An instability of the MnO4- molecular ion in KI is reported that occur
s under intense resonant excitation in the 1A1 to 1T2 optical transiti
on of the impurity. The intensities of the resonantly excited vibratio
nal Raman lines and the absorption strength are used to monitor the ti
me dependence of this effect which is investigated for different tempe
ratures and excitation powers. A physical model is discussed that invo
lves ionization of the molecular ion and qualitatively accounts for th
e experimental observations.