Photon-induced near-field electron microscopy (PINEM) has emerged as a powerful technique for imaging optical excitations with nanometer spatial and sub-picosecond temporal resolution. Recent years have extended the bandwidth of operation of PINEM experiments from the visible range to the mid-infrared, revealing the spatiotemporal dynamics of polaritons and their exotic phenomena. In this study, we nearly double the bandwidth of PINEM, going deeper into the infrared up to 12 um. Leveraging this advancement, we investigate the spatiotemporal dynamics of phonon polaritons (PhPs) in α-MoO3, a material of growing interest thanks to its in-plane anisotropy. Visualizing PhPs in a cavity-like flake reveals their spatial distribution, dynamics, and wavelength-dependent lifetime. Our work pushes the frontiers of PINEM imaging and highlights its potential for probing hard-to-access polaritonic properties of novel van der Waals materials.

Spatial and temporal light modulation is a well-established technology that enables dynamic shaping of the phase and amplitude of optical fields, significantly enhancing the resolution and sensitivity of imaging methods. Translating this capability to electron beams is highly desirable within the framework of a transmission electron microscope (TEM) to benefit from the nanometer spatial resolution of this instrument. In this work, we report on the experimental realization of a photonic-based free-electron modulator integrated into the column of two ultrafast TEMs for presample electron-beam shaping. Electron-photon interaction is employed to coherently modulate both the transverse and longitudinal components of the electron wave function (through lateral phase imprinting and temporal profiling, respectively), while leveraging dynamically controlled optical fields and tailored designs of the electron-laser-sample interaction geometry. Using energy- and momentum-resolved electron detection, we successfully reconstruct the shaped electron wave function at the TEM sample plane. These results demonstrate the ability to manipulate the electron wave function before probing the sample, paving the way for photonics-inspired imaging and spectroscopy techniques in ultrafast electron microscopy.

We present free-electron imaging of sub-cycle spatio-temporal dynamics of 2D polariton wavepackets, demonstrating the first simultaneous time-, space-, and phase-resolved measurement of such phenomena, and resolving their novel features like vortex-anti-vortex singularities for record-low intensities.

The tomography of photonic quantum states is key in quantum optics, impacting quantum sensing, computing, and communication. Conventional detectors are limited in their temporal and spatial resolution, hampering high-rate quantum communication and local addressing of photonic circuits. Here, we propose to utilize free electron-photon interactions for quantum state tomography, introducing electron homodyne detection with potential for femtosecond-temporal and nanometer-spatial resolutions. The detectable quantum information level depends on the electron-photon interaction strength. Our Letter opens avenues for free-electron-based photodetection utilizing the ultrafast, subwavelength, nondestructive nature of free electrons.

We experimentally demonstrate the generation of chiral electron beams in an ultrafast transmission electron microscope without the necessity for chiral light or chiral-shaping structures, but by breaking mirror symmetry in the light-electron interaction.

Accessing the low-energy non-equilibrium dynamics of materials with simultaneous spatial and temporal resolutions has been a bold frontier of electron microscopy in recent years. One of the main challenges is the ability to retrieve extremely weak signals while simultaneously disentangling amplitude and phase information. Here, we present an algorithm-based microscopy approach that uses light-induced electron modulation to demonstrate the coherent amplification effect in electron imaging of optical near-fields. We provide a simultaneous time-, space-, and phase-resolved measurement in a micro-drum made from a hexagonal boron nitride membrane, visualizing the sub-cycle spatio-temporal dynamics of 2D polariton wavepackets therein. The phase-resolved measurement reveals vortex-anti-vortex singularities on the polariton wavefronts, together with an intriguing phenomenon of a traveling wave mimicking the amplitude profile of a standing wave. Our experiments show a 20-fold coherent amplification of the near-field signal compared to conventional electron near-field imaging, resolving peak field intensities of ~W/cm2 (field amplitude of few kV/m). As a result, our work opens a path toward spatio-temporal electron microscopy of biological specimens and quantum materials - exciting yet sensitive samples, which are currently difficult to investigate.

We present a novel method to shape single-electron wavepackets via their interaction with tunable plasmonic fields. We further demonstrate the first instance of electron diffraction from a standing electromagnetic surface wave – a plasmonic Kapitza-Dirac effect.

Spatial modulation of electron beams is an essential tool for various applications such as nanolithography and imaging, yet its implementations are severely limited and inherently non-tunable. Conversely, light-driven electron spatial modulation could potentially allow arbitrary electron wavefront shaping via the underlying mechanism of photon-induced near-field electron microscopy (PINEM). Here, we present tunable photon-induced spatial modulation of electrons through their externally-controlled interaction with surface plasmon polaritons (SPPs). Using recently developed methods of shaping SPP patterns, we demonstrate a dynamic control of the electron beam with a variety of high-quality electron distributions. Intriguingly, by utilizing the intrinsic interaction nonlinearity, we attain the first observation of 2D spatial Rabi oscillations and generate electron features below the SPP wavelength. Our work paves the way to on-demand electron wavefront shaping at ultrafast timescales, with prospects for aberration correction, nano-fabrication and material characterization.

The interaction of free-electron pulses with THz near-fields imprints a rich structure on the electron spectrum. We exploit this interaction in an ultrafast electron microscope distinguishing THz-generating non-linear mechanisms of optical rectification and photo-Dember effect.

Cat states and Gottesman-Kitaev-Preskill (GKP) states play a key role in quantum computation and communication with continuous variables. The creation of such states relies on strong nonlinear light-matter interactions, which are widely available in microwave frequencies as in circuit quantum electrodynamics platforms. However, strong nonlinearities are hard to come by in optical frequencies, severely limiting the use of continuous variable quantum information in the optical range. Here we propose using the strong interactions of free electrons with light as a source for optical cat and GKP states. The strong interactions can be realized by phase-matching of free electrons with photonic structures such as optical waveguides and photonic crystals. Our approach enables the generation of optical GKP states with above 10 dB squeezing and fidelities above 90% at post-selection probability of 10%, even reaching >30% using an initially squeezed vacuum state. Furthermore, the free-electron interaction allows for conditional rotations on the photonic state, enabling to entangle a pair of GKP states into a GKP Bell state. Since electrons can interact resonantly with light across the electromagnetic spectrum, our approach may be used for the generation of cat and GKP states over the entire electromagnetic spectrum, from radio-waves to X-rays.

Controlling optical fields on the subwavelength scale is at the core of nanophotonics. Laser-driven nanophotonic particle accelerators promise a compact alternative to conventional radiofrequency-based accelerators. Efficient electron acceleration in nanophotonic devices critically depends on achieving nanometer control of the internal optical nearfield. However, these nearfields have so far been inaccessible due to the complexity of the devices and their geometrical constraints, hampering the design of future nanophotonic accelerators. Here we image the field distribution inside a nanophotonic accelerator, for which we developed a technique for frequency-tunable deep-subwavelength resolution of nearfields based on photon-induced nearfield electron-microscopy. Our experiments, complemented by 3D simulations, unveil surprising deviations in two leading nanophotonic accelerator designs, showing complex field distributions related to intricate 3D features in the device and its fabrication tolerances. We envision an extension of our method for full 3D field tomography, which is key for the future design of highly efficient nanophotonic devices.

Organic–inorganic lead halide perovskite materials have attractive properties not only for solar cells but also for LED because of their high performance and wavelength tunability. Such an efficient light-emitting and lasing nature are indispensable for their applications, and the essential needs are miniaturization and low lasing threshold. One material that satisfies these requirements is lead halide perovskite. To understand the time evolution of the interaction between light and matter in a perovskite crystal system, it is necessary to reveal the carrier dynamics in each crystal. In this study, the transient absorption spectra of CH 3 NH 3 PbBr 3 crystals were measured using a femtosecond transient absorption microscopy. Surprisingly, strong spectra modulation has been observed and these results indicate the charge separation on the surface of the crystal. Amplified spontaneous emission dynamics were also observed in the transient absorption spectra.

The complex range of interactions between electrons and electromagnetic fields gave rise to countless scientific and technological advances. A prime example is photon-induced nearfield electron microscopy (PINEM), enabling the detection of confined electric fields in illuminated nanostructures with unprecedented spatial resolution. However, PINEM is limited by its dependence on strong fields, making it unsuitable for sensitive samples, and its inability to resolve complex phasor information. Here, we leverage the nonlinear, overconstrained nature of PINEM to present an algorithmic microscopy approach, achieving far superior nearfield imaging capabilities. Our algorithm relies on free-electron Ramsey-type interferometry to produce orders-of-magnitude improvement in sensitivity and ambiguity-immune nearfield phase reconstruction, both of which are optimal when the electron exhibits a fully quantum behavior. Our results demonstrate the potential of combining algorithmic approaches with state-of-the-art modalities in electron microscopy and may lead to various applications from imaging sensitive biological samples to performing full-field tomography of confined light.

For over 80 years of research, the conventional description of free-electron radiation phenomena, such as Cherenkov radiation, has remained unchanged: classical three-dimensional electromagnetic waves. Interestingly, in reduced dimensionality, the properties of free-electron radiation are predicted to fundamentally change. Here, we present the first observation of Cherenkov surface waves, wherein free electrons emit narrow-bandwidth photonic quasiparticles propagating in two-dimensions. The low dimensionality and narrow bandwidth of the effect enable to identify quantized emission events through electron energy loss spectroscopy. Our results support the recent theoretical prediction that free electrons do not always emit classical light and can instead become entangled with the photons they emit. The two-dimensional Cherenkov interaction achieves quantum coupling strengths over two orders of magnitude larger than ever reported, reaching the single-electron-single-photon interaction regime for the first time with free electrons. Our findings pave the way to previously unexplored phenomena in free-electron quantum optics, facilitating bright, free-electron-based quantum emitters of heralded Fock states.

We show that the coherent interaction between free electrons and photons can be used for universal control of continuous-variable photonic quantum states in the form of Gottesman-Kitaev-Preskill (GKP) qubits. Specifically, we find that electron energy combs enable nondestructive measurements of the photonic state and can induce arbitrary gates. Moreover, a single electron interacting with multiple photonic modes can create highly entangled states such as Greenberger-Horne-Zeilinger states and cluster states of GKPs.

Quantized vortices are topological defects found in different two-dimensional geometries, from liquid crystals to ferromagnets, famously involved in spontaneous symmetry breaking and phase transitions. Their optical counterparts appear in planar geometries as a universal wave phenomenon, possessing topologically protected orbital angular momentum (OAM). So far, the spatiotemporal dynamics of optical vortices, including vortex-pair creation and annihilation, has been observed only in Bose–Einstein condensates. Here we observe optical vortices in van der Waals materials and measure their dynamics, including events of pair creation and annihilation. Vortices of opposite OAM are involved in pair creation/annihilation events, and their relative signs determine the surrounding field profile throughout their motion. The vortices are made of phonon polaritons in hexagonal boron nitride, which we directly probe using free electrons in an ultrafast transmission electron microscope. Our findings promote future investigations of vortex phenomena in van der Waals platforms, toward their use for chiral plasmonics, quantum simulators, and control over selection rules in light–matter interactions.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Laser light can modulate the kinetic energy spectrum of free electrons and induce extremely high acceleration gradients, which are instrumental to electron microscopy and electron acceleration, respectively. We present a design scheme for a silicon photonic slot waveguide which hosts a supermode to interact with free electrons. The efficiency of this interaction relies on the coupling strength per photon along the interaction length. We predict an optimum value of 0.4266, resulting in the maximum energy gain of 28.27 keV for an optical pulse energy of only 0.22 nJ and duration 1 ps. The acceleration gradient is 1.05 GeV/m, which is lower than the maximum imposed by the damage threshold of Si waveguides. Our scheme shows how the coupling efficiency and energy gain can be maximized without maximizing the acceleration gradient. It highlights the potential of silicon photonics technology in hosting electron-photon interactions with direct applications in free-electron acceleration, radiation sources, and quantum information science.

We present the first observation of phonon-polaritons in a planar-anisotropic 2D material using ultrafast transmission electron microscopy, revealing their spatiotemporal dynamics.

The ability to form monoenergetic electron beams is vital for high-resolution electron spectroscopy and imaging. Such capabilities are commonly achieved using an electron monochromator, which energy filters a dispersed electron beam, thus reducing the electron flux to yield down to meV energy resolution. This reduction in flux hinders the use of monochromators in many applications, such as ultrafast transmission electron microscopes (UTEMs). Here, we develop and demonstrate a mechanism for electron energy monochromation that does not reduce the flux-a lossless monochromator. The mechanism is based on the interaction of free-electron pulses with single-cycle THz near fields, created by nonlinear conversion of an optical laser pulse near the electron beam path inside a UTEM. Our experiment reduces the electron energy spread by a factor of up to 2.9 without compromising the beam flux. Moreover, as the electron-THz interaction takes place over an extended region of many tens of microns in free space, the realized technique is highly robust-granting uniform monochromation over a wide area, larger than the electron beam diameter. We further demonstrate the wide tunability of our method by monochromating the electron beam at multiple primary electron energies from 60 to 200 keV, studying the effect of various electron and THz parameters on its performance. Our findings have direct applications in the fast-growing field of ultrafast electron microscopy, allowing time- and energy-resolved studies of exciton physics, phononic vibrational resonances, charge transport effects, and optical excitations in the mid IR to the far IR.