The first attempt to dissect the reaction mechanism of the light-induced chromophore hydration in Dreiklang was described by Lacombat et al. following their femtosecond spectroscopy experiments. The authors of a later study formulated critical comments on this tentatively proposed mechanism and suggested an alternative scheme by results of computational simulations. The key finding of Ref. is that the population of the excited-state level of a charge-transfer character in the ON-state, which is nearly isoenergetic with the locally excited state, is an essential step in the ON → OFF photochemical reaction in Dreklang. Preliminary characterization of the reaction intermediates described in Ref. is based on the AIMD molecular dynamics simulations carried out with the Q-Chem program . The ONIOM version of the QM(DFT(ωB97X-D))/MM(CHARMM27) approach was applied to analyze 250 fs trajectories for the two lowest electronic states obtained in the TDDFT approach. This analysis suggested several possible candidates for the reaction intermediate X; however, lacking a confirmation of the observed transient absorption band of X and reliable estimates of its energy in the ground electronic state.