Journal of Dental Research

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Relaxation of Polymerization Contraction Stresses by Flow in Dental Composites

C.L. Davidson and A.J. De Gee
J DENT RES 1984 63: 146
DOI: 10.1177/00220345840630021001

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Relaxation of Polymerization Contraction Stresses by Flow in Dental Composites
C. L. DAVIDSON and A. J. de GEE
Department of Dental Materials Science of the University ofAmsterdam, Louwesweg 1, 1066 EA Amsterdam, The Netherlands
The hardening stresses in wall-to-wall bonded composites were
measured and related to calculated values obtained from freely
shrinking materials.
Since the ultimate tensile strength of the materials contracting
under restricted conditions was not lower than that of composites
which were not hindered during the polymerization shrinkage, the
conclusion was drawn that the contraction was compensated for
by flow instead of internal disruptions.
J Dent Res 63(2):146-148, February, 1984
Introduction.
The advantages of adhesion of composite restorations to
the cavity wall are well established (Craig, 1980). Discus-
sion still exists about whether contraction during polymeri-
zation may damage the restoration and its marginal seal
(Asmussen, 1975; Lee and Orlowski, 1977; Bausch et al.,
1982; Lambrechts et al., 1983; Bowen et al., 1983). It can
be expected that the polymerizing material which shrinks
under restricted conditions -e.g., due to adhesion to the
cavity wall - may be disrupted or will lose its bond to the
tooth structure. Fractured margins or loose fillings may be
the result. However, if gelation of the resin proceeds gradu-
ally, the material could yield to the stresses, without damag-
ing the internal structure and adhesive bonds. In such a
case, polymerization shrinkage may not be as harmful to
the adhesive restoration as often as has been stated.
The purpose of this study was to investigate the flow of
two composite materials during the early stage of setting, in
which most of the polymerization shrinkage occurs.
Materials and methods.
The materials used in this study, Silar and Concise, differ
in structure but belong to the same chemical family (see
Table 1), containing Bis-GMA and TEGDMA as the main
components of the resin phase. Polymerization was started
by mixing two pastes according to the manufacturer's
instructions. Mixing and setting took place at 240C ± 1 0.
The volumetric polymerization shrinkage was determined
with a modified dilatometer as described by De Gee et al.
(1981). In order to study the flow right from the moment
of gelation, a special dumbbell-shaped mould was designed
(see Fig. 1). Both steel heads were connected to the heads
of a tensilometerl and aligned with a thin, flexible, cylin-
drical foil (inner diameter 2.7 mm, and length 7.5 mm),
which was fixed with an adhesive to the cylinder wall of the
vertical bore in the upper steel head. The foil did not
counteract the shrinkage of the materials to be tested. The
horizontal bores of the upper and lower steel heads were
taped off at one side. Freshly-mixed material was injected
into the mould through the horizontal bore of A (cf Fig.
1) with a syringe2 extended with a tube reaching into the
compartment of the lower head (B). This procedure was
carried out within 50 sec from the start of mixing.
Subsequently, the composite materials were allowed to
Received for publication July 18, 1983
Accepted for publication November 4, 1983
1 Zwick 146 3/0, Eisinger, West Germany
2HAWE Centrix, Neos, Switzerland
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exert tension on the system by polymerization contraction.
The upper cross-head connected to the load cell was dis-
placed by the contracting material, and the corresponding
forces were recorded, starting at the moment of gelation,
and continually during a period of 45 min. Each micro-
meter displacement of the head corresponded to a 100-N
force. The lower cross-head of the tensilometer counter-
acted the contracting resin material fully passively. For
free unrestricted conditions, the lower steel head (B) was
detached from the cross-head of the tensilometer and was
counter-balanced by elastic bands connected to the upper
steel head (A). At 45 min from the start of mixing, the foil
was cut in the middle over its full circumference, and the
motordrive was subsequently switched on for tensile
loading (cross-head speed, 0.1 mm/min) in order to deter-
mine the momentary elastic stress-strain ratio and the
tensile strength. The average values and standard deviations
were calculated for each material from five readings. From
the stress-strain ratio and the polymerization contraction
measurements, the "theoretical" contraction stress could be
calculated. The discrepancy between this value and the
actual stress was attributed to flow.
Results.
Fig. 2 shows representative curves for the free volu-
metric polymerization shrinkage of Silar and Concise
measured with the dilatometer at 24 0C. Table 1 gives the
values of the total volumetric polymerization shrinkage and
rigid contraction up to 45 min, and the moment of gela-
tion, measured at 24 0C. The moment of gelation corre-
sponds to the moment at which the setting composites start
to displace the load-cell of the tensilometer by contracting
forces. From this moment on, the setting materials are
considered to contract "rigidly" ("rigid contraction"). The
contraction stresses built up at 45 min, in our experimental
set-up, are shown in Table 2. If there is a completely rigid
polymerization shrinkage from the moment of gelation,
both Silar and Concise would have undergone a linear con-
traction of 0.75% at 45 min. From the Young's modulus
determined at 45 min (given in Table 2), it can be calcu-
lated that straining the samples for 0.75% to their original
length would produce a stress of acalc = 32.2 MPa in Silar
and acalc = 68.2 MPa in Concise. Experimentally, however,
stresses of aexp = 3.9 and 2.8 MPa were observed for Silar
and Concise, iespectively. The percentage of relaxation, p,
can be calculated by p = acalcUTcalc x 100%, being 88%
for Silar and 96% for Concise.
Discussion.
Composite resin systems shrink considerably during
setting. The contraction before the moment of gelation is
not regarded as having clinical relevance (Bausch et al.,
1982). The rigid contraction, however, has received much
attention in dentistry and is often assigned as the cause of
marginal defects (Asmussen, 1975; Lee and Orlowski, 1977;
Lambrechts et al., 1982; Bowen et al., 1983).
In contemporary dentistry, where, due to pre-treatment
of enamel and (in some cases) dentin, adhesion between
Vol. 63 No. 2 FLOW OF DENTAL COMPOSITES 147

TABLE 1
THE MATERIALS USED IN THIS STUDY: TOTAL VOLUMETRIC POLYMERIZATION SHRINKAGE AND RIGID CONTRACTION
UP TO 45 MIN AND THE MOMENT OF GELATION, MEASURED AT 24 °C
Polymerization Contraction
Paste Moment of (vol%)
Material Mfg. Co. A B Gelation (sec) Total* Rigidt
Silar 3M, St. Paul (USA) ON1 OK2 170 2.75 (0.08) 2.25 (0.11)
Concise 3M, St. Paul (USA) 9L15 9N15 133 2.43 (0.09) 2.22 (0.11)
* Total volumetric contraction between 1.5 and 45 min after the start of mixing.
t Volumetric contraction between the moment of gelation and 45 min after the start of mixing.
(Number of specimens per experiment was five; standard deviations in parentheses.)

(vol.%)
"
A

C Fig. 1 - Dumbbell-shaped
mould for determining flow of
composite materials during
setting. A and B: upper and
B lower cylindrical steel heads,
connected to the cross-heads
of the tensilometer. C: compo-
site material cylindrically
shaped by a thin flexible foil
(diameter = 2.7 and length
7.5 mm). Arrows indicate
direction of tensile loading.
filling material and cavity wall can be achieved, polymeri-
zation shrinkage may be of less importance. From our
experiments, it can be concluded that, in a setting com-
posite, stress causes flow, which compensates for shrinkage.
In the earliest stage of setting, the shrinkage is maximal,
but fortunately the material is still weak and able to yield.
Presumably, only chain formation takes place, and cross-
linking is not at full reaction. The molecules can slip into
new positions and orientations. After some time, the ma-
terial gains strength but also has less to yield, because the
contraction decreases. Although it must be realized that
the relaxation of the hardening stresses proceeds continu-
ously with time, we based the estimation of the relaxation
on readings at one given moment. At 45 min, approximate-
ly 95% of the total polymerization contraction has expired.
If the materials had contracted the total 0.75%, the
0 10 20 30 40 50 60 70 80
=
time (minutes)-
Fig. 2 - Volumetric polymerization shrinkage curves of Silar
and Concise measured with the modified dilatometer at 24 °C.
- : moment of gelation.
samples would have been strained under fully restricted
conditions for the same 0.75%. However, for Silar and for
Concise, strains of 0.09% and 0.03%, respectively, were
demonstrated experimentally. This means that a consider-
able part of the hardening stress is compensated for by
flow.
That the material is not damaged internally by the yield-
ing has been demonstrated by the equal tensile strengths of
samples hardened under either free or restricted conditions.
In Fig. 3, the remaining stress situation is drawn sche-
matically. The drawn line shows the theoretical stress
approaching the stress of a completely set sample settled at
100%. The interrupted line represents the relaxation of
stress by flow of the material setting under restricted con-

TABLE 2
CONTRACTION STRESS, YOUNG'S MODULUS, TENSILE STRENGTH AND FLOW UNDER RESTRICTED CONDITIONS, AND
YOUNG'S MODULUS AND TENSILE STRENGTH UNDER FREE CONTRACTION CONDITIONS DETERMINED
45 MIN AFTER MIXING AT 24 °C
Contraction Contraction Stress Young's Modulus Tensile Strength Relaxation
Material Condition (MPa) (MPa) (MPa) (%)
Silar restricted 3.9 (0.3) 4300 (525) 20.6 (2.0) 88 (3)
Concise restricted 2.8 (0.3) 9220 (745) 27.3 (2.6) 96 (1)
Silar free 4170 (660) 20.4 (1.9)
Concise free 8650 (925) 27.5 (3.8)
(Number of specimens per experiment was five; standard deviations in parentheses.)
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148
stress W°O
DA VIDSON & DE GEE
0 t moment of
Igelation
theoretical stress
n remaining stress
time
Fig. 3 Schematic representation of the remaining stress in
-
polymerizing composite materials when setting contraction is re-
stricted.
-theoretical stress, calculated when completely rigid contraction
occurs from the moment of gelation (100% at 24 hr).
---- relaxation due to flow, calculated from the difference between
theoretical and experimental stress.
ditions. The vertical distance between these two lines
represents the remaining elastic stress. This stress gradually
grows from zero at the moment of gelation to approximate-
ly 10% of the theoretical stress at 45 min from the start of
the mixing.
The maximum contraction stress in a composite material
is probably dependent on the measuring device. The charac-
teristics of the tensilometer (displacement force transducer)
determine the actual transformation of contraction into
force. The less displacement needed for producing forces,
the more realistic the readings. Therefore, the length of the
samples plays an important role. But the diameter of the
sample may also be relevant because of transverse contrac-
tions.
In one study, Bowen et al. (1983) obtained results that
varied with the method of investigation. Their samples
were 6 mm in diameter compared to ours (diameter, 2.7
mm). This may explain their observation of a higher maxi-
mum hardening stress (for Silar and Concise, 6.1 -6.4 and
5.5 -7.3 MPa, respectively). A similar explanation may be
valid, too, for the results of Hegdahl and Gjerdet (1977),
which are rather lower than ours.
The findings are of great importance for the evaluation
of adhesion in dentistry. For a following study, we modi-
fied the mould in such a way that one steel head was re-
placed by a flat piece of etched enamel. Since the bond
between sample and enamel did not fracture in any of these
experiments, it can be concluded that, during the whole
process of setting, the adhesion survives the yield stress.
These findings are in agreement which those of Hegdahl
and Gjerdet (1977).
In our study, it has been shown that the adhesive com-
posite-enamel junction can resist the polymerization con-
traction forces and that the material is not damaged by this
Downloaded from jdr.sagepub.com at UNIVERSITY OF WINDSOR on October 19, 2014 For personal use only. No other uses without permission.
., . . . .
.ceai
Fig..opst
~ ~ ~ ~ ~. ,. tenamel
.......'.'.
......... ..........
.restoration
> 0 -
rersntto of
withadhsio (t enmel retritedan
denin:fre cntrctin)
..
1 l t 1 | '
tadeion(t
enho
,.
J Dent Res February 1984
............
..........
tensile stress. It still must be investigated whether the com-
posite-dentin bond can resist the contraction stresses. Even
....
if such a bond will only exist for a relatively short period,
e.g., during curing of the resin, this adhesion is of para-
mount importance for the adaptation of the composite
filling to the cavity wall.
In the absence of an adequate adherence of the compo-
site to the dentin, the filling will loosen from the bottom of
the cavity, leading to a gap (see Fig. 4). The presence of
such a gap has been emphasized by Hansen (1982). How-
ever, when a proper composite-dentin bond exists initially,
the material will flow during polymerization. Good adapta-
tion will be maintained even if the adhesion is released after
some time.
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ASMUSSEN, E.: Composite Restorative Resins. Composition versus
Wall-to-wall Polymerization Contraction, Acta Odontol Scand
33:337-344, 1975.
BAUSCH, J.R.; de LANGE, C.; DAVIDSON, C.L.; PETERS, A.; and
de GEE, A.J.: The Clinical Significance of the Polymerization
Shrinkage of Composite Restorative Materials, J Prosthet Dent
48:59-67, 1982.
BOWEN, R.L.; NEMOTO, K.; and RAPSON, J.E.: Adhesive Bond-
ing of Various Materials to Hard Tooth Tissues: Forces Develop-
ing in Composite Materials During Hardening, JADA 106:475-
477, 1983.
CRAIG, R.G.: Restorative Dental Materials, VIth ed., St. Louis,
Toronto, London: The C.V. Mosby Co., 1980.
HANSEN, E.K.: Contraction Pattern of Composite Resins in Dentin
Cavities, Scand J Dent Res 90:480483, 1982.
HEGDAHL, T. and GJERDET, N.R.: Contraction Stresses of Com-
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de GEE, A.J.; DAVIDSON, C.L.; and SMITH, A.: A Modified
Dilatometer for Continuous Recording of Volumetric Polymeri-
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3642, 1981.
LAMBRECHTS, P.; AMEYE, C.; and VAN HERLE, G.: Conven-
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J Prosthet Dent 48:5 27-53 8, 1982.
LEE, H.L. and ORLOWSKI, J.A.: Differences in Physical Properties
of Composite Dental Restoratives: Suggested Causes and Clinical
Effects, J Oral Rehabil 4:227-236, 1977.
ZIDAN, O.; ASMUSSEN, E.; and JORGENSEN, K.D.: Tensile
Strength of Restorative Resins, Scand J Dent Res 88:285-289,
1980.