We present several new materials made of acceptor units (TCNQ and [Ni(dmit)
(2)]) and stilbazolium-based chromophores for second-order optical nonlinea
rity. The subtil adjustement in the redox potentials necessary for: (i) mai
ntaining the material in a semi-conducting state, to offer a good range of
transparency in a broad near-infrared domain; (ii) allowing electronic inte
raction, to promote a pathway towards efficient interplays between the prop
erties is analyzed The possibility of combining both properties on the same
entity with the TTF skeleton is also discussed.