The approach we developed in this work can be applied to D The DMS from our ML-based charges significantly improves the predictions of these dielectric properties, particularly the appearance of the hydrogen-bond stretch peak around 200 cm -1 , which is absent in the spectra computed from non-polarizable models. After removing the CT in the ML-based model through a neutralization procedure, we find that the hydrogen-bond stretch peak vanishes, whereas the dielectric constant barely changes. This result indicates that within our point-charge description of the DMS, the intermolecular CT is the major source of the peak intensity at 200 cm -1 , whereas the intramolecular polarization dominates the enhancement of the dielectric constant. We also revisit how the increasing percentage of exact HF exchange in the hybrid functional affects the polarization and CT in liquid water. Consistent with our previous work, the trend for our ML based charges shows that polarization increases while CT decreases with increasing percentage of exact HF exchange, which consequently leads to the increase of the dielectric constant and the reduced intensity of the 200 cm -1 peak in the IR spectrum of liquid water. The success of our model demonstrates the possibility of using a different set of partial atomic charges for the DMS from those used for the PES, and expands the use of the efficient rigid non-polarizable water models for the accurate prediction of DMS-related properties. We plan to extend our model to more heterogeneous systems (e.g., water interfaces ) and the simulations of nonlinear spectroscopy (e.g., nonlinear terahertz spectroscopy ), where polarization and CT may have more pronounced effects. Furthermore, the idea of employing different sets of partial atomic charges for PES and DMS may see broader applications beyond water in the simulation community using force fields.