We present new experimental results on second-harmonic generation in h
ighly conjugated organic molecules and molecular crystals recently dev
eloped in our group, as well as on electro-optic effects in thin-film
polymers. A large value of the molecular hyperpolarizability of a new
hydrazone-type molecule crystallizing in a noncentrosymmetric point gr
oup is reported. Large nonlinear optical coefficients of up to 840+/-2
00 pm/V were measured in crystals of 4'-dimethylamino-N-methyl-4-stilb
azolium tosylate (DAST). The new experimental results are compared wit
h theoretical calculations of limiting values of nonlinear optical coe
fficients. Computer modeling of crystal structures shows good agreemen
t with experimental results. Measurements on electro-optic polymers wi
th high thermal stability are presented.