The enhancing and diminishing of polarization on the surrounding water are considered to appear as differences in the interaction energy components (E ES , E EXREP , E POL , E CT , and E DISP ) in the aqueous TMAO/TBA solution (Figures 4, S7, S8, and Tables ). Therefore, the interaction energy components near the hydrophilic/hydrophobic groups are discussed. ). The natural bond orbital analysis explains the charge-transfer interaction with a dimer model (Figures S9, S10 and Table ).