Ultrafast generation and control of an electron vortex beam via chiral plasmonic near fields

Imparting orbital angular momentum (OAM) to particle beams opens unique opportunities for applications and exploration of fundamental science. Electron beams carrying OAM are commonly achieved via passive phase masks that imprint a transverse modulation on the particle wave function. Here, we show that a chiral plasmonic near field can be used to generate an OAM-carrying electron beam and dynamically control its vorticity. By monitoring the phase change of the transverse electron wave function in both real space and reciprocal space using ultrafast transmission electron microscopy, we demonstrate that an optically-excited chiral near-field with azimuthal order m = 1 is able to imprint an azimuthally varying 2πℓm phase shift on the electron wave function, where ℓ is the number of exchanged plasmons. In contrast to other passive monolithic methods, our approach enables a dynamic coherent control over the vortex beam properties with attosecond precision. This is achieved by properly modifying the optical field distribution using a sequence of two phase-locked light pulses with independent polarization states and delayed by fractions of their optical cycles. We discuss the potential extension of our method to composite charged particles to yield insights into their inner structure, with particular attention to the proton and the origin of its spin.