A sharplike modulation of the linear electrooptic (LEO) coefficient with pr
essure (p) and temperature (T) has been observed for the first time. The mo
dulation depth of the LEO (r(222)) tenser component in the C-60-TTF (for th
e He-Ne laser, lambda = 633 nm) was equal to about 2.6%. By varying the app
lied hydrostatic pressure to up to 15 GPa and the temperature from 4.2 to 2
5 K, we have unambiguously demonstrated that the observed effect is caused
by the incorporation of the TTF moiety. This effect is absent from the unsu
bstituted fullerenes when the applied hydrostatic pressure is increased to
19 GPa and the temperature varied from 4.2 to 150 K. Norm-conserving self-c
onsistent pseudopotential and molecular dynamics simulations independently
reproduce these modulations and attribute them to the electron-vibration in
teractions associated with the LEO coefficients. The contribution of the in
terconformational tunneling under the applied pressure and temperature is d
emonstrated. The data obtained give a possibility for using the discovered
effect for contactless measurements of low temperatures and high pressures.