The exclusion of the TIP4P/ε model is attributed to its lack of internal degrees of freedom. We also provide additional mode-wise vibratioanl density of states in the Supporting Information. ). This unphysical behavior is unsurprising since the OH bond strength constant of SPC/Fw was designed to fit the simulation data to the IR spectrum obtained in both gaseous and liquid phases . Conversely, the DPMD model exhibits a stronger concordance with the experiment, showcasing peak positions that are more closely matched and a broader, overlapping mode that spans a wide frequency range, mirroring the characteristics observed in the experimental data. A small but noticeable mismatch of the maximum frequency (ν DP,stretch = 3550 cm -1 may explain why the second damped harmonic oscillator peak of the dielectric spectrum obtained in the DPMD simulation is located ) libration (rotation) band (L, 625 cm -1 ), (3) bending band (B, 1650 cm -1 ), ( ) bounded OH stretching band (BS, 3400 cm -1 ), and ( ) free OH stretching band (FS, 3700 cm -1 ) . In (d), the relationship between the bending frequency ν HOH and the stretching frequency ν OH also clearly demonstrates the superiority of the DPMD model. This relationship is obtained by the data from water in different organic solvents including acetone, propylene carbonate, liquid H 2 O-D 2 O and more.