In both the TD-ADGA and the two TI-ADGA calculations the equilibrium geometry for the A ′ state was used as the reference geometry for the PES fits. In the TI-ADGA calculations to obtain the reference A ′ and A states, a mean VSCF density consisting of the lowest eight eigenstates were used. This high number of eigenstates was used to ensure a good description of the PES in a broad domain of the PES. The settings were also modified to place the initial SPs at a displacement of ± 1.1180 Bohr from the used reference distance of 5.1386 Bohr. This was done in to reduce the number of SPs required by the TI-ADGA algorithm as many SPs were placed when extending the potential boundaries using the default initialization. In total 18 SPs were used to fit the A ′ surface and 26 SPs were used to fit the A surface. In Fig. , we show how the TD-ADGA algorithm constructs a PES for the A state during the dynamics. Figs. 2a, 2b, and 2c shows the zeroth, first, and fifth sub-iteration of the zeroth TD-ADGA iteration, respectively. In Fig. , the zeroth sub-iteration of the zeroth TD-ADGA iteration is started by inputting the initial density. The initial density is space-smoothened (dashed green line) and then inputted to the TD-ADGA algorithm (full green line). The TD-ADGA then places SPs at the reference geometry and at two displacements, such that the initial density is contained. A PES is then fitted to the initial SPs and the integration boxes defined by the initial SPs are evaluated. In Fig. , the integration boxes are all sub-divided by adding new SPs and the convergence of each box is evaluated. Integration boxes that are not converged are further sub-divided in the subsequent sub-iterations until convergence is obtained. Fig. shows the PES and SPs obtained after the fifth sub-iteration of the zeroth TD-ADGA iteration. After this sub-iteration, the PES is converged and the TD-ADGA algorithm continues. The values of the integration boxes at this step is saved and used to evaluate the change in all the subsequent TD-ADGA iterations until new SPs are evaluated. The time propagation is now started and the TD-ADGA convergence is checked at intervals of 100 a.u. (2.42 fs). Fig. shows the 21st TD-ADGA iteration, where the density has moved enough for the TD-ADGA to request a new SP. After the new SP has been evaluated the integration boxes are again evaluated and checked for convergence compared to the boxes evaluated just before the SP was added. It is found in this iteration that the PES is converged after only adding a single SP and the TD-ADGA algorithm continues. This TD-ADGA iteration was carried out after 2000 a.u.