The Impact of the Molecular Weight on the Nonequilibrium Glass Transition Dynamics of Poly(Phenylmethyl Siloxane) in Cylindrical Nanopores

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Abstract
Changes in the glass transition dynamics caused by the nanoconfinement reveal pronounced out-of-equilibrium features. Therefore, the confinement effects weaken with time. Using the Dielectric Spectroscopy (DS), we have investigated the impact of the molecular weight on the equilibration kinetics of the studied polymer embedded within anodic aluminum oxide (AAO) nanoporous templates. For our research, we have used poly(phenylmethyl siloxane) with low (Mw = 2530 g/mol) and high (Mw = 27800 g/mol) molecular weight. We have found that the observed faster dynamics of the nanopore-confined systems weaken with time, and ultimately it is possible to regain the bulk-like mobility. The equilibration time increases with reducing the pore size and lowering the annealing temperature much below the glass transition temperature of the interfacial layer, Tg_interface. The experimental data analysis has also revealed that the molecular weight of the nanopore-confined polymer’s influences the recovery of the bulk segmental relaxation time, τα. Low-molecular-weight poly(phenylmethyl siloxane) rearrange and reach denser packing of the polymer chains with greater ease than the high-molecular-weight one. Finally, we have also demonstrated that the molecular weight affects the relationship between the time constant characterizing the equilibration kinetics and the characteristic time of the viscous flow in the cylindrical channels of the nanometer size.
Funding Information
  • Narodowe Centrum Nauki (OPUS 14 nr. UMO-2017/27/B/ST3/00402)

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