  Raman scattering experiments on CdCr2S4 single crystals show pronounced
anomalies in intensity and frequency of optical phonon modes with an onset
temperature T*=130 K that coincides with the regime of giant magnetocapacitive
effects. A loss of inversion symmetry and Cr off-centering are deduced from the
observation of longitudinal optical and formerly infrared active modes for
T<T_c=84 K. The intensity anomalies are attributed to the enhanced electronic
polarizability of displacements that modulate the Cr-S distance and respective
hybridization. Photo doping leads to an annihilation of the symmetry reduction.
Our scenario of multiferroic effects is based on the near degeneracy of polar
and nonpolar modes and the additional low energy scale due to hybridization.
