The molecular geometries were optimized using Becke's three-parameter hybrid functional (B3LYP) and the atom-centered polarized triple-zeta basis set (def2-TZVP) with tight SCF convergence criteria. The def2/J auxiliary basis set was utilized for faster calculations. In the case of tellurium substituted diradical dication, relativistic effects were included via the ZORA Hamiltonian and ZORA-def2-TZVP basis set with the SARC/J auxiliary basis. The geometry optimizations were performed in both BS and triplet states. Frequency calculations were devoid of imaginary frequencies, confirming that the geometries obtained are local minima. The BS-DFT approach to determine 2J utilized a variety of functionals along with the def2-TZVP basis set and def2/J auxiliary basis. The spin-constrained BS-DFT (CBS-DFT) calculations were performed using the 6-311G* basis set. For multireference calculations, the state-averaged CASSCF (SA-CASSCF) method was employed with the resolution of identity (RI) approximation for improved performance. The BS-DFT and multirefence calculations presented here were performed in ORCA 5.0.3. The NWchem package was used for the CBS-DFT calculations. π orbital composition analysis was carried out using the the Multifwn package to understand the nature of the singly occupied orbitals in the diradical dications. The tertiary-butyl groups in the modeled diradical dication have been replaced with methyl groups for the benefit of reduced computational cost as seen in Fig. . This truncation has minimal influence on the magnetic exchange as can be seen from the ground state spin densities of tb 2 SH 2+•• and SH 2+•• calculated at WB97X-D3/def2-TZVP level, shown in Fig. and c respectively. It is observed that only negligible spin density is present in both tertiary-butyl and methyl groups which does not affect the magnetic exchange coupling between the radical centers. The 2J values computed using various functionals for the fully optimized