Atomic motion dynamics during structural changes or chemical reactions have been visualized by pico- and femtosecond pulsed electron beams via ultrafast electron diffraction and microscopy. Imaging the even faster dynamics of electrons in atoms, molecules, and solids requires electron pulses with subfemtosecond durations. We demonstrate here the all-optical generation of trains of attosecond free-electron pulses. The concept is based on the periodic energy modulation of a pulsed electron beam via an inelastic interaction, with the ponderomotive potential of an optical traveling wave generated by two femtosecond laser pulses at different frequencies in vacuum. The subsequent dispersive propagation leads to a compression of the electrons and the formation of ultrashort pulses. The longitudinal phase space evolution of the electrons after compression is mapped by a second phase-locked interaction. The comparison of measured and calculated spectrograms reveals the attosecond temporal structure of the compressed electron pulse trains with individual pulse durations of less than 300 as. This technique can be utilized for tailoring and initial characterization of suboptical-cycle free-electron pulses at high repetition rates for stroboscopic time-resolved experiments with subfemtosecond time resolution.

The temporal resolution of ultrafast electron diffraction and microscopy experiments is currently limited by the available experimental techniques for the generation and characterization of electron bunches with single femtosecond or attosecond durations. Here, we present proof of principle experiments of an optical gating concept for free electrons via direct time-domain visualization of the sub-optical cycle energy and transverse momentum structure imprinted on the electron beam. We demonstrate a temporal resolution of 1.2±0.3 fs. The scheme is based on the synchronous interaction between electrons and the near-field mode of a dielectric nano-grating excited by a femtosecond laser pulse with an optical period duration of 6.5 fs. The sub-optical cycle resolution demonstrated here is promising for use in laser-driven streak cameras for attosecond temporal characterization of bunched particle beams as well as time-resolved experiments with free-electron beams.

We report on a theoretical and experimental study of the energy transfer between an optical evanescent wave, propagating in vacuum along the planar boundary of a dielectric material, and a beam of sub-relativistic electrons. The evanescent wave is excited via total internal reflection in the dielectric by an infrared (λ = 2 μm) femtosecond laser pulse. By matching the electron propagation velocity to the phase velocity of the evanescent wave, energy modulation of the electron beam is achieved. A maximum energy gain of 800 eV is observed, corresponding to the absorption of more than 1000 photons by one electron. The maximum observed acceleration gradient is 19 ± 2 MeV/m. The striking advantage of this scheme is that a structuring of the acceleration element’s surface is not required, enabling the use of materials with high laser damage thresholds that are difficult to nano-structure, such as SiC, Al₂O₃ or CaF₂.

We experimentally demonstrate several physical concepts necessary for the future development of dielectric laser accelerators—photonic elements that utilize the inelastic interaction between electrons and the optical near fields of laser-illuminated periodic nanostructures. To build a fully photonic accelerator, concatenation of elements, large energy gains, and beam steering elements are required. Staged acceleration is shown using two spatio-temporally separated interaction regions. Further, a chirped silicon grating is used to overcome the velocity dephasing of subrelativistic electrons with respect to its optical near fields, and last, a parabolic grating geometry serves for focusing of the electron beam.

In this paper, we describe an ultrafast scanning electron microscope setup developed for the research of inelastic scattering of electrons at optical near-fields of periodic dielectric nanostructures. Electron emission from the Schottky cathode is controlled by ultraviolet femtosecond laser pulses. The electron pulse duration at the interaction site is characterized via cross-correlation of the electrons with an infrared laser pulse that excites a synchronous periodic near-field on the surface of a silicon nanostructure. The lower limit of 410 fs is found in the regime of a single electron per pulse. The role of pulse broadening due to Coulomb interaction in multielectron pulses is investigated. The setup is used to demonstrate an increase in the interaction distance between the electrons and the optical near-fields by introducing a pulse-front-tilt to the infrared laser beam. Furthermore, we show the dependence of the final electron spectra on the resonance condition between the phase velocity of the optical near-field and the electron propagation velocity. The resonance is controlled by adjusting the initial electron energy/velocity and by introducing a linear chirp to the structure period allowing the increase of the final electron energy gain up to a demonstrated value of 3.8 keV.