Abstract: The two D-π-A dyad compounds (6a, 7a) were prepared from monopyrrolotetrathiafulvalenes (1) via Vilsmeier formylation and Wittig reaction or cross-coupling reaction . For comparison with 6a and 7a, the N-methylated two D-π-A dyad compounds (6b, 7b) were also obtained from mono-pyrroletetrathiafulvalene(2) using the same process. Their electrochemical and photophysical properties were studied with cyclic voltammetry and UV-VIS spectrum, and theoretical calculation were carried out for their nonlinear optical properties.

Key words: theoretical studies, nonlinear optics, pyrrolotetrathiafulvalene, electrochemistry