Novel organometallic compounds (suitable for nonlinear optical applica
tions), consisting of oligothiophene substituted Fischer-type carbene
complexes, have been studied by using absorption, emission and Raman s
pectroscopies. The nature of the low-lying charge transfer transition
is investigated. It is established that the electrical dipole reverses
its direction upon photoexcitation from the ground to the first excit
ed state, thus accounting for the enhanced second-order nonlinear opti
cal response of this compound. The perturbation on the pi conjugated e
lectrons induced by the transition-metal atom is studied and discussed
. (C) 1998 Elsevier Science S.A.