Controlled interaction of laser light with electron beams is fundamental for ultrafast electron microscopy and electron-based quantum optics, yet their direct coupling is forbidden in free space. Here we use longitudinally polarized light at a thin membrane and show that the emerging focal fields can modulate the electron beam in a direct, coherent and linear way, without the need for nanostructured materials or slanted interaction geometries. Also, we use vectorial polarizations to excite and probe three-dimensional nanophotonic near-fields in metallic mesocrystals by coherent electron energy gain and loss. We find that longitudinal electric fields excite axial near-fields in a direct way while longitudinal magnetic fields excite oscillating ring currents via azimuthal electric fields. These possibilities enable tilt-free, collinear generation of attosecond electron pulses or free-electron qubits and provide novel imaging modes in ultrafast electron microscopy and metamaterial tomography.
Controlled interaction of laser light with electron beams is fundamental for ultrafast electron microscopy and electron-based quantum optics, yet their direct coupling is forbidden in free space. Here we use longitudinally polarized light at a thin membrane and show that the emerging focal fields can modulate the electron beam in a direct, coherent and linear way, without the need for nanostructured materials or slanted interaction geometries. Also, we use vectorial polarizations to excite and probe three-dimensional nanophotonic near-fields in metallic mesocrystals by coherent electron energy gain and loss. We find that longitudinal electric fields excite axial near-fields in a direct way while longitudinal magnetic fields excite oscillating ring currents via azimuthal electric fields. These possibilities enable tilt-free, collinear generation of attosecond electron pulses or free-electron qubits and provide novel imaging modes in ultrafast electron microscopy and metamaterial tomography.
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.
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.
Electron beams are an exceptional tool for probing nanophotonic systems [1]. Combining electron microscopy with external optical excitation in ultrafast transmission electron microscopes has enabled nanoscale [2,3] and attosecond phase-resolved mapping of optical near-fields [4] by stimulated inelastic scattering between electrons and light. Recently, the underlying interaction strength of this process has been increased significantly by harnessing resonant enhancement of the optical field and velocity phase matching [5]. Such an increased interaction strength also benefits the spontaneous scattering of electrons with light, thus promoting single-particle-based scattering experiments [6]. Here, we demonstrate the generation of nonclassical multiphoton states via coherent cathodoluminescence (CL) from an optical waveguide, approaching near-unity coupling in electron spectroscopy of nanophotonic systems [7]. To this end, we scatter swift electrons at the optical mode of a custom silicon nitride photonic chip. Specifically, inside of a transmission electron microscope, a beam of free electrons (100-keV kinetic energy) passes parallel to the waveguide surface in an aloof geometry (cf. Fig. 1a). The electrons can inelastically scatter with the evanescent tail of the guided optical mode, generating photons at a wavelength around 1400 nm in the fundamental quasi-TM mode, while the electrons lose multiples N of the corresponding photon energy of 0.88 eV (cf. Fig. 1b). The photons are then coupled via optical fibers to a balanced beam splitter and two single-photon avalanche diodes (SPADs), implementing a Hanbury Brown and Twiss (HBT) setup (cf. Fig. 1c). Probing the ensemble average using the 2nd-order correlation function g(2), we observe Poissonian photon statistics in accordance with the underlying coherent scattering mechanism (Fig. 1d, top). A parallel single-particle-resolved measurement using an event-based electron camera (Timepix3 ASIC) coupled to an EEL spectrometer provides information on both electron energy and arrival time. This allows us to further investigate the photon statistics of the generated light as a function of the electron energy. Using this electron-heralded HBT setup, we verify the generation of single photons following an energy loss of E = ℏω (Fig. 1d, bot), and photon pairs for double scattering events. Characterizing the electron-driven photon generation using established metrics for heralded single-photon sources, such as spontaneous parametric down-conversion (SPDC), we find an intrinsic single-photon heralding efficiency of 10% and a coincidence-to-accidental ratio > 30. This establishes a new source for electron-heralded quantum light, which may find its applications in quantum photonics. Practically, efficient electron-photon coupling and event-based detention, offers a new pathway for coincidence-enhanced electron spectroscopy of photonic materials [8]. Besides eliminating undesired and formerly unrecoverable averaging, access to the full scattering distribution of the involved particles can strongly suppress noise in ultrafast electron experiments [6]. Furthermore, for systems that can be directly pumped by single electrons, ultrafast dynamics can be studied using continuous electron beams, achieving sub-nanosecond resolution, only limited by the employed detector technology. Finally, this work represent an essential step toward quantum-enhanced electron imaging and enables the heralding of individual electrons for dose-sensitive applications. a) Electrons are scattered at an extended waveguide, generating light by coherent cathodoluminescence. b) Electron energy loss into discrete sidebands is observed, spaced by the photon energy ℏω. c) Event-based coincidence spectroscopy enables electron-heralded detection of photon number states. d) The discrete 2nd-order correlation function g(2)[q] shows Poissonian statistics for unheralded photon detection, while conditioning on an ℏω energy loss produces high-contrast single-photon states.
Light is routinely used to steer the motion of atoms in free space, enabling cooling and trapping of matter waves through ponderomotive interaction and Doppler-mediated photon scattering. In parallel, optical interaction with free electrons has recently emerged as a powerful way 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 by inelastic interaction with optical fields, allowing us to modulate the translational wave function and produce temporally and spatially compressed atomic beam pulses.
The coherent interaction between free electrons and optical near-fields enables the active modulation of electron wave packets, a mechanism central to photon-induced near-field electron microscopy (PINEM). While existing theories effectively describe these interactions at high kinetic energies, the growing interest in low-energy ultrafast electron microscopy demands frameworks that explicitly account for finite wave packet geometries and recoil effects. In this paper, we develop a rigorous 3D quantum scattering theory for electron wave packets interacting with time-periodic potentials, capturing the case of optical near-field interaction. By mapping the time-dependent dynamics into an extended Floquet space, we formally connect the modulation process to time-independent multi-channel scattering. We evaluate the resulting scattering amplitudes using both an exact R-matrix approach and a multi-channel eikonal approximation. The latter analytical approach recovers PINEM-like probabilities weighted by the wave packet's transverse profile. Application of the theory to an oscillating potential demonstrates the generation of distinct energy sidebands, revealing that the modulation strength is sensitive to the transverse focusing of the incident electron pulse, underlining the importance of a fully 3D treatment.