We have measured the relative probability of excited state ͓Li 0 (2p)͔ formation versus the work-function change induced by alkali-metal adsorbates when hyperthermal energy Li ϩ ions are incident on alkali-metalcovered Cu͑001͒. This probability is broadly peaked as the work function decreases, and decreases by approximately an order of magnitude when the velocity of the ions in the incident beam is decreased from 1.05ϫ10 5 to 0.52ϫ10 5 m s Ϫ1 , and the incident angle is i ϭ65°as measured from the surface normal. Theoretical calculations based on a many-body solution to the time-dependent Anderson-Newns model of charge transfer ͑discussed in the preceding paper͒ qualitatively reproduce the observed trends. These calculations suggest that the peak in the excited-state probability results mainly from two effects: first, the decreasing difference between the energy of the Li 0 (2p) state and the Fermi level as the work function decreases, which tends to increase the excited-state probability; and second, the competition of the Li 0 (2p) state with the Li Ϫ (2s 2 ) negative ion state at low work functions, which tends to decrease the excited-state probability. Differences between the Li 0 (2s) and Li 0 (2p) lifetimes also play a role in the formation of the peak, as does electron-hole pair production.