We report the experimental observation of intrinsic dynamically localized v
ibrational states in crystals of the highly nonlinear halide-bridged mixed-
valence transition metal complex {[Pt(en)(2)] [Pt(en)(2)Cl-2] (ClO4)(4)}, w
here en = ethylenediamine. These states are identified by the distinctive s
tructure and strong redshifts they impose upon the overtone resonance Raman
spectra. Quantitative modeling of the observed redshifts is presented base
d on a nonadiabatic coupled electron-lattice model that self-consistently p
redicts strong nonlinearity and highly localized multiquanta bound states.
[S0031-9007(99)08915-2].