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Aging phenomena in poly(methyl methacrylate) thin films: Memory and rejuvenation effects

Department of Polymer Science, Kyoto Institute of Technology, Matsugasaki, Kyoto 606-8585, Japan

^*Corresponding author. Electronic address: fukao@kit.ac.jp
^†Present address: Department of Macromolecular Science, Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043, Japan.

Phys. Rev. E 71, 041803 – Published 21 April, 2005

DOI: https://doi.org/10.1103/PhysRevE.71.041803

Abstract

The aging dynamics in thin films of poly(methyl methacrylate) (PMMA) have been investigated through dielectric measurements for different types of aging processes. The dielectric constant was found to decrease with increasing aging time at an aging temperature in many cases. An increase in the dielectric constant was also observed in the long-time region $(⩾ 11 h)$ near the glass transition temperature for thin films with thickness less than $26 nm$ . In the constant-rate mode including a temporary stop at a temperature $T_{a}$ , the memory of the aging at $T_{a}$ was found to be kept and then to be recalled during the subsequent heating process. In the negative-temperature cycling process, a strong rejuvenation effect has been observed after a temperature shift from the initial temperature $T_{1}$ to the second temperature $T_{2}$ $(= T_{1} + Δ T)$ when $Δ T \approx - 20 K$ . Furthermore, a full memory effect has also been observed for the temperature shift from $T_{2}$ to $T_{1}$ . This suggests that the aging at $T_{1}$ is totally independent of that at $T_{2}$ for $Δ T \approx - 20 K$ . As $∣ Δ T ∣$ decreases, the independence of the aging between the two temperatures was found to be weakened—i.e., the effective time, which is a measure of the contribution of the aging at $T_{1}$ to that at $T_{2}$ , is a decreasing function of $∣ Δ T ∣$ in the negative region of $Δ T$ . As the film thickness decreases from $514 nm to 26 nm$ , the $∣ Δ T ∣$ dependence of the effective time was found to become much stronger. The contribution of the aging at $T_{2}$ to that at $T_{1}$ disappears more rapidly with increasing $∣ Δ T ∣$ in thin-film geometry than in the bulk state.

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Aging phenomena in poly(methyl methacrylate) thin films: Memory and rejuvenation effects

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