As the next step in refining our understanding of the computational accuracy of our approach, we investigated the impact of basis set size. For this, we utilized the segmented contracted versions of the polarization consistent basis sets (pcseg-n). The convergence of the vibrational frequencies and IR and Raman intensities for a single snapshot is presented in Fig. , Fig. , and Fig. for acetone in water or vacuum using pcseg-3 or pcseg-4 as a reference, respectively.