Although we used one of the best functionals (ωB97X-D) ? in our AIMD simulations, the analysis of structural parameters (g OO (r), the number of hydrogen bonds formed) shows that our AIMD water is somewhat over-structured relative to TIP3P and state-of-the-art simulations , similar to the simulations using less accurate density functionals. However, the structure of the second solvation shell appears to be reproduced better with AIMD than with TIP3P, as compared to the experimental g OO (r). The detailed analysis of structural parameters extracted from the MD and AIMD simulations as well as comparison with other simulations are given in the SI. Overall, we find that the differences between the spectra computed with MD and AIMD snapshots are small and are washed out by the statistical averaging. However, it is desirable to improve the sampling in future work by using, for example, path-integral simulations with accurate many-body potentials as was done in Ref.