Intrinsic vibrational coherence in face-centered cubic supra-crystals of silver nanocrystals: Raman scattering measurements

The ordering of silver nanocrystals is tuned from amorphous aggregates to highly well-ordered, face-centered cubic supra-crystals, using various substrates and controlling their temperature to obtain this. Low-frequency Raman scattering, for the first time, demonstrates vibrational coherence in fcc supra-crystals of nanocrystals. This is shown by a narrowing of the peak corresponding to the quadrupolar modes of the nanocrystals. However, this is obtained when the supra-crystals are smaller than the excitation wavelength. When the supra-crystals are larger, the narrowing cannot be observed. Furthermore, for any size of the supra-crystals, a shift to low frequency of the Raman peak due to the Lorentz field effect is seen.