By analyzing Fig. and 7 it is possible to see that the CT-TSH approaches, where all the atoms were considered in the computation of the quantum momentum (CT-TSH-FGAC and CT-TSH-TGCA), presented better agreement with TSH-ODC concerning the populations decay and Φ. The much slower decay of the S 2 state observed in CT-TSH when only the CNNC atoms were taken into account in the computation of the quantum momentum (CT-TSH-FGLA and CT-TSH-TGLA) can be attributed to the even higher occurrence of hops and "back" hops between the S 1 and S 2 states when compared to the other methodologies. For intance, in the case of CT-TSH-TGLA, the occurrence of hops and "back" hops between those states increases by 51% and 61%, respectively, when compared to CT-TSH-FGAC, and by 46% and 36% when compared to CT-TSH-TGAC. It is expected that large values of the Gaussian widths lead to an underestimation of the quantum momentum. By contrast, widths that are too small have the effect to produce a very "bumpy" density: this could potentially lead to a large quantum momentum that changes its direction for small nuclear displacements. Consequently, the ct contribution to the time derivative of the electronic coefficients undergoes frequent phase changes, inducing fluctuations in the state probabilities.