While the results of the spin-PLDM approach in these ab initio test cases did not provide superior accuracy compared to SH, SQC, or spin-LSC methods, it is worthwhile to take a closer look at the spin-PLDM correlation function to better understand the approach, especially given that PLDM approach usually provides more accurate dynamics in system-bath models. Fig. presents the partial contributions P λλ to the total spin-PLDM correlation function C AB = λλ P λλ (Eq. 24) for all four molecular models explored in this work. The total spin-PLDM correlation function requires a summation of overall possible initially focused conditions {λ, λ } of the electronic mapping variables {Z, Z }, leading to N 2 initial conditions that need to be converged with respect to the number of trajectories (1000 ×F 2 = 4000 trajectories in this work).