Single-Pixel Imaging in Space and Time with Optically Modulated Free Electrons.

Single-pixel imaging, originally developed in light optics, facilitates fast three-dimensional sample reconstruction as well as probing with light wavelengths undetectable by conventional multi-pixel detectors. However, the spatial resolution of optics-based single-pixel microscopy is limited by diffraction to hundreds of nanometers. Here, we propose an implementation of single-pixel imaging relying on attainable modifications of currently available ultrafast electron microscopes in which optically modulated electrons are used instead of photons to achieve subnanometer spatially and temporally resolved single-pixel imaging. We simulate electron beam profiles generated by interaction with the optical field produced by an externally programmable spatial light modulator and demonstrate the feasibility of the method by showing that the sample image and its temporal evolution can be reconstructed using realistic imperfect illumination patterns. Electron single-pixel imaging holds strong potential for application in low-dose probing of beam-sensitive biological and molecular samples, including rapid screening during in situ experiments.

Near-real-time diagnosis of electron optical phase aberrations in scanning transmission electron microscopy using an artificial neural network.

The key to optimizing spatial resolution in a state-of-the-art scanning transmission electron microscope is the ability to measure and correct for electron optical aberrations of the probe-forming lenses precisely. Several diagnostic methods for aberration measurement and correction have been proposed, albeit often at the cost of relatively long acquisition times. Here, we illustrate how artificial intelligence can be used to provide near-real-time diagnosis of aberrations from individual Ronchigrams. The demonstrated speed of aberration measurement is important because microscope conditions can change rapidly. It is also important for the operation of MEMS-based hardware correction elements, which have less intrinsic stability than conventional electromagnetic lenses.

Ultrafast Transverse Modulation of Free Electrons by Interaction with Shaped Optical Fields.

Spatiotemporal electron-beam shaping is a bold frontier of electron microscopy. Over the past decade, shaping methods evolved from static phase plates to low-speed electrostatic and magnetostatic displays. Recently, a swift change of paradigm utilizing light to control free electrons has emerged. Here, we experimentally demonstrate arbitrary transverse modulation of electron beams without complicated electron-optics elements or material nanostructures, but rather using shaped light beams. On-demand spatial modulation of electron wavepackets is obtained via inelastic interaction with transversely shaped ultrafast light fields controlled by an external spatial light modulator. We illustrate this method for the cases of Hermite-Gaussian and Laguerre-Gaussian modulation and discuss their use in enhancing microscope sensitivity. Our approach dramatically widens the range of patterns that can be imprinted on the electron profile and greatly facilitates tailored electron-beam shaping.

Automatic Alignment of an Orbital Angular Momentum Sorter in a Transmission Electron Microscope Using a Convolutional Neural Network.

We report on the automatic alignment of a transmission electron microscope equipped with an orbital angular momentum sorter using a convolutional neural network. The neural network is able to control all relevant parameters of both the electron-optical setup of the microscope and the external voltage source of the sorter without input from the user. It can compensate for mechanical and optical misalignments of the sorter, in order to optimize its spectral resolution. The alignment is completed over a few frames and can be kept stable by making use of the fast fitting time of the neural network.

Multipole-phase division multiplexing.

The control of structured waves has recently opened innovative scenarios in the perspective of radiation propagation, advanced imaging, and light-matter interaction. In information and communication technology, the spatial degrees of freedom offer a wider state space to carry many channels on the same frequency or increase the dimensionality of quantum protocols. However, spatial decomposition is much more arduous than polarization or frequency multiplexing, and very few practical examples exist. Among all, beams carrying orbital angular momentum gained a preeminent role, igniting a variety of methods and techniques to generate, tailor, and measure that property. In a more general insight into structured-phase beams, we introduce here a new family of wave fields having a multipole phase. These beams are devoid of phase singularities and described by two continuous spatial parameters which can be controlled in a practical and compact way via conformal optics. The outlined framework encompasses multiplexing, propagation, and demultiplexing as a whole for the first time, describing the evolution and transformation of wave fields in terms of conformal mappings. With its potentialities, versatility, and ease of implementation, this new paradigm introduces a novel playground for space division multiplexing, suggesting unconventional solutions for light processing and free-space communications.

Single-particle cryo-EM: alternative schemes to improve dose efficiency.

Imaging of biomolecules by ionizing radiation, such as electrons, causes radiation damage which introduces structural and compositional changes of the specimen. The total number of high-energy electrons per surface area that can be used for imaging in cryogenic electron microscopy (cryo-EM) is severely restricted due to radiation damage, resulting in low signal-to-noise ratios (SNR). High resolution details are dampened by the transfer function of the microscope and detector, and are the first to be lost as radiation damage alters the individual molecules which are presumed to be identical during averaging. As a consequence, radiation damage puts a limit on the particle size and sample heterogeneity with which electron microscopy (EM) can deal. Since a transmission EM (TEM) image is formed from the scattering process of the electron by the specimen interaction potential, radiation damage is inevitable. However, we can aim to maximize the information transfer for a given dose and increase the SNR by finding alternatives to the conventional phase-contrast cryo-EM techniques. Here some alternative transmission electron microscopy techniques are reviewed, including phase plate, multi-pass transmission electron microscopy, off-axis holography, ptychography and a quantum sorter. Their prospects for providing more or complementary structural information within the limited lifetime of the sample are discussed.

A sorter for electrons based on magnetic elements.

The orbital angular momentum (OAM) sorter is an electron optical device for the measurement of an electron's OAM. It is based on two phase elements, which are referred to as an "unwrapper" and a "corrector" and are located in Fourier conjugate planes. The simplest implementation of the sorter is based on electrostatic phase elements, such as a charged needle for the unwrapper and electrodes with alternating charges or potentials for the corrector. Here, we use a formal analogy between phase shifts introduced by charges and vertical currents to propose alternative designs for the sorter elements, which are based on phase shifts introduced by magnetic fields. We use this concept to provide a general guide for phase element design, which promises to provide improved reliability of phase control in electron optics.

Experimental Demonstration of an Electrostatic Orbital Angular Momentum Sorter for Electron Beams.

The component of orbital angular momentum (OAM) in the propagation direction is one of the fundamental quantities of an electron wave function that describes its rotational symmetry and spatial chirality. Here, we demonstrate experimentally an electrostatic sorter that can be used to analyze the OAM states of electron beams in a transmission electron microscope. The device achieves postselection or sorting of OAM states after electron-material interactions, thereby allowing the study of new material properties such as the magnetic states of atoms. The required electron-optical configuration is achieved by using microelectromechanical systems technology and focused ion beam milling to control the electron phase electrostatically with a lateral resolution of 50 nm. An OAM resolution of 1.5ℏ is realized in tests on controlled electron vortex beams, with the perspective of reaching an optimal OAM resolution of 1ℏ in the near future.

Exploring the Spatial Features of Electronic Transitions in Molecular and Biomolecular Systems by Swift Electrons.

We devise a new kind of experiment that extends the technology of electron energy loss spectroscopy to probe (supra-)molecular systems: by using an electron beam in a configuration that avoids molecular damage and a very recently introduced electron optics setup for the analysis of the outcoming electrons, one can obtain information on the spatial features of the investigated excitations. Physical insight into the proposed experiment is provided by means of a simple but rigorous model to obtain the transition rate and selection rule. Numerical simulations of DNA G-quadruplexes and other biomolecular systems, based on time dependent density functional theory calculations, point out that the conceived new technique can probe the multipolar components and even the chirality of molecular transitions, superseding the usual optical spectroscopies for those cases that are problematic, such as dipole-forbidden transitions, at a very high spatial resolution.

Defect-assisted synthesis of magneto-plasmonic silver-spinel ferrite heterostructures in a flower-like architecture.

Artificial nano-heterostructures (NHs) with controlled morphology, obtained by combining two or more components in several possible architectures, make them suitable for a wide range of applications. Here, we propose an oleate-based solvothermal approach to design silver-spinel ferrite flower-like NHs. Small oleate-coated silver nanoparticles were used as seeds for the growth of magnetic spinel ferrite (cobalt ferrite and spinel iron oxide) nanodomains on their surface. With the aim of producing homogeneous flower-like heterostructures, a careful study of the effect of the concentration of precursors, the reaction temperature, the presence of water, and the chemical nature of the spinel ferrite was carried out. The magnetic and optical properties of the NHs were also investigated. A heterogeneous growth of the spinel ferrite phase on the silver nanoparticles, through a possible defect-assisted mechanism, was suggested in the light of the high concentration of stacking faults (intrinsic and twins) in the silver seeds, revealed by Rietveld refinement of powder X-ray diffraction patterns and High-Resolution electron microscopy.

Design of electrostatic phase elements for sorting the orbital angular momentum of electrons.

The orbital angular momentum (OAM) sorter is a new electron optical device for measuring an electron's OAM. It is based on two phase elements, which are referred to as the "unwrapper" and "corrector" and are placed in Fourier-conjugate planes in an electron microscope. The most convenient implementation of this concept is based on the use of electrostatic phase elements, such as a charged needle as the unwrapper and a set of electrodes with alternating charges as the corrector. Here, we use simulations to assess the role of imperfections in such a device, in comparison to an ideal sorter. We show that the finite length of the needle and the boundary conditions introduce astigmatism, which leads to detrimental cross-talk in the OAM spectrum. We demonstrate that an improved setup comprising three charged needles can be used to compensate for this aberration, allowing measurements with a level of cross-talk in the OAM spectrum that is comparable to the ideal case.

In-plane Aligned Colloidal 2D WS2 Nanoflakes for Solution-Processable Thin Films with High Planar Conductivity.

Two-dimensional transition-metal dichalcolgenides (2D-TMDs) are among the most intriguing materials for next-generation electronic and optoelectronic devices. Albeit still at the embryonic stage, building thin films by manipulating and stacking preformed 2D nanosheets is now emerging as a practical and cost-effective bottom-up paradigm to obtain excellent electrical properties over large areas. Herein, we exploit the ultrathin morphology and outstanding solution stability of 2D WS2 colloidal nanocrystals to make thin films of TMDs assembled on a millimetre scale by a layer-by-layer deposition approach. We found that a room-temperature surface treatment with a superacid, performed with the precise scope of removing the native insulating surfactants, promotes in-plane assembly of the colloidal WS2 nanoflakes into stacks parallel to the substrate, along with healing of sulphur vacancies in the lattice that are detrimental to electrical conductivity. The as-obtained 2D WS2 thin films, characterized by a smooth and compact morphology, feature a high planar conductivity of up to 1 µS, comparable to the values reported for epitaxially grown WS2 monolayers, and enable photocurrent generation upon light irradiation over a wide range of visible to near-infrared frequencies.

Mechanistic insight into the formation of colloidal WS2 nanoflakes in hot alkylamine media.

Developing convenient and reliable synthetic methodologies for solution processable 2D layered ultrathin nanostructures with lateral size control is one of the major challenges for practical applications. In this study, a rational understanding a long-chain amphiphilic surfactant assisted non-hydrolytic synthesis that is able to generate dimension-controllable 2D-WS2 nanocrystal flakes in a single-step protocol is proposed. The evolution of the starting soft organic-inorganic lamellar template into ultrathin few-layer 2D-WS2 nanostructures with lateral size modulation over a range between 3 and 30 nm is monitored. The initial formation of WS2 nanoseeds occurs in a self-assembled sacrificial precursor source, acting as a template, where larger two-dimensional nanostructures can grow without undergoing significant thickness variation. Overall, the chemical nature and steric hindrance of the alkylamines are essential to modulate the reactivity of such WS2 nanoclusters, which correlate with the lateral size of the resulting nanoflakes.

Magnetic Shape Memory Turns to Nano: Microstructure Controlled Actuation of Free-Standing Nanodisks.

Magnetic shape memory materials hold a great promise for next-generation actuation devices and systems for energy conversion, thanks to the intimate coupling between structure and magnetism in their martensitic phase. Here novel magnetic shape memory free-standing nanodisks are proposed, proving that the lack of the substrate constrains enables the exploitation of new microstructure-controlled actuation mechanisms by the combined application of different stimuli-i.e., temperature and magnetic field. The results show that a reversible areal strain (up to 5.5%) can be achieved and tuned in intensity and sign (i.e., areal contraction or expansion) by the application of a magnetic field. The mechanisms at the basis of the actuation are investigated by experiments performed at different length scales and directly visualized by several electron microscopy techniques, including electron holography, showing that thermo/magnetomechanical properties can be optimized by engineering the martensitic microstructure through epitaxial growth and lateral confinement. These findings represent a step forward toward the development of a new class of temperature-field controlled nanoactuators and smart nanomaterials.

Towards a holographic approach to spherical aberration correction in scanning transmission electron microscopy.

Recent progress in phase modulation using nanofabricated electron holograms has demonstrated how the phase of an electron beam can be controlled. In this paper, we apply this concept to the correction of spherical aberration in a scanning transmission electron microscope and demonstrate an improvement in spatial resolution. Such a holographic approach to spherical aberration correction is advantageous for its simplicity and cost-effectiveness.

Generalized optical angular momentum sorter and its application to high-dimensional quantum cryptography.

The orbital angular momentum (OAM) carried by optical beams is a useful quantity for encoding information. This form of encoding has been incorporated into various works ranging from telecommunications to quantum cryptography, most of which require methods that can rapidly process the OAM content of a beam. Among current state-of-the-art schemes that can readily acquire this information are so-called OAM sorters, which consist of devices that spatially separate the OAM components of a beam. Such devices have found numerous applications in optical communications, a field that is in constant demand for additional degrees of freedom, such as polarization and wavelength, into which information can also be encoded. Here, we report the implementation of a device capable of sorting a beam based on its OAM and polarization content, which could be of use in works employing both of these degrees of freedom as information channels. After characterizing our fabricated device, we demonstrate how it can be used for quantum communications via a quantum key distribution protocol.

Observation of nanoscale magnetic fields using twisted electron beams.

Electron waves give an unprecedented enhancement to the field of microscopy by providing higher resolving power compared to their optical counterpart. Further information about a specimen, such as electric and magnetic features, can be revealed in electron microscopy because electrons possess both a magnetic moment and charge. In-plane magnetic structures in materials can be studied experimentally using the effect of the Lorentz force. On the other hand, full mapping of the magnetic field has hitherto remained challenging. Here we measure a nanoscale out-of-plane magnetic field by interfering a highly twisted electron vortex beam with a reference wave. We implement a recently developed holographic technique to manipulate the electron wavefunction, which gives free electrons an additional unbounded quantized magnetic moment along their propagation direction. Our finding demonstrates that full reconstruction of all three components of nanoscale magnetic fields is possible without tilting the specimen.Beyond high resolving power, electron microscopy can be used to study both the electronic and magnetic properties of a sample. Here, Grillo et al. combine electron vortex beams with holographic detection to measure out-of-plane nanoscale magnetic fields.

Measuring the orbital angular momentum spectrum of an electron beam.

Electron waves that carry orbital angular momentum (OAM) are characterized by a quantized and unbounded magnetic dipole moment parallel to their propagation direction. When interacting with magnetic materials, the wavefunctions of such electrons are inherently modified. Such variations therefore motivate the need to analyse electron wavefunctions, especially their wavefronts, to obtain information regarding the material's structure. Here, we propose, design and demonstrate the performance of a device based on nanoscale holograms for measuring an electron's OAM components by spatially separating them. We sort pure and superposed OAM states of electrons with OAM values of between -10 and 10. We employ the device to analyse the OAM spectrum of electrons that have been affected by a micron-scale magnetic dipole, thus establishing that our sorter can be an instrument for nanoscale magnetic spectroscopy.