In this work, we simulated 151 trajectories for each of the studied systems, whereas only 76 trajectories per system were simulated in our previous work on the ππ * -initiated dynamics (except for tetramer 5.5 Å, for which additional 75 trajectories were run in ref. 47 to check the effect of enlargement of the ensemble on the quantum yield). In Tab. First of all, comparing within a given batch (76 or 151 trajectories), we see that the nπ * quantum yield is higher than the ππ * quantum yield, namely ∼14% vs. ∼11% (151 trajectories) and ∼18% vs. ∼15% (76 trajectories). While this is correct qualitatively, we see that the nπ * quantum yield is only 1.2-1.3 times larger than the ππ * quantum yield instead of a known factor of ∼2. In this respect, we note that in this work we use FOMO-CIS, i.e., only single excitations within an active space of HOMO-1, HOMO, and LUMO are taken into account. To reveal the role of double excitations, we performed SH simulations with FOMO-CISD within the same active space, resulting in nine Slater determinants used to construct wave functions. These calculations resulted in a quantum yield (for the monomer) of ∼30% (29.8 ± 3.7% for 151 trajectories and 30.3 ± 5.3% for 76 trajectories). The corresponding nπ * lifetime is 1092 fs. Thus, while inclusion of double excitations considerably increases the quantum yield (from ∼14% (CIS) to ∼30% (CISD) in the case of the full set of 151 trajectories), the nπ * lifetime still remains long, ∼1 ps (it decreases from 1266 fs (CIS) to 1092 fs (CISD), see Fig. for S 1 populations calculated with both methods). Expansion of the active space is therefore needed to obtain a shorter lifetime compatible with earlier works. Further, similarly to the case of the ππ * excitation, we observe smaller quantum yields when going from the monomer to the tetrameric models (Tab. 3). Specifically, the nπ * quantum yields are ∼7-8% for models with a = 5.5 Å and tetramer 3.5 Å, and 0 for SAM 3.5 Å.