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@INPROCEEDINGS{Zorn:1023009,
author = {Zorn, Reiner and Chua, Yeong-Zen and Schmelzer, Jürn W. P.
and Holderer, Olaf and Zamponi, Michaela and Schick,
Christoph},
title = {{D}etermination of the cooperativity length in glass
forming liquids and polymers},
reportid = {FZJ-2024-01595},
year = {2023},
abstract = {Although the idea of a ‘characteristic’ or
‘cooperativity’ length scale ξ related to the glass
transition is now wide-spread, there is much less consensus
on whether this length scale can be related to thermodynamic
fluctuations and, if yes, whether one has to consider
temperature fluctuations δT. The crucial experiment to this
end has to compare values of ξ from ‘thermodynamic’
formulae to independent values from structural-dynamics
experiments.An experiment with the aim of determining the
cooperativity length ξ in glass forming materials was
proposed some time ago by Ernst Donth [1]. The basic idea of
this experiment is to assign a length scale to the
AC-calorimetric relaxation time using the spatial resolution
of quasielastic neutron scattering. The main problem is to
find a range of relaxation times that is accessible by both
methods. From the very beginning it is clear that only
neutron-spin echo (NSE) is suited for this task. This raises
the additional problem that incoherent scattering has to be
measured. Therefore, significant progress in the performance
of NSE as well as AC calorimetry was required to conduct
this experiment.A first experiment of this kind was realised
on a glass-forming liquid, propylene glycol (PG) [2]. The
result was that agreement with the thermodynamic
calculations was better if temperature fluctuations were
accounted for. Nevertheless, in PG the difference between
the two thermodynamic estimates is small and the dynamics of
the methyl groups overlaps with the α relaxation.
Therefore, a material with a higher ‘contrast’ between
the alternatives was of interest and used in a second
experiment, poly(ethylmethacrylate) (PEMA). In addition,
neutron backscattering experiments showed that the methyl
group dynamics is better separated in PEMA. Finally, the
experiment benefitted from the upgrade of J-NSE with
superconducting coils. The new results show a clear
agreement with the thermodynamic calculation involving
temperature fluctuations.[1] E. Donth, Eur. Phys. J. E 12,
11 (2003).[2] Y. Z. Chua, R. Zorn, O. Holderer, J. W. P.
Schmelzer, C. Schick, E. Donth, J. Chem. Phys. 146, 104501
(2017).},
month = {Aug},
date = {2023-08-12},
organization = {9th International Discussion Meeting
on Relaxation in Complex Systems,
Makuhari Messe (Japan), 12 Aug 2023 -
18 Aug 2023},
subtyp = {Invited},
cin = {JCNS-1 / IBI-8},
cid = {I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)IBI-8-20200312},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G4 - Jülich Centre for Neutron
Research (JCNS) (FZJ) (POF4-6G4) / 5251 - Multilevel Brain
Organization and Variability (POF4-525) / 5241 - Molecular
Information Processing in Cellular Systems (POF4-524)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G4 /
G:(DE-HGF)POF4-5251 / G:(DE-HGF)POF4-5241},
experiment = {EXP:(DE-MLZ)J-NSE-20140101 / EXP:(DE-MLZ)SPHERES-20140101},
typ = {PUB:(DE-HGF)6},
url = {https://juser.fz-juelich.de/record/1023009},
}