1. Introduction
Despite the technological significance of the Payne
effect in rubber applications [1], this strain-induced
softening phenomenon is often regarded as a spe-
cial area of physics specific to filled elastomers [2].
Practically, the effect is measured as decreasing
storage modulus with increasing strain amplitude at
fixed temperature and fixed frequency during
dynamic-mechanical testing of filled rubbers. Par-
allel, the corresponding loss modulus runs through
a maximum value with increasing strain amplitude.
Basic characteristics of the relationships between
dynamic modulus and strain amplitude are similar
for all kinds of investigated rubbers filled with con-
ventional fillers like carbon black and silica (see,
for example, reference [2]), or even for non-conven-
tional rubber nanocomposites which were prepared,
for example, via clay–NR latex dispersion and sub-
sequent vulcanization [3, 4].
It is essential to note that dynamic strain-induced
decrease of the stiffness of filled rubbers shows a
striking similarity to what is known phenomenolog-
ically about the glass transition of solid materials
and the jamming transition of granular materials [5,
6]. This analogy stems from the reality that shear
strain in dynamic mechanical measurements intro-
duces fluctuations in a filler network by forcing the
system to explore different configurations. Such
fluctuations can be described by an ‘effective tem-
perature’ that has many attributes of a true tempera-
ture, and particularly is proportional to the strain
amplitude [7, 8]. Thus, filled rubbers with respect to
strain will display many unusual phenomena that
are usually observed in glass-forming materials, but
now demonstrated in filled rubbers, including asym-
metric kinetics, crossover effects, and glasslike
kinetic transitions [2, 5–7]. Indeed, the increase of
the particle concentration may lead to jamming and
291
A statistical mechanical approach to the Payne effect in
filled rubbers
G. Heinrich
1*
, T. A. Vilgis
2
1
Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Str. 6, 01069 Dresden, Germany
2
Max-Planck-Institut für Polymerforschung Mainz, Postfach 3148, 55021 Mainz, Germany
Received 1 October 2014; accepted in revised form 30 November 2014
Abstract. In this paper we apply and discuss some new aspects to the steric interaction of filler particles in reinforced elas-
tomers under dynamic mechanical loading conditions. At certain concentration the filler particles (for example, carbon black,
or silica) form loose clusters which themselves interact with each other and form a filler network with a significant contri-
bution to the dynamic modulus of the rubber material. The filler concentration is relatively high, so that it is likely that the
clusters undergo a ‘jamming transition’. With increasing strain amplitude under periodic mechanical deformation the disrup-
tion of the filler network resp. of finite filler cluster configurations leads to dejamming observed as softening of the rubber.
As a theoretical approach we map the problem on a simple one dimensional Ising model. We present here a static model of
this jamming (dejamming) and discuss the consequences on the mechanical and deformation properties of the filled rubber.
Keywords: rubber, mechanical properties, Payne effect, statistical mechanics
eXPRESS Polymer Letters Vol.9, No.3 (2015) 291–299
Available online at www.expresspolymlett.com
DOI: 10.3144/expresspolymlett.2015.26
*
Corresponding author, e-mail: gheinrich@ipfdd.de
© BME-PT