The quadrupole channel of two-photon double ionization of He exhibits two distinctly different modes of correlated motion of the photoelectron pair. The kinematics of the mode associated with the center-of-mass motion favors large total momenta maximized at parallel emission where the interelectron repulsion is strong. In contrast, the mode associated with the relative motion favors large relative momenta maximized at antiparallel emission where the interelectron repulsion is relatively weak. This difference in the interelectron repulsion allows for much wider angular correlation width in the relative motion mode as compared to the center-of-mass mode.
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