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Molecular dynamic heterogeneity in relation to free volume and relaxation dynamics in organic glass formers: oligomeric cis-1,4-poly(isoprene)

Abstract

A combined study of the molecular rotation dynamics and the free volume in cis-1,4–poly(isoprene) using two external probing techniques via ESR and PALS together with relaxation dynamics of the host medium via BDS is presented. The spectral evolution of spin probe TEMPO from simulations over a wide range from 100 K up to 300 K exhibits three different regions of its correlation time consisting of a slow regime at low temperatures followed by the molecular dynamic heterogeneity zone from TX1slow = Tin,fast = 155K = 0.82×TgDSC up to Tc ≅ 236K =1.26×TgDSC and ending with a fast regime at high temperatures with the further characteristic ESR temperatures: TX2slow = 186K ≅ TgDSC and TX1fast = 260K. These are in close coincidence with four characteristic PALS temperatures: Tb1G = 160K, TgPALS = 190K, Tb1L = 227K and Tb2L = 263K. Finally, using BDS we reveal that the high-frequency features of the structural relaxation of 1,4-PIP 0.8k are related to the observed effects in the ESR and PALS response of the liquid state.

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Publication details

The article was received on 20 Jan 2017, accepted on 16 May 2017 and first published on 17 May 2017


Article type: Paper
DOI: 10.1039/C7CP00446J
Citation: Phys. Chem. Chem. Phys., 2017, Accepted Manuscript
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    Molecular dynamic heterogeneity in relation to free volume and relaxation dynamics in organic glass formers: oligomeric cis-1,4-poly(isoprene)

    H. Svajdlenkova, S. Arrese-Igor, Z. Nogelova, A. Alegria and J. BARTOS, Phys. Chem. Chem. Phys., 2017, Accepted Manuscript , DOI: 10.1039/C7CP00446J

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