Nonlinear Polarizabilities of Donor-Acceptor Substituted Conjugated Polyenes

The polarizabilities of conjugated polyenes with 8−36 carbon atoms are calculated using the time dependent Hartree−Fock (TDHF) technique. By examining the reduced single-electron density matrix, we explore the relations among the ground state chemical bonding structure and off-resonant and resonant susceptibilities. The effects of a donor−acceptor substitution on oligomers of different sizes are investigated.