Photon-induced Near-field Electron Microscopy (PINEM) effect has revealed the quantum interaction between free electrons and optical near filed, which demonstrated plenty of novel phenomena of manipulating free electron wave packet and detecting/shaping quantum photonic states. However, free electrons generally only absorb/emit one photon at a time, while the physical mechanism and phenomena of free electron-two-photon interaction have not been studied yet. Moreover, the relationship between PINEM and Kapitza-Dirac (KD) effect and nonlinear Compton scattering is still unclear. Here we develop the full quantum theory of electron-photon interaction considering the two-photon process. It is revealed that the emission/absorption of two photons by electrons can be greatly enhanced by manipulating the electric field component of optical near field, and the quantum interference between single-photon and two-photon processes can occur in some circumstances, which affects the photon number state, electron energy states and electron-photon entanglement. Meanwhile, it is found that the KD effect (elastic electron-photon scattering) and nonlinear Compton scattering (inelastic electron-photon scattering) are also a kind of two-photon process and the distribution of electrons can be deduced analytically based on the full quantum theory. Our work uncovers the possible abundant phenomena when free electron interacting with two photons, paves the way for more in-depth studies of nonlinear processes in electron-photon quantum interactions in the future.
Photon-induced Near-field Electron Microscopy (PINEM) effect has revealed the quantum interaction between free electrons and optical near filed, which demonstrated plenty of novel phenomena of manipulating free electron wave packet and detecting/shaping quantum photonic states. However, free electrons generally only absorb/emit one photon at a time, while the physical mechanism and phenomena of free electron-two-photon interaction have not been studied yet. Moreover, the relationship between PINEM and Kapitza-Dirac (KD) effect and nonlinear Compton scattering is still unclear. Here we develop the full quantum theory of electron-photon interaction considering the two-photon process. It is revealed that the emission/absorption of two photons by electrons can be greatly enhanced by manipulating the electric field component of optical near field, and the quantum interference between single-photon and two-photon processes can occur in some circumstances, which affects the photon number state, electron energy states and electron-photon entanglement. Meanwhile, it is found that the KD effect (elastic electron-photon scattering) and nonlinear Compton scattering (inelastic electron-photon scattering) are also a kind of two-photon process and the distribution of electrons can be deduced analytically based on the full quantum theory. Our work uncovers the possible abundant phenomena when free electron interacting with two photons, paves the way for more in-depth studies of nonlinear processes in electron-photon quantum interactions in the future.
Electron beams are a formidable tool for probing nanophotonic systems [1]. Combining electron microscopy with external optical excitation in ultrafast transmission electron microscopes has enabled the mapping of optical near-fields [2] and the bunching of electrons in attosecond pulses [3, 4]. These developments are based on the stimulated inelastic scattering between electrons and light [5, 6], in which the electrons gain energy from or lose energy to the optical field. Recently, the underlying interaction strength of this process has been increased significantly by harnessing resonant enhancement of the optical field and velocity phase matching [7]. Such an increased interaction strength also benefits the spontaneous scattering of electrons with light, thus promising applications like generating complex quantum states of light [8]. In this presentation, we discuss a set of experiments on free electron quantum optics that investigate single-electron-single-photon interactions and probe the resulting entanglement. Specifically, we consider scenarios in which optical waveguide structures are placed inside a transmission electron microscope (TEM) facilitating the interaction. Electrons passing by, for example, an integrated photonic structure (cf. Fig. 1a) can inelastically scatter with the optical mode, leading to the emergence of electron-photon pair states [9]. The resulting correlation between energy-loss electrons and photons, illustrated in Fig. 1b, can be probed employing time- and energy-resolved detection of both particles, revealing a pronounced coincidence peak between their arrival times, schematically shown in Fig. 1c. Extending the photon detection setup by a second detector to allow for Hanbury Brown and Twiss (HBT) measurements, the photon statistics heralded by such energy-loss electrons can be studied [10]. The observed anti-bunching behavior indicates a nonclassical optical state with single-photon properties. The inelastic electron-light scattering underlying the electron-photon pair generation is further expected to induce entanglement in the particle energies [11], however, direct observation of quantum entanglement would be exceedingly difficult given the large number of independent quantum states available in these degrees of freedom. Therefore, we propose experiments based on the quantum eraser scheme to demonstrate this free-electron-photon entanglement in different degrees of freedom [12,13]. Specifically, we consider a double-slit geometry coherently illuminated by an electron beam such that an interference pattern can be observed on a distant screen (cf. Fig. 2a). If electrons passing through the left or right (denoted |Land |R, respectively) slit generate distinct marker photons with vertical (|V)or horizontal (|H) polarization, this interference pattern would disappear due to the entanglement of electron path and photon polarisation (cf. Fig. 2b). However, if this which-path information carried by the marker photon is erased, e.g. by mixing the polarisation states, the interference pattern can be recovered when detecting electrons and photons in coincidence. We describe an extension of this idea to an entanglement test, before discussing possible realistic implementations and presenting preliminary results on several experimental key aspects. In summary, we discuss the inelastic electron-light scattering at integrated photonic structures with applications ranging from coherent electron beam modulation using continuous-wave optical fields to the electron-driven generation of quantum optical states of light. Delving deeper into single electron-single photon interactions, we outline feasible experiments to generate and verify electron-photon entanglement with a potential extension to electron pairs based on entanglement swapping. All this adds to the toolbox of free electron quantum optics, potentially enabling novel sources of quantum light as well as quantum-enhanced sensing in electron microscopy. Generation of correlated electron-photon pairs. (a) Electrons pass over a photonic integrated circuit placed in the sample plane of a TEM, generating photons in the optical waveguides via inelastic scattering. Energy-loss electrons are detected and time-tagged behind an imaging spectrometer in coincidence with photons exiting the waveguide. (b) Inelastic scattering links the electron energy loss (green, right ladder) to the generation of photons (red, left ladder), creating correlations in energy and time. (c) A strong temporal correlation between the loss electrons and detected photons, indicated by the red dot, is observed relative to the uncorrelated zero-loss background electrons (blue line). Free-electron-photon quantum eraser. (a) Coherent electron illumination of a double-slit structure results in interference between the two pathways |Land |R.(b) If the electrons generate distinguishable marker photons, e.g. of orthogonal polarizations |Vand |H, no interference pattern can be observed due to the electron-photon entanglement. (c) Collecting these marker photons and erasing the which-path information, e.g. using a half-wave plate (λ/2), the electron interference can be recovered using electron-photon coincidence detection with single-photon detectors (SPDs) placed behind a polarizing beam splitter (PBS).
Since the birth of quantum optics, the measurement of quantum states of nonclassical light has been of tremendous importance for advancement in the field. To date, conventional detectors such as photomultipliers, avalanche photodiodes, and superconducting nanowires, all rely at their core on linear excitation of bound electrons with light, posing fundamental restrictions on the detection. In contrast, the interaction of free electrons with light in the context of quantum optics is highly nonlinear and offers exciting possibilities. The first experiments that promoted this direction appeared over the past decade as part of photon-induced nearfield electron microscopy (PINEM), wherein free electrons are capable of high-order multi-photon absorption and emission. Here we propose using free electrons for quantum-optical detection of the complete quantum state of light. We show how the precise control of the electron before and after its interaction with quantum light enables to extract the photon statistics and implement full quantum state tomography using PINEM. This technique can reach sub-attosecond time resolutions, measure temporal coherence of any degree (e.g., g(1), g(2)), and simultaneously detect large numbers of photons with each electron. Importantly, the interaction of the electron with light is non-destructive, thereby leaving the photonic state (modified by the interaction) intact, which is conceptually different from conventional detectors. By using a pulse of multiple electrons, we envision how PINEM quantum detectors could achieve a single-shot measurement of the complete state of quantum light, even for non-reproducible emission events. Altogether, our work paves the way to novel kinds of photodetectors that utilize the ultrafast duration, high nonlinearity, and non-destructive nature of electron-light interactions.
Light is used to steer the motion of atoms in free space, enabling cooling and trapping of matter waves through ponderomotive forces and Doppler-mediated photon scattering. Likewise, light interaction with free electrons has recently emerged as a versatile approach to modulate the electron wave function for applications in ultrafast electron microscopy. Here, we combine these two worlds, theoretically demonstrating that matter waves can be optically manipulated via inelastic interactions with optical fields. This allows us to modulate the translational part of the wave function and produce temporally and spatially compressed atomic beam pulses. We realize such modulation through stimulated photon absorption and emission by atoms traversing phase-matching evanescent optical fields generated upon light scattering by a nanostructure and via stimulated Compton scattering in free space without any assistance from material media. Our results support optical manipulation of matter waves as a powerful tool for microscopy, spectroscopy, and exploration of fundamental phenomena associated with light-atom interactions.
Light is extensively used to steer the motion of atoms in free space, enabling cooling and trapping of matter waves through ponderomotive forces and Doppler-mediated photon scattering. Likewise, light interaction with free electrons has recently emerged as a versatile approach to modulate the electron wave function for applications in ultrafast electron microscopy. Here, we combine these two worlds by theoretically demonstrating that matter waves can be optically manipulated via inelastic interactions with optical fields, allowing us to modulate the translational wave function and produce temporally and spatially compressed atomic beam pulses. Specifically, we realize such modulation through stimulated photon absorption and emission by atoms traversing phase-matching evanescent optical fields generated upon light scattering by a nanostructure, but also via stimulated Compton scattering in free space without any assistance from material media. Our results support optical manipulation of matter waves as a powerful tool for microscopy, spectroscopy, and the exploration of novel fundamental phenomena associated with light-atom interactions.
Coherent optical modulation of free-electron wavepackets offers a route to ultrafast beam steering, energy exchange, temporal compression, and quantum-state shaping. Recent advances in photon-induced near-field electron microscopy (PINEM), ultrafast Kapitza-Dirac effect (KDE) and dielectric laser acceleration (DLA) have demonstrated strong light-electron coupling, but longitudinal energy modulation, transverse momentum transfer, and wavepacket-dependent diffraction are still commonly described with separate models. Here, we develop a unified Light-Electron Modulation (LEM) framework that treats optical near fields as programmable phase modulators for free-electron wavepackets. Within this framework, we identify longitudinal and transverse modulation channels, analogous to electro-optic phase modulation and acousto-optic diffraction of light, respectively, and show how their operation depends on wavepacket extent, recoil, phase matching, and optical-field geometry. This formulation organizes PINEM, Raman-Nath and Bragg diffraction, DLA-like acceleration, and anomalous PINEM as limiting regimes of a common modulation picture. The resulting framework provides design principles for free-electron modulators that can control energy spectra, temporal density, transverse wavefronts, and electron-photon quantum interfaces, establishing LEM as a device-level platform for programmable femtosecond-to-attosecond matter-wave control.
We present the possibility of spin-dependent Kapitza-Dirac scattering based on a two-photon interaction only. The interaction scheme is inspired from a Compton scattering process, for which we explicitly show the mathematical correspondence to the spin dynamics of an electron diffraction process in a standing light wave. The spin effect has the advantage that it already appears in a Bragg scattering setup with arbitrary low field amplitudes, for which we have estimated the diffraction count rate in a realistic experimental setup at available x-ray free-electron laser facilities.