Several decades ago, the mapping approach was used for the calculation of spectroscopic signals . Nowadays, the methodology has actively been used and advanced . Yet it is rather demanding to employ the mapping method for the calculation of three-time NRFs, owing to the necessity to do multiple forward and backward propagations on a three-dimensional time grid. Hence the methodology is usually applied to model systems, because its use for the onthe-fly spectroscopic simulations of realistic molecules is computationally costly. Spectroscopic signals can also be computed by combining the SQC/MM dynamics with the time-dependent nonperturbation approach . However, this implementation is highly demanding for on-the-fly simulations: It requires a direct inclusion of the laser field into the Hamiltonian, and each time delay between the pulses requires a separate calculation.