[en] Cross sections for single-electron transfer forming the metastable state ⁴He⁺(2s) have been measured for a ⁴He⁺⁺ beam incident on thin He, Ar, H₂, and N₂ gas targets. The ⁴He⁺⁺ energy range was 7--70 keV. The experiments utilized detection of the 2s state via a delayed time coincidence between a field-induced Lyman-α photon and the ion itself. While the measured cross sections are believed accurate to plus-or-minus 35%, they are three times larger than the recent cross sections of Shah and Gilbody using incident ³He⁺⁺ ions. The present time-coincidence technique directly measured the fraction of the total electron-transfer cross section resulting in metastable production with results ranging between 5% and 17%