In this paper, we report the measurements of the third-order susceptibiliti
es of new dithienylethylenes in solutions using the degenerate four-wave mi
xing technique at lambda =532 nm in the picosecond regime. From these measu
rements we deduced the second-order hyperpolarizabilities gamma values, whi
ch are about 10(3) larger than the gamma value of CS2 and are comparable wi
th the corresponding values for the new synthesized diphenylpolyene derivat
ives. We also determined the optical power limiting properties of the menti
oned compounds using nanosecond laser pulses in the visible range. The disp
ersion of nonlinear absorption coefficients is obtained in the framework of
Gaussian collimated beam propagation in sample. Kerr ellipsometry measurem
ents are responsible for the excited absorption cross section and are spect
rally shifted comparing with the optical limiting processes (up to 50 nm).
The appropriate quantum chemical calculations are done. The contributions o
f electronic and vibration subsystems as well as contribution of the partic
ular parts of each molecule into the output third nonlinear optical respons
e are given. (C) 2001 American Institute of Physics.