contact with gases and liquids
Thin porous layers are largely used, but a reliable method to quantify their porosity is missing. Here the authors demonstrate a method, based on quartz crystal microbalance measurements with dissipation monitoring, for accurate assessment of porosity and mechanical properties in thin porous films.
- Netanel Shpigel
- , Sergey Sigalov
- & Doron Aurbach
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Article
| Open AccessTunable assembly of truncated nanocubes by evaporation-driven poor-solvent enrichment
Versatile methods that can predictably assemble nanocrystals into large, well-ordered superlattices are rare. Here, the authors develop such a method–evaporation-driven poor-solvent enrichment–and rigorously determine the effect of various experimental parameters on the size, morphology, and mesoscopic order of the superlattices, giving the approach high predictive power.
- Zhong-Peng Lv
- , Martin Kapuscinski
- & Lennart Bergström
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Article
| Open AccessCharacterization of suprathermal electrons inside a laser accelerated plasma via highly-resolved K⍺-emission
Suprathermal electrons in laser-generated plasmas are potentially useful in many plasma environments. Here the authors show the characterization of suprathermal electrons in laser-generated Cu plasma using a high-resolution X-ray spectroscopy combined with hydrodynamic and atomic modeling.
- M. Šmíd
- , O. Renner
- & F. B. Rosmej
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Article
| Open AccessLarge-scale parallelization of nanomechanical mass spectrometry with weakly-coupled resonators
Designing large-scale parallelization of nanomechanical array measurements remains elusive. Here, the authors propose weak-coupling between similar devices to evaluate the resonance frequencies of a whole resonator array with a single measurement.
- Stefano Stassi
- , Giulia De Laurentis
- & Carlo Ricciardi
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Article
| Open AccessStiffening of graphene oxide films by soft porous sheets
Graphene oxide sheets have been used as a model system to study how the mechanical properties of individual 2D building blocks scale to their bulk form. Here the authors show that the modulus of multilayer graphene oxide films can be enhanced if some of the sheets are weakened by introducing in-plane porosity.
- Lily Mao
- , Hun Park
- & Jiaxing Huang
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Article
| Open AccessVirus lasers for biological detection
Many ligand-binding assays still rely on signals that scale linearly with probe concentration. The authors present lasing detection probes with a dye-labelled virus as the gain medium to optically amplify the signal, which could enable much higher signals than for fluorescent quantification.
- John E. Hales
- , Guy Matmon
- & Gabriel Aeppli
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Article
| Open AccessUnderstanding hydrogen-bonding structures of molecular crystals via electron and NMR nanocrystallography
Electron diffraction can be used to determine nanocrystal structures, but is unsuitable for locating hydrogen atoms. Here the authors combine electron diffraction, solid-state NMR and first-principles calculations to resolve the crystal structures and hydrogen-bonding networks of L-histidine and cimetidine form B.
- Candelaria Guzmán-Afonso
- , You-lee Hong
- & Yusuke Nishiyama
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Article
| Open AccessTime-resolved XUV ARPES with tunable 24–33 eV laser pulses at 30 meV resolution
Currently, it is difficult to reach high momenta with narrow energy resolution via laser-based angle-resolved photoemission spectroscopy (ARPES). Here, Sie et al. develop a time-resolved XUV based ARPES setup which can access the first Brillouin zone of all materials with narrow energy resolution.
- Edbert J. Sie
- , Timm Rohwer
- & Nuh Gedik
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Review Article
| Open AccessUnderstanding memristive switching via in situ characterization and device modeling
Memristor as the fourth basic element of electric circuits has drawn substantial attention for developing future computing technologies. Sun et al. report the progress and the challenges facing researchers on understanding memristive switching, and advocate continuous studies using a synergistic approach.
- Wen Sun
- , Bin Gao
- & Huaqiang Wu
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Article
| Open Access3D-structured supports create complete data sets for electron crystallography
3D electron crystallography enables structure determination of submicron-sized crystals, but obtaining complete data is difficult due to preferred orientations. Here the authors develop sample supports that allow sampling nanocrystals with full data completeness, and demonstrate this with ZSM-5 zeolites.
- Julian T. C. Wennmacher
- , Christian Zaubitzer
- & Tim Gruene
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Article
| Open AccessProbing a battery electrolyte drop with ambient pressure photoelectron spectroscopy
Here the authors probe a model electrolyte of a Li-ion battery for insights into the composition and concentration variation using ambient pressure photoelectron spectroscopy. The work highlights the necessity to stabilize the liquid phases and to differentiate surface and bulk compositions in the measurements.
- Julia Maibach
- , Ida Källquist
- & Maria Hahlin
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Article
| Open AccessNon-conventional mechanism of ferroelectric fatigue via cation migration
Ferroelectric fatigue degrades ferroelectric properties upon polarization cycling, but its underlying chemistry is poorly understood. Here, the authors show by multimodal chemical imaging that fatigue in PbZr0.2Ti0.8O3 thin films is associated with Cu + ions migration from the electrode into the film structure.
- Anton V. Ievlev
- , Santosh KC
- & Olga S. Ovchinnikova
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Article
| Open AccessProvenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material
The larger particulates from reactor Unit 1 of the Fukushima Daiichi Nuclear Power Plant have received sparse attention compared to the Unit 2 particulate. Here the authors perform the higher-resolution and 3-dimentional analysis of several high-density micron-scale fragments, from within a larger Unit 1-derived representative ejecta particle.
- Peter G. Martin
- , Marion Louvel
- & Thomas B. Scott
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Article
| Open AccessLocal atomic order and hierarchical polar nanoregions in a classical relaxor ferroelectric
The understanding of relaxor ferroelectrics is hindered by the complexity of nanoscale perturbations of their structure. Here, a data set of independent techniques treated on common footing provides a multiscale description of atomic order which reconciles conflicting models derived from single methods.
- M. Eremenko
- , V. Krayzman
- & I. Levin
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Article
| Open AccessAtomic-scale mapping of hydrophobic layers on graphene and few-layer MoS2 and WSe2 in water
Interfacial water plays a crucial role in mediating hydrophobic interactions. Here, the authors directly image the interfacial water organization in graphene, few-layer MoS2 and WSe2 through 3D-AFM technique to unveil that the distance between adjacent layers is about 0.30 nm larger than theoretically predicted values.
- Manuel R. Uhlig
- , Daniel Martin-Jimenez
- & Ricardo Garcia
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Article
| Open AccessAtomic-resolution imaging of surface and core melting in individual size-selected Au nanoclusters on carbon
Much remains unresolved about the mechanisms of nanoparticle melting. Here, by observing and simulating individual gold nanoclusters at atomic level as they are heated inside an electron microscope, the authors find that the particle surface melts before the interior. Their experimental results in combination with the atomistic simulations confirm the coexistence of a liquid shell and solid core during melting, as well as size-dependent melting point suppression.
- D. M. Foster
- , Th. Pavloudis
- & R. E. Palmer
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Article
| Open AccessPartitioning surface ligands on nanocrystals for maximal solubility
Entropic ligands can dramatically improve the solubility of nanocrystals, but it is not known how these mixed ligand systems actually arrange and interact on a particle surface. Here, the authors use advanced solid-state NMR techniques to understand the partitioning and dynamics of entropic mixed ligand shells on CdSe nanocrystals, and relate this molecular picture to the particles’ macroscopic solubility behavior.
- Zhenfeng Pang
- , Jun Zhang
- & Xiaogang Peng
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Article
| Open AccessFast lithium growth and short circuit induced by localized-temperature hotspots in lithium batteries
Operation of lithium batteries at high, non-uniform temperatures can lead to safety issues, but the effects of localized high temperatures are difficult to probe. Here the authors use micro-Raman spectroscopy to show that local-temperature hotspots can induce lithium metal growth and trigger circuit shorting.
- Yangying Zhu
- , Jin Xie
- & Yi Cui
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Article
| Open AccessRapid evaluation of bioactive Ti-based surfaces using an in vitro titration method
In vitro testing of implant materials bioactivity is important and the current methods take time. Here, the authors report on the development of a faster titration based method for assessing the mineralization activity of materials and validate the method in vitro and in vivo using titanium surfaces.
- Weitian Zhao
- , David Michalik
- & Paul Bowen
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Article
| Open AccessStand-off nuclear reactor monitoring with neutron detectors for safeguards and non-proliferation applications
Nuclear power reactors need to be monitored for safety and security while in operation. Here the authors discuss monitoring and safeguarding research reactors and small modular reactors using detection of neutrons up to a hundred meters away from the reactor shielding.
- B. M. van der Ende
- , L. Li
- & B. Sur
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Article
| Open AccessLaser restructuring and photoluminescence of glass-clad GaSb/Si-core optical fibres
Semiconductor-core optical fibres are of interest for their non-linear optical and electro-optical properties. Here, GaSb/Si composite-core optical fibres were fabricated and a CO2 laser was used to facilitate controlled GaSb segregation within the silicon. This has implications for embedding light sources in IR-transmitting fibers
- S. Song
- , K. Lønsethagen
- & U. J. Gibson
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Article
| Open AccessA stochastic view on surface inhomogeneity of nanoparticles
Determining the spatial arrangement of molecules on a nanoparticle’s surface is key to understanding its interactions. Here, the authors use dSTORM imaging and probabilistic modelling to map the distribution of fluorophores on a nanoparticle, finding that ligand coverage is heterogeneous and highly variable between individual particles.
- R. A. J. Post
- , D. van der Zwaag
- & R. W. van der Hofstad
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Article
| Open AccessExistence of multiple critical cooling rates which generate different types of monolithic metallic glass
Quantifying the complexity of glass formation is difficult because it usually requires cooling at enormous speeds. Here, the authors use fast differential scanning calorimetry to classify metallic glasses into two types, one with quenched-in nuclei and one without.
- Jürgen E. K. Schawe
- & Jörg F. Löffler
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Article
| Open AccessLabel-free detection of conformational changes in switchable DNA nanostructures with microwave microfluidics
Methods to study conformational changes in biomolecules are limited in resolution and require labelling or other modifications of target analytes. Here the authors present a label-free, microwave microfluidic approach to detect conformational changes of DNA nanostructures based on ionic conductivity.
- Angela C. Stelson
- , Minghui Liu
- & James C. Booth
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Article
| Open AccessUltrafast photonic micro-systems to manipulate hard X-rays at 300 picoseconds
It is desirable to improve spatiotemporal control of light generated by synchrotron user facilities or table-top X-ray sources. Here the authors demonstrate manipulation of hard X-rays using microelectro mechanical systems (MEMS) oscillators on timescales of 300 ps, approaching the synchrotron pulse width.
- Pice Chen
- , Il Woong Jung
- & Jin Wang
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Article
| Open AccessTime-space-resolved origami hierarchical electronics for ultrasensitive detection of physical and chemical stimuli
Developing portable, disposable and cost-effective electronics for multifunctional sensing is desirable. Here, the authors present origami-based hierarchical electronics with time-space-resolved high-discriminative pattern recognition (TSR-HDPR) features for multifunctional detection of complex physical and chemical stimuli.
- Min Zhang
- , Jiaxing Jeccy Sun
- & Hossam Haick
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Article
| Open AccessIn-situ aerosol nanoparticle characterization by small angle X-ray scattering at ultra-low volume fraction
State‐of‐the‐art aerosol nanoparticle techniques are limited by the shortcomings of removing the nanoparticles from their original environment. Here, the authors apply small angle X‐ray scattering as an in‐situ measurement technique, enabling the measurement of the primary particles and the aggregates.
- P. S. Bauer
- , H. Amenitsch
- & P. M. Winkler
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Article
| Open AccessThermochemiluminescent peroxide crystals
Chemiluminescence is known in solution, but has remained undetected in macroscopic crystalline solids so far. Here the authors demonstrate direct transduction of heat into light by thermochemiluminescence in a centimeter-size lophine hydroperoxide crystal.
- Stefan Schramm
- , Durga Prasad Karothu
- & Panče Naumov
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Article
| Open AccessAtomic insight into hydration shells around facetted nanoparticles
Experimental structural insight into hydration shells around nanoparticles is challenging. Here the authors use X-ray scattering and pair distribution function analysis to reveal interatomic distances in the very first adsorbed water layer as well as extended restructured layers out to 15 Å, with a bulk-like signature.
- Sabrina L. J. Thomä
- , Sebastian W. Krauss
- & Mirijam Zobel
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Article
| Open AccessStrain engineering in perovskite solar cells and its impacts on carrier dynamics
The residual strains in the mixed halide perovskite thin films and their effects on the solar cell devices are less understood. Here Zhu et al. study the impact of the gradient in-plane strain on the carrier dynamics of the strained perovskite films and optimize the device efficiency.
- Cheng Zhu
- , Xiuxiu Niu
- & Qi Chen
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Article
| Open AccessUltimate limit in size and performance of WSe2 vertical diodes
Vertical charge transport through homogeneous WSe2 layers can be effectively tuned by the layer number and contacting metals deposited. Here, the authors report WSe2 vertical diodes with superior device performance characteristics based on variable WSe2 thickness and gadolinium and platinum contact metals.
- Ghazanfar Nazir
- , Hakseong Kim
- & Suyong Jung
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Matters Arising
| Open AccessCharacterizing coral skeleton mineralogy with Raman spectroscopy
- Thomas M. DeCarlo
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Article
| Open AccessAll-optical field-free three-dimensional orientation of asymmetric-top molecules
Alignment and orientation of the molecules allows studying the photon-molecule interactions in greater detail. Here the authors demonstrate the three-dimensional orientation of SO2 molecules in using COLTRIMS and orthogonally polarized laser pulses but in the absence of DC field.
- Kang Lin
- , Ilia Tutunnikov
- & Jian Wu
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Article
| Open Access39Ar dating with small samples provides new key constraints on ocean ventilation
The rare noble gas isotope 39Ar is the ideal tracer to investigate the ventilation of the deep ocean in the time range of 50 to 1000 years. Here the authors constrain transit time distributions in the eastern Tropical Atlantic with 39Ar-measurements done on a sample size of 5 L of water utilising modern atom-optical techniques.
- Sven Ebser
- , Arne Kersting
- & Markus K. Oberthaler
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Article
| Open AccessApparent self-heating of individual upconverting nanoparticle thermometers
Nanoparticles are often used as nanothermometers by measuring their luminescence from upconverted energy under illumination. The authors uncover the artificial appearance of a temperature rise at high excitation intensities due to effects involving higher energy states.
- Andrea D. Pickel
- , Ayelet Teitelboim
- & Chris Dames
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Article
| Open AccessDetermination of the two-dimensional distributions of gold nanorods by multiwavelength analytical ultracentrifugation
Characterization of nanoparticles is a complex and important problem for the vast number of applications that require them. Here, the authors present a method to uncover the two-dimensional distribution of length and diameter of anisotropic nanoparticles like gold nanorods with a single measurement by combining spectroscopic and sedimentation data.
- Simon E. Wawra
- , Lukas Pflug
- & Wolfgang Peukert
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Article
| Open AccessDirect oxygen isotope effect identifies the rate-determining step of electrocatalytic OER at an oxidic surface
Understanding reaction mechanisms is crucial for catalyst design. Here, natural-abundance isotope quantifications of O2 yield mechanistically significant reaction kinetic isotope effects for water oxidation over metal oxide electrodes, the bottleneck step of water electrolysis.
- Sandra Haschke
- , Michael Mader
- & Julien Bachmann
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Article
| Open AccessA high-energy sulfur cathode in carbonate electrolyte by eliminating polysulfides via solid-phase lithium-sulfur transformation
Carbonate-based electrolytes can impart advantages in lithium sulfur batteries, but performance is often limited by incompatibility with sulfur-based cathodes. Here the authors elucidate a mechanism for conversion of sulfur to lithium sulfide and demonstrate improved performance in a Li-S cell.
- Xia Li
- , Mohammad Banis
- & Xueliang Sun
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Article
| Open AccessMass spectrometry and Monte Carlo method mapping of nanoparticle ligand shell morphology
Determining the arrangement of ligands on a nanoparticle is challenging, given the limitations of existing characterization tools. Here, the authors describe an accessible method for resolving ligand shell morphology that uses simple MALDI-TOF mass spectrometry measurements in conjunction with an open-access Monte Carlo fitting program.
- Zhi Luo
- , Yanfei Zhao
- & Francesco Stellacci
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Article
| Open AccessPhase-controlled Fourier-transform spectroscopy
Fourier transform spectrometers are generally limited to slow scanning rates at high resolution. Here the authors demonstrate highly efficient Fourier transform spectroscopy using a dynamic phase-control technique that enables fast acquisition without compromising bandwidth or resolution.
- Kazuki Hashimoto
- & Takuro Ideguchi
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Article
| Open AccessSingle Particle Automated Raman Trapping Analysis
Enabling concurrent, high throughput analysis of single nano particles would greatly increase the capacity to study size, composition and inter and intra particle population variance. Here, the authors present a comprehensive platform for single particle automated Raman trapping analysis without any target modification.
- Jelle Penders
- , Isaac J. Pence
- & Molly M. Stevens
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Article
| Open AccessSpectral field mapping in plasmonic nanostructures with nanometer resolution
Characterizing plasmonic coupling has proven elusive. Here, the authors obtain a spectrally resolved deflection map related to a focused electron beam, which has excited a surface plasmon resonance, and relate this deflection to the spectral component of the induced electric and magnetic fields pertaining to the mode.
- J. Krehl
- , G. Guzzinati
- & A. Lubk