Two new two-dimensional charge transfer (2DCT) chromophore molecules for nonlinear optics (NLO) were designed and synthesized with pyridinium as electron acceptor gorup. They are tranes -4,4-di[p-[N- ethyl-N-hydroxyethyl) amino] styry}-N,N'-(1,2-ethylene)-2,2'- bipyridinium ditetraphenylborate and trans-N-hexyl- carbazole-3,6-di(p- ethenyl-N-hydroxyethyl-pyridinium) dietrapenylborate. The first hyperpolarizability(β) values were determined by Hyper-Rayleigh Scattering (HRS) techique.The large βvalues are obtained as 786x10^- ^3^0esu and 1770x10^-^3^0esu at 1064 nm and corresponding β0 are 215x10^-^3^0esu and 119x10^-^3^0esu calculated according to two-level model, respectively. The large value of βwas explained qualitatively from the point of view of molecular structure.

Key words: PYRIDINE P, CHARGE TRANSFER, MOLECULAR DESIGN, POLARIZABILITIES, NON LINEAR OPTICS