Abstract
We report the experimental observation of intrinsic dynamically localized vibrational states in crystals of the highly nonlinear halide-bridged mixed-valence transition metal complex ${[\mathrm{Pt}(\mathrm{en}{)}_{2}][\mathrm{Pt}(\mathrm{en}{)}_{2}{\mathrm{Cl}}_{2}]({\mathrm{ClO}}_{4}{)}_{4}}$, where $\mathrm{en}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}\mathrm{ethylenediamine}$. These states are identified by the distinctive structure and strong redshifts they impose upon the overtone resonance Raman spectra. Quantitative modeling of the observed redshifts is presented based on a nonadiabatic coupled electron-lattice model that self-consistently predicts strong nonlinearity and highly localized multiquanta bound states.
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