We have observed the characteristic temperature dependence of the intermolecular phonon spectrum in the organic dimer Mott insulator kappa-(ET)2Cu2(CN)3 exhibiting a dielectric anomaly at 30 K. The anomalous spectral narrowing of the 55 cm-1 phonon peak at 30 K was analyzed in terms of motional narrowing within the framework of a stationary Gaussian process, i. e., the phonon frequency is modulated by the ultrafast charge fluctuation. The spectral narrowing occurs because the time constant of the correlation time tau_c and the amplitude of the frequency modulation delta satisfy the relation tau_c<delta at 30 K. At temperatures below 30 K, the motional narrowing is disturbed by the increasing of tau_c, near the charge-glass or the short-range order at 6 K. On the other hand, for temperatures above 30 K, the motional narrowing is disturbed by the increase of delta with increasing temperature.
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