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Revealing the pure confinement effect in glass-forming liquids by dynamic mechanical analysis

Autor(en)
Johannes Koppensteiner, Wilfried Schranz, Michael Allan Carpenter
Abstrakt

The dynamic mechanical response of mesoporous silica with coated inner surfaces confining the glass-forming liquid salol is measured as a function of temperature and frequency (1–100 Hz) for various pore sizes (2.4–7.3 nm). Compared to former results on natural pores, a distinct acceleration of dynamics due to the removal of surface-related retardation of molecular dynamics is found now, which can be fitted by a homogeneous relaxation using an unmodified Vogel-Fulcher-Tammann relation. This lubrication effect leads to a stronger decrease in the glass transition temperature Tg with decreasing pore size. The present data allow to quantify and separate competing side effects as surface bondings and negative pressure from the pure confinement induced acceleration of molecular dynamics with decreasing pore size. We analyze the dynamic elastic susceptibility data in terms of a recently proposed procedure [C. Dalle-Ferrier et al., Phys. Rev. E 76, 041510 (2007)], which relates the number Ncorr,T of molecules, whose dynamics is correlated with a local enthalpy fluctuation, to the three-point dynamic susceptibility chi T. The observed increase of Ncorr,T with decreasing temperature strongly indicates that the size xi of dynamic heterogeneities increases when approaching the glass transition.

Organisation(en)
Physik Funktioneller Materialien
Externe Organisation(en)
University of Cambridge
Journal
Physical Review B
Band
81
Anzahl der Seiten
8
ISSN
1098-0121
DOI
https://doi.org/10.1103/PhysRevB.81.024202
Publikationsdatum
2010
Peer-reviewed
Ja
ÖFOS 2012
1030 Physik, Astronomie
Link zum Portal
https://ucrisportal.univie.ac.at/de/publications/7b458dbb-da63-4a41-86e5-44b282356a07