  We present a computational investigation of the intramolecular exchange
coupling in [LnPc$_2$]$^0$ (Ln = Tb, Dy, Ho, and Er) between the Ln$^{3+}$ 4f
electrons and the spin-1/2 radical on the phthalocyanine ligands. A series of
ab initio multi-configurational/multi-reference Complete/Restricted Active
Space Self-Consistent-Field calculations (CASSCF/RASSCF), including
non-perturbative spin--orbit coupling, were performed on [LnPc$_2$]$^0$ and on
the smaller model compound [LnPz$_2$]$^0$. We find that the exchange coupling
mechanisms are restricted by symmetry, but also dependent on the spin
polarization effect triggered by the Pc$_2$ ligands $\pi$--$\pi^*$ excitations.
The calculated exchange splittings are small, amounting to at most a few
cm$^{-1}$, in disagreement with previous literature reports of strong
antiferromagnetic coupling, but in good agreement with recent EPR experiments
on [TbPc$_2$]$^0$. Furthermore, the coupling strength is found to decrease from
[TbPc$_2$]$^0$ to [ErPc$_2$]$^0$, with decreasing number of unpaired electron
spins in the lanthanide ground (Hund's rule) Russell--Saunders term.
