Breakdown of one-to-one correspondence between the photoelectron emission angle and the tunneling instant in the attoclock scheme

Abstract

Attoclock is a promising chronoscopy of the ultrafast dynamics of atoms and molecules in intense laser fields. The attoclock procedure is established based on the one-to-one correspondence between the photoelectron emission angle and the tunneling instant at each photoelectron kinetic energy for ionization of atoms and molecules subject to elliptically polarized strong laser fields. In this work, our joint theoretical and experimental study demonstrates that this correspondence could be broken down for photoelectrons emitted in a direction close to the minimum yield. Two trajectories with different tunneling instants and different initial velocities are found to correspond to a specific final momentum of the photoelectron in this direction, and a multi-peak structure appears in the photoelectron kinetic energy spectrum that can be attributed to interference between these two trajectories. Our work is essential for a deeper understanding and further development of the attoclock scheme.