The solution third-order non-linear optical susceptibility chi(3) values, measured by laser self-trapping at 514.5 nm for chloroform solutions of bis(dicyanovinyl)thiophene 4 (2.9 x 10(-7) esu), bis- (dicyanovinyl)dithienyl 5 (1.1 x 10(-4) esu), bis(dicyanovinyl)trithienyl 6 (1.1 x 10(-5) esu), values are affected by resonance and solution heating effects. Chi(3) (-omega; omega, omega, -omega) was measured by degenerate four-wave mixing at 1064 nm for chloroform (C) and pyridine (P) solutions of dicyanovinylthiophene 1, dicyanovinyldithienyl 2, dicyanovinylterthienyl 3, and bis(dicyanovinyl)thiophene 4. The molecular second-order hyperpolarizabilities are gamma/esu = 8.7 x 10(-33) (1, C), -6.3 X 10(-33) (1, P), 2.2 x 10(-33) (2, C), 3.7 x 10(-31) (3,C), 6.1 X 10(-32) esu (3, P), 2.8 x 10(-31) (4, P).