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Parallel Emergence of Rigidity and Collective Motion in a Family of Simulated Glass-Forming Polymer Fluids
Authors
Jack F. Douglas
Wen-Sheng Xu
Xiaolei Xu
Publication date
13 June 2023
Publisher
View
on
arXiv
Abstract
The emergence of the solid state in glass-forming materials upon cooling is accompanied by changes in both thermodynamic and viscoelastic properties and by a precipitous drop in fluidity. Here, we investigate changes in basic elastic properties upon cooling in a family of simulated polymer fluids, as characterized by a number of stiffness measures. We show that
Ο
Ξ±
\tau_{\alpha}
Ο
Ξ±
β
can be expressed quantitatively both in terms of measures of the material ``stiffness'',
G
p
G_p
G
p
β
and
β¨
u
2
β©
\langle u^2 \rangle
β¨
u
2
β©
, and the extent
L
L
L
of cooperative particle exchange motion in the form of strings, establishing a direct relation between the growth of emergent elasticity and collective motion. Moreover, the macroscopic stiffness parameters,
G
p
G_p
G
p
β
,
B
B
B
, and
f
s
,
q
β
f_{s, q^*}
f
s
,
q
β
β
, can all be expressed quantitatively in terms of the molecular scale stiffness parameter,
k
B
T
/
β¨
u
2
β©
k_{\mathrm{B}}T / \langle u^2 \rangle
k
B
β
T
/
β¨
u
2
β©
with
k
B
k_{\mathrm{B}}
k
B
β
being Boltzmann's constant, and we discuss the thermodynamic scaling of these properties. We also find that
G
p
G_p
G
p
β
is related to the cohesive energy density
Ξ
C
E
D
\Pi_{\mathrm{CED}}
Ξ
CED
β
, pointing to the critical importance of attractive interactions in the elasticity and dynamics of glass-forming liquids. Finally, we discuss fluctuations in the local stiffness parameter as a quantitative measure of elastic heterogeneity and their significance for understanding both the linear and nonlinear elastic properties of glassy materials.Comment: 69 pages, 18 figure
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oai:arXiv.org:2306.07759
Last time updated on 16/06/2023