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A universal mechanism of ultrafast two-electron orbital swap is discoveredthrough two-photon sequential double ionization of Li. After a $1s$ electron inLi is ionized by absorbing an EUV photon, the other two bound electrons locatedon two different shells have either parallel or antiparallel spin orientations.In the latter case, these two electrons are in the superposition of the singletand triplet states with different energies, forming a quantum beat and givingrise to the two-electron orbital swap with a period of several hundredattoseconds. The orbital swap mechanism can be used to manipulate the spinpolarization of photoelectron pairs by conceiving the attosecond-pumpattosecond-probe strategy, and thus serves as a knob to control spin-resolvedmultielectron ultrafast dynamics.

Ultrafast Two-electron Orbital Swap in Li Initiated by Attosecond pulses