Journal
SOFT MATTER
Volume 11, Issue 4, Pages 719-731Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4sm01893a
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Funding
- French Department for Higher Education and Research
- EU-US Transatlantic Degree Program in Engineering
- Upper Normandy region
- National Science Foundation [CMMI-1068952, IIA-1338988]
- Nebraska Research Initiative
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1068952] Funding Source: National Science Foundation
- Office Of Internatl Science &Engineering
- Office Of The Director [1338988] Funding Source: National Science Foundation
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The effect of structural constriction on molecular mobility is investigated by broadband dielectric spectroscopy (BDS) within three types of molecular arrangements: monomers, oligomers and self-assembled monolayers (SAMs). While disordered monomers exhibit a variety of cooperative and local relaxation processes, the constrained nanodomains of oligomers and highly ordered structure of monolayers exhibit much hindered local molecular fluctuations. Particularly, in SAMs, motions of the silane headgroups are totally prevented whereas the polar endgroups forming the monolayer canopy show only one cooperative relaxation process. This latter molecular fluctuation is, for the first time, observed independently from other overlapping dielectric signals. Numerous electrostatic interactions among those dipolar endgroups are responsible for the strong cooperativity and heterogeneity of the canopy relaxation process. Our data analyses also revealed that the bulkiness of dipolar endgroups can disrupt the organization of the monolayer canopy thus increasing their ability to fluctuate as temperature is increased.
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