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We demonstrate the simultaneous production of spin-polarized ions/electrons using two-color, two-photon ionization of laser-ablated metallic atoms. Specifically, we have applied the developed technique to laser-ablated Sr atoms, and found that the electron-spin polarization of Sr ϩ ions, and accordingly, the spin polarization of photoelectrons is 64%Ϯ9%, which is in good agreement with the theoretical prediction we have recently reported ͓T. Nakajima and N. Yonekura, J. Chem. Phys. 117, 2112doi:10.1063/1.1610800 fatcat:2rtiuii4ivawbbb5vw4kpqu5am