In this paper we present ab initio calculations for the evaluation of molec
ular hyperpolarizabilities of symmetric cyanine molecules. The influence on
the electronic properties of the presence of a counterion is discussed tak
ing into account the relative position of the molecule and the counterion i
tself. Use is made of the vibrational method to determine the vibrational c
ontribution to molecular hyperpolarizabilities. (C) 2001 Elsevier Science B
.V. All rights reserved.