R. Zadoyan et al., LATTICE-DYNAMICS FROM THE EYES OF THE CHROMOPHORE - REAL-TIME STUDIESOF I-2 ISOLATED IN RARE-GAS MATRICES, Faraday discussions, (108), 1997, pp. 255-269
Molecular iodine isolated in rare gas solids is used as a model system
to develop the framework for interpretation of condensed phase pump-p
robe observables, specializing in information content regarding multi-
body dynamics. The principles are illustrated through a series of exam
ples, where, beside the molecular vibronic coherence, the cage motions
can be directly dissected. The large variety of behaviors which can b
e staged in this system include: elastic cage recoil, highly non-linea
r and dissipative cage response, long-lived cage coherence driven thro
ugh guest-host resonances, nearly decoupled guest-host dynamics, and c
age induced dynamical solvation of electronic surfaces. Although the u
nderlying dynamics can be understood in great depth when aided by simu
lations, we attempt a clear distinction between direct experimental ob
servables and inferences based on simulations.