We report the observation of giant quantum coherence effects in the localiz
ed modes of ionized hydrogen in synthetic fluorite. Infrared free induction
decay experiments on the substitutional H+ center thew dramatic modulation
s at negative delay times due to interference between multiple vibrational
levels. Spectrally resolving the degenerate four wave mixing signal allows
unambiguous assignments of the participating vibrational states. The depend
ence of the signal intensity upon the delay path between the exciting free
electron laser pulses can be accounted for in terms of the resonant third o
rder polarization with a common dephasing rime for the excited states.