Hydrogen bonding between water and amine is clearly evident in the MD ensembles, as seen from the projection plots of the atomic density around different origin atoms, as shown in Figures in the Supplemental Information. The color contour plots show atomic density distributions around a central molecule from the solvent-water mixture with xA = 0.42. Figures and show a strongly localized atomic density of water around the nitrogen moiety of DIPA, as expected due to hydrogen bond formation. In principle, amines can hydrogen bond to each other with an N-H-N interaction, but the calculations show that this tendency is very weak. There is a slight tendency for DIPA molecules to coordinate one another but the DIPA atomic density around DIPA molecules in the mixture is fairly isotropic, as evident by the generally uniform ring of amine around the central amine molecule (Figures and). As expected, we do see a strong hydrogen bonding tendency of water around water (Figures and). The fact that significant water-water hydrogen bonded interactions are present in the MD ensembles of the xA = 0.42 mixture supports the picture that there is significant clustering of water in the mixture despite the two species, water and amine, being present in fairly equal proportion. This is in agreement with our hypothesized DIPA-water-DIPA MCSs.