A gauge-origin invariant formulation of the frequency-dependent Verdet cons
tant V(omega) of magneto-optical rotation and of the Faraday B term of magn
etic circular dichroism for coupled-cluster wave functions is derived withi
n the framework of variational response theory. Working expressions suitabl
e for implementation in ab initio program packages are presented. These exp
ressions have a structure similar to that of the expressions for the first
hyperpolarizability and the two-photon transition moment, respectively, for
the Verdet constant and the B term. The approach is general and can easily
be extended to other similar frequency-dependent properties as well as to
other wavefunction models. Pilot results at the CCSD level are presented fo
r V(omega) of HF and H-2. (C) 2000 American Institute of Physics. [S0021-96
06(00)30233-1].