In this work, we leverage the efficiency of the SH/LVC approach to screen the photodynamics of vanadium(III) complexes for their potential use as near-infrared emitters. By using strongfield ligands such as N,N'-dimethyl-N,N'-dipyridine-2-ylpyridine-2,6-diamine (ddpd), vanadium(III) complexes become emissive in the near-infrared region. This makes them rare examples of early 3d transition-metal complex luminophores 40 that due to their Earth-abundance are designed to become sustainable replacements for currently used near-infrared emitter based on expensive noble metals and rare earth elements. We have previously studied the photodynamics of the emissive VCl 3 (ddpd) complex using SH and LVC potentials. When excited from its triplet ground-state, the complex undergoes intersystem crossing to the singlet states which are long-lived and emit in the near-infrared region at 1111 and 1219 nm, see Figure . Our simulations revealed the mechanism behind the population of the singlet states as well as of the competing nonradiative relaxation pathways back to the triple ground state. The character of the electronic states suggested that the relaxation mechanism can be modified to increase the population in the singlet states and thus lead to larger phosphorescence quantum yields by designing ligands that induce even larger ligand-field splitting in the complex. To do this, we have modified the ligand-structure in VCl 3 (ddpd) following rules established for other 3d-complexes. We first screened their excited-state energies using different electronic structure methods, and then performed SH/LVC dynamics simulations to test our hypothesis for the four most promising complexes. Our simulations show two complexes with similar or larger singlet populations that suggest increased phosphorescence yields.