The prediction of the 2J value for SH 2+•• using DFT results in inconsistent magnitudes due to various errors like spurious spin delocalization, excess spin contamination, and improper description of the singlet. The CBS-DFT method was used to mitigate the excess spin delocalization by constraining the spin densities to the sulfur-doped rings, resulting in more accurate estimates of the 2J. The SF-TDDFT method on the other hand was not able to improve upon the BS-DFT results for the B3LYP and WB97X-D3 functionals but showed improvement for the functionals with a higher percentage of HF exchange. The functional dependence of computed 2J values still persists even in CBS-DFT and SF-TDDFT methods, highlighting one of the flaws of DFT. The CASSCF+NEVPT2 method was used to obtain a value of magnetic exchange coupling that is consistent with experimental results. To overcome the challenge of choosing the correct active space, a method of active-space scanning, relying on the difference between CASSCF and CASSCF+NEVPT2 results was devised and successfully utilized to find the active space of all the modeled diradical dications. The nature of the coupling between radical centers in dichalcogenide diradical dications is dependent on the nature of the chalcogen atom. The heavier chalcogen atoms have a larger covalent radius, giving rise to significant distortion to the molecular geometry and a subsequent reduction