Attosecond Vortex Photoelectron Holography for Probing Phase-Encoded Chirality

Strong-field photoelectron holography (SFPH) is a powerful tool for retrieving the phase of photoelectron wave packets, offering insights into the intrinsic atomic/molecular structure and ultrafast dynamics. Here, we generalize the SFPH theory, conventionally applied to plane-phase electron wave packets, to vortex electrons. By employing a synthetic chiral atomic model with helical orbitals, we demonstrated that photoelectron holography maps the helicity of the bound states to the interference fringes and resolves enantio-sensitive phase shifts, providing direct access to the chiral information encoded in the phase of the photoelectrons. Our approach establishes a phase-sensitive diagnostic of chirality, complementary to the amplitude-based chiral spectroscopies. The intrinsic attosecond temporal resolution of SFPH further enables the measurement of ultrafast chiral electron dynamics.