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@INPROCEEDINGS{Richter:1008203,
author = {Richter, Dieter and Allgaier, J. and Monkenbusch, Michael
and Kruteva, Margarita},
title = {{O}n the dynamics of large ring polymers in the melt - a
{SANS}, neutron spin echo and {PFG} - {NMR} study},
reportid = {FZJ-2023-02249},
year = {2023},
abstract = {The non-crossing requirement in non-concatenated ring
polymers creates topological constraints, which impose
important restrictions on the phase space of the system. For
ring polymers interpenetration is costly entropically and
compact structures evolve for high molecular weights - ring
polymers are assumed to become mass fractals confining rings
into territories. Other than the dynamics of linear or
branched chains that predominantly takes place via the chain
ends, rings do not feature ends and their dynamics is
considered to be self-similar and thus fundamentally
different to those of chains displaying ends. The present
state of the art model for the description of the internal
relaxations in dense ring systems was developed by
Rubinstein et al. /1/. This self-consistent Fractal Loopy
Globule (FLG) model is based on the conjecture that the
overlap criterion /2,3/ in the packing model for
entanglements also governs the rule for overlapping loops in
polymer rings. The constant overlap of loops is conjectured
to occur in a self-similar way over a wide range of length
scales from the elementary loop size Ne up to ring size R.
The dynamics of such rings in a melt is governed by
topological constraints that dilute with progressing time,
because with time loops of increasing sizes are relaxed and
cease to be obstacles.Recently, combining results of SANS
/4/ with PFG- NMR and NSE the unique topology driven
self-similar internal ring dynamics predicted by the FLG
model could be verified experimentally /5/: We find the
center of mass diffusion taking place in three dynamic
regimes from short to long times: (i) a strongly
sub-diffusive regime, where the center-of-mass mean square
displacement scales as $t^\alpha$ (0.4 ≤ $\alpha$ ≤ 0.6)
, until it reaches roughly the value $R_g^2;$ (ii) a second
regime with a $t^0.75$ scaling that (iii) at roughly 2.5
$R_g^2$ crosses over to Fickian diffusion. While the second
anomalous diffusion regime has been found in simulations and
was predicted by theory, we attribute the first one to the
effect of cooperative dynamics resulting from the
correlation hole potential. The internal dynamics at scales
below the elementary loop size is well described by ring
Rouse motion. At larger scales the dynamics is self-similar
and follows very well the predictions of the scaling models
with preference for the FLG model.ReferencesReferences:1. T.
Ge, S. Panyukov, and M. Rubinstein, Macromolecules 49,
708–722 (2016)2. T. A. Kavassalis and J. Noolandi,
Macromolecules 22, 2709–2720 (1989)3. L. J. Fetters, D. J.
Lohse, D. Richter, T. A. Witten, and A. Zirkel,
Macromolecules (1994)4. M. Kruteva, J. Allgaier, M.
Monkenbusch, L. Porcar, and D. Richter, ACS Macro Letters ,
507–511 (2020)5. M. Kruteva,M. Monkenbusch, J. Allgaier,
O. Holderer, S. Pasini, I. Hofmann and D. Richter, Phys.
Rev. Lett. (2020)},
month = {Jun},
date = {2023-06-14},
organization = {Flagship Workshop Ring Polymer
Dynamics, Monash University Prato
Centre (Italy), 14 Jun 2023 - 16 Jun
2023},
subtyp = {Invited},
cin = {JCNS-2 / PGI-4 / JARA-FIT / JCNS-1},
cid = {I:(DE-Juel1)JCNS-2-20110106 / I:(DE-Juel1)PGI-4-20110106 /
$I:(DE-82)080009_20140620$ / I:(DE-Juel1)JCNS-1-20110106},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G4 - Jülich Centre for Neutron
Research (JCNS) (FZJ) (POF4-6G4)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G4},
typ = {PUB:(DE-HGF)6},
url = {https://juser.fz-juelich.de/record/1008203},
}