The interfaces then become occupied by randomly coiled segments, which include those that have detached from the solid surface. 9 Although this explanation does not assume a delayed formation of the layered structure above Mc or the fact that the layered structure is metastable, a similar interpretation consistent with our results is possible with some modifications based on the segmental substitution on the solid surface. The layered structure is metastabilized by the solid surface / liquid molecule interaction on the closest layer and the intermolecular interactions between the layers. After the substitution process on the closest layer, the segments released from the solid surface make the loops and tails. Since these structures act as conformational obstacles for maintaining the layered density distribution, the substitution process on the closest layer destabilizes the layered structure. This causes the stability of the layered structure on the interface to decrease over time, resulting in random coiling on the interface.