As mentioned above, after 29 h of the contact at room temperature, the molecules near the solid surface were oriented parallel to the solid surface, forming a layered density distribution (Figure (b)). However, the charge-dipole interactions are broken at a particular rate by the thermal motion of the molecules, and the other molecules replace the molecular chain segments on the charge sites if the vacant sites make a new bond with the different molecular segments. This displacement proceeds irreversibly due to the conformational entropy gain because the released chain segments by the substitution can form a three-dimensional conformation. After this displacement progresses, the number of PDMS molecules directly attracting the solid surfaces is increased, and only partial segments of the PDMS molecules interact with the charge sites. In this situation, the volume occupied by the PDMS molecules that directly attract the solid surfaces also increases. Note that, since the molecular chain length of PDMS used in this study is as long as 250 nm, the molecular motion of the segments not interacting with the solid surface is also limited when the other segments are making charge-dipole bonds. Thus, the increased volume occupied by these molecules suppresses molecular mobility over longer distances. Since the lower molecular mobility at the interface results in an excess of both viscosity and elasticity at the interface compared to the bulk, an increase in the number of molecules interacting with the solid surface increases the decay length λd of the long-range repulsive force Fcons, long. In addition, As mentioned above, the increase in ∆γ-∆γhyd near the solid surface (Figures ), 4(e, f), 5(e, f)) demonstrated the low mobility of the molecules in the layers closest to the solid surface. This result also suggests that the charge-dipole interaction on the closest layer is strong and limits the mobility of the molecular segments directly interacting with solid surfaces. Therefore, the fact that the activation energy of the λd elongation ∆Elong was significantly larger than ∆Eη was most likely based on the substitution of charge-dipole bond.