Controlling free electrons with optical whispering-gallery modes.

Free-electron beams are versatile probes of microscopic structure and composition1,2, and have revolutionized atomic-scale imaging in several fields, from solid-state physics to structural biology3. Over the past decade, the manipulation and interaction of electrons with optical fields have enabled considerable progress in imaging methods4, near-field electron acceleration5,6, and four-dimensional microscopy techniques with high temporal and spatial resolution7. However, electron beams typically couple only weakly to optical excitations, and emerging applications in electron control and sensing8-11 require large enhancements using tailored fields and interactions. Here we couple a free-electron beam to a travelling-wave resonant cavity mode. The enhanced interaction with the optical whispering-gallery modes of dielectric microresonators induces a strong phase modulation on co-propagating electrons, which leads to a spectral broadening of 700 electronvolts, corresponding to the absorption and emission of hundreds of photons. By mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the lifetime of the the microresonator following a femtosecond excitation and observe the spectral response of the cavity. The natural matching of free electrons to these quintessential optical modes could enable the application of integrated photonics technology in electron microscopy, with broad implications for attosecond structuring, probing quantum emitters and possible electron-light entanglement.

Observation of fluctuation-mediated picosecond nucleation of a topological phase.

Topological states of matter exhibit fascinating physics combined with an intrinsic stability. A key challenge is the fast creation of topological phases, which requires massive reorientation of charge or spin degrees of freedom. Here we report the picosecond emergence of an extended topological phase that comprises many magnetic skyrmions. The nucleation of this phase, followed in real time via single-shot soft X-ray scattering after infrared laser excitation, is mediated by a transient topological fluctuation state. This state is enabled by the presence of a time-reversal symmetry-breaking perpendicular magnetic field and exists for less than 300 ps. Atomistic simulations indicate that the fluctuation state largely reduces the topological energy barrier and thereby enables the observed rapid and homogeneous nucleation of the skyrmion phase. These observations provide fundamental insights into the nature of topological phase transitions, and suggest a path towards ultrafast topological switching in a wide variety of materials through intermediate fluctuating states.

Probing Chirality with Inelastic Electron-Light Scattering.

Circular dichroism spectroscopy is an essential technique for understanding molecular structure and magnetic materials; however, spatial resolution is limited by the wavelength of light, and sensitivity sufficient for single-molecule spectroscopy is challenging. We demonstrate that electrons can efficiently measure the interaction between circularly polarized light and chiral materials with deeply subwavelength resolution. By scanning a nanometer-sized focused electron beam across an optically excited chiral nanostructure and measuring the electron energy spectrum at each probe position, we produce a high-spatial-resolution map of near-field dichroism. This technique offers a nanoscale view of a fundamental symmetry and could be employed as "photon staining" to increase biomolecular material contrast in electron microscopy.

Probing Light Atoms at Subnanometer Resolution: Realization of Scanning Transmission Electron Microscope Holography.

Atomic resolution imaging of light elements in electron-transparent materials has long been a challenge. Biomolecular materials, for example, are rapidly altered by incident electrons. We demonstrate a scanning transmission electron microscopy (STEM) technique, called STEM holography, capable of efficient structural analysis of beam-sensitive nanomaterials. STEM holography measures the absolute phase and amplitude of electrons passed through a specimen via interference with a vacuum reference wave. We use an amplitude-dividing nanofabricated grating to prepare multiple beams focused at the sample. We configure the postspecimen microscope imaging system to overlap the beams, forming an interference pattern. We record and analyze the pattern at each 2D-raster-scan-position, reconstructing the complex object wave. As a demonstration, we image gold nanoparticles on an amorphous carbon substrate at 2.4 Å resolution. STEM holography offers higher contrast of the carbon while maintaining gold atomic lattice resolution compared to high angle annular dark field STEM.

Origins and demonstrations of electrons with orbital angular momentum.

The surprising message of Allen et al. (Allen et al. 1992 Phys. Rev. A 45, 8185 (doi:10.1103/PhysRevA.45.8185)) was that photons could possess orbital angular momentum in free space, which subsequently launched advancements in optical manipulation, microscopy, quantum optics, communications, many more fields. It has recently been shown that this result also applies to quantum mechanical wave functions describing massive particles (matter waves). This article discusses how electron wave functions can be imprinted with quantized phase vortices in analogous ways to twisted light, demonstrating that charged particles with non-zero rest mass can possess orbital angular momentum in free space. With Allen et al. as a bridge, connections are made between this recent work in electron vortex wave functions and much earlier works, extending a 175 year old tradition in matter wave vortices.This article is part of the themed issue 'Optical orbital angular momentum'.

Streamlined approach to mapping the magnetic induction of skyrmionic materials.

Recently, Lorentz transmission electron microscopy (LTEM) has helped researchers advance the emerging field of magnetic skyrmions. These magnetic quasi-particles, composed of topologically non-trivial magnetization textures, have a large potential for application as information carriers in low-power memory and logic devices. LTEM is one of a very few techniques for direct, real-space imaging of magnetic features at the nanoscale. For Fresnel-contrast LTEM, the transport of intensity equation (TIE) is the tool of choice for quantitative reconstruction of the local magnetic induction through the sample thickness. Typically, this analysis requires collection of at least three images. Here, we show that for uniform, thin, magnetic films, which includes many skyrmionic samples, the magnetic induction can be quantitatively determined from a single defocused image using a simplified TIE approach.

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.

Efficient linear phase contrast in scanning transmission electron microscopy with matched illumination and detector interferometry.

The ability to image light elements in soft matter at atomic resolution enables unprecedented insight into the structure and properties of molecular heterostructures and beam-sensitive nanomaterials. In this study, we introduce a scanning transmission electron microscopy technique combining a pre-specimen phase plate designed to produce a probe with structured phase with a high-speed direct electron detector to generate nearly linear contrast images with high efficiency. We demonstrate this method by using both experiment and simulation to simultaneously image the atomic-scale structure of weakly scattering amorphous carbon and strongly scattering gold nanoparticles. Our method demonstrates strong contrast for both materials, making it a promising candidate for structural determination of heterogeneous soft/hard matter samples even at low electron doses comparable to traditional phase-contrast transmission electron microscopy. Simulated images demonstrate the extension of this technique to the challenging problem of structural determination of biological material at the surface of inorganic crystals.