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The effect of structural constriction on molecular mobility is investigatedby broadband dielectric spectroscopy (BDS) within three types of moleculararrangements: monomers, oligomers and self-assembled monolayers (SAMs). Whiledisordered monomers exhibit a variety of cooperative and local relaxationprocesses, the constrained nanodomains of oligomers and highly orderedstructure of monolayers exhibit much hindered local molecular fluctuations.Particularly, in SAMs, motions of the silane headgroups are totally preventedwhereas the polar endgroups forming the monolayer canopy show only onecooperative relaxation process. This latter molecular fluctuation is, for thefirst time, observed independently from other overlapping dielectric signals.Numerous electrostatic interactions among those dipolar endgroups areresponsible for the strong cooperativity and heterogeneity of the canopyrelaxation process. Our data analyses also revealed that the bulkiness ofdipolar endgroups can disrupt the organization of the monolayer canopy thusincreasing their ability to fluctuate as temperature is increased.

From Monomers to Self-Assembled Monolayers: The Evolution of Molecular Mobility with Structural Confinements