Compared to TDDFT, similar results are also being obtained when computing ∆E LFS using the multi-reference methods CASSCF and CASPT2, see Figure (c), with ∆E LFS of the four designed complexes being larger than that of VCl 3 (ddpd). In particular, ∆E LFS values computed using CASPT2 are similar to the TDDFT excitation energies, suggesting that TDDFT can in fact be used to estimate ∆E LFS in these type of vanadium(III) complexes. In the CASPT2 calculations, we tested both using an IPEA-shift correction as well as using the non-shifted variant (denoted NOIPEA) which resulted only in minor differences of < 0.04 eV. Compared to CASPT2, CASSCF predicts ∆E LFS values that are systematically smaller by 0.2-0.3 eV. While both TDDFT and the CASPT2 variants predict larger ∆E LFS values of the four discussed complexes, their order changes between TDDFT and CASPT2. In particular, CASPT2 predicts the largest ∆E LFS for [VCl 3 (im-ph-im)] -closely followed by the carbene-bearing VCl 3 (im-im-im) and VCl 3 (bi-bi-bi) complexes, while TDDFT predicts the largest ∆E LFS for [VCl 3 (py-ph-py)] -. As both CASSCF/CASPT2 and TDDFT predict larger ∆E LFS for the four complexes 4, 11, 12, and 18, we decided to perform nonadiabatic dynamics simulations for each of them. These simulations will be discussed in the next section. This section concludes with a general discussion of our design strategies based on our TDDFT results.