ULTRAFAST DYNAMICS OF SMALL CLUSTERS ON THE TIME-SCALE OF NUCLEAR MOTION

We present a theoretical study of the multistate dynamics of the Ag-3( -)/Ag-3/Ag-3(+) system on the time scale of nuclear motion, as explore d by femtosecond pump-probe negative ion-to neutral-to positive ion (N ENEPO) spectroscopy. The dynamics of the Ag-3 cluster initiated from i ts linear transition state involves configurational relaxation, intrac luster collision, and onset of IVR, resonant and dissipative IVR and v ibrational equilibration, whose time scales were determined. Our analy sis reveals that theory is essential for the elucidation of the rich d ynamic information regarding geometrical change, completion of IVR, an d vibrational coherence effects in the NENEPO femtosecond signals.