As an extension of our first article of this series (J. Chem. Phys. 97 (1992) 5316), in which we reported data of the induced dipole moment differences Δμ i n d of nonpolar dyes in polymeric matrices, we present results which were obtained with polar optical probe molecules, namely, chlorin and naphthazarin. We used the technique of persistent spectral hole burning to investigate both the frequency dependence of the permanent dipole moment differences Δμ p e r of polar dyes, and the correlation of the dipole moment differences measured in the absorption maximum, (Δμ p e r a b s m a x ), with the low-temperature dielectric constant ε H e . In contrast to the difference Δμ i n d of the induced dipole moments of centrosymmetric molecules, the difference Δμ p e r of the permanent dipole moments of polar dyes does not increase from higher to lower optical frequencies but is constant or decreases with decreasing frequency in matrices which are nonpolar or only moderately polar. The (Δμ p e r a b s m a x ) values exhibit a linear dependence on the low-temperature dielectric constant, which is similar to the behavior found for centrosymmetric molecules. This linear dependence allows the separation of the matrix-induced contribution to the Δμ p e r values and the molecular Δμ m o l values. Implications of the dependences of Δμ on the absorption frequency and on the dielectric constant of the matrix are discussed.