Unlike conventional AIMD simulations, EFP-MD can be utilized to investigate the time evolution of dipole moments in aqueous TMAO/TBA solutions (Figure ). On average, the dipole moment of each water molecule is enhanced (4.20 D, +46%) when it approaches the N + O - group of TMAO. Similarly, when the water molecule approaches the OH group of TBA, the dipole moment is enhanced (3.78 D, +32%). The ensemble averages indicate that water molecules near the N + O -group of TMAO (r < 3.5 Å) and the corresponding OH group of TBA increased the dipole moment by an average of 3.22 D (+12%) and 3.01 D (+5%), respectively, compared to the water molecules in pure water (Table ). The former exhibits a more significant dipole moment because TMAO has a large dipole moment of 9.39 D in an aqueous