Gaussian-based Self Consistent Field (SCF) MOs are obtained at various nuclear geometries for the MnS4 cluster in the external potential of cubic ZnS. Electronic relaxation and d-shell electron correlation effects are then included. For Td symmetry, quartet d-d excitation energies calculated as functions of R(Mn-S) qualitatively resemble the simple CF diagram. While separations between successive quartet levels agree closely with experiment, the threshold is about 0.5 eV high; much of this discrepancy is removed by including additional correlation effects from charge-transfer states. Large Jahn-Teller (JT) splittings of 4T1 and 4T2 levels are found with D2d distortion. Difficulty in accurately evaluating force constants interferes with predicting the corresponding deformations and stabilization energies. Estimates, encorporating the observed Stokes'; shift and JT stabilization energy, are that R(Mn-S) decreases by ∼0.1 Å and the S-Mn-S dihedral angle increases by 7sim;8°, in the lowest quartet level.