Dental Materials (2004) 20, 530–534

http://www.intl.elsevierhealth.com/journals/dema

Color and opacity variations in three different

resin-based composite products after water aging
Alessandro Vichia,b,*, Marco Ferraria,b, Carel Leon Davidsonc

a
University of Siena, Siena, Italy
b
Tufts University, Boston, MA, USA
c
Academic Center for Dentistry ACTA, Amsterdam, The Netherlands

Received 29 August 2002; accepted 11 November 2002

KEYWORDS Summary Objectives. Correct shade selection and clinical procedures may be
Color; Composite resin; invalidated as a result of intrinsic color shifting with time. The aim of this study was
Aging to test the influence of exposure to water on the color stability of three structurally
different resin-based composites.
Methods. Six comparable Vita shades of three different resin-based composite
systems were selected. For each product at each shade, three disks were made, 1 mm
in thickness and 15 mm in diameter. The samples were studied with a spectropho-
tometer equipped with an integrating sphere. For color determinations, a 50% gray
card was used as background, and the data were recorded in the CIE Lp ap bp system.
Opacity was calculated as the ratio of the reflectance of a specimen disk when backed
by a black standard that when backed by a white standard. After the initial
measurements, the samples were stored for 30 days in a 60 8C water bath and then
measured again under the same conditions. The color shifts were calculated using the
formula: DE ¼ ½ðL1 2 L2 Þ2 þ ða1 2 a2 Þ2 þ ðb1 2 b2 Þ2 1=2 :
Results. If the standard of DE , 3:3 as clinically acceptable was taken into
consideration, one of the three materials involved in the study showed an
unacceptable color shift for all shades. Only one of the three materials remained
completely within an acceptable shade shift ðDE , 3:3Þ after aging. The difference in
the color stability between products was significant ðp , 0:001Þ: The differences may
be due to the different nature of the matrix and could also be correlated with filler
particles dimensions. With reference to opacity; the results showed a similar pattern
as that of the color and the statistical analysis also correlated.
Significance. From this work, it can be concluded that for some products, aging of
composites in water leads to color instability and opacity variation.
Q 2003 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.

Introduction restoration. 1 – 3 Unfortunately, although great

One of the major challenges for modern dentistry is
achieving a perfect color match between tooth and
*Corresponding author. Tel./fax: þ39-056425384.
E-mail address: avichi@mclink.it
improvements have been achieved during recent
years, color stability is still a problem.
As esthetic failures are one of the most common
reasons for replacing restorations,4 one would like
to employ predictable materials. However, due to
the quick turnover of dental materials resulting

0109-5641/$ - see front matter Q 2003 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.dental.2002.11.001
Color and opacity variations in three different resin-based composite products after water aging
from research progress and because of commercial
pressure, long-term clinical experience is usually
absent. To accelerate the aging process, in vitro
tests have been developed to predict the esthetic
performances of materials clinically.5 – 10 Most of
them are related to color stability, while only few
data are available on opacity changes with time.11
The results of these studies are difficult to
compare because composites shade differ from
brand to brand.12 More recently, several manufac-
turers introduced resin-based composite systems
whose available colors correlate to the Vita shade
guide.
Many factors have been claimed to be respon-
sible for the discoloration that takes place in the
oral environment.11,13 The aim of this study was to
evaluate color and opacity shifts in equal shades of
different last generation resin-based composite
products using the widely diffused test proposed
by Asmussen.8
Materials and methods
Three restorative systems were selected for this
study: Spectrum TPH (De Trey, Konstanz,
Germany), Tetric Ceram (Ivoclar, Schaan, Liech-
tenstein) and Z100 (3M, St Paul, MN, USA) (Table 1).
For each material, the availability of Vita shades
was checked and those shades that were simul-
taneously present in all three brands were selected
for the trial. Six colors were selected: A2, A3, A3.5,
A4, B2 and B3.
In a cylindrical mold, 1 mm thick sample discs of
15 mm in diameter were made. After application of
the material into the mold, a mylar sheet was
pressed over the surface with a glass plate in order
to obtain a flat surface. After 10 s curing with a
Visilux 2 light source (3M, St Paul, MN, USA), the
glass plate was removed in order to have
the optical-fiber tip closer to the sample, leaving
the mylar matrix in situ, and the samples were
polymerized for another 50 s. Great attention was
given to avoid bubble formation. No polishing
Table 1 Material selected for the trial (batch).
Tetric Ceram Spectrum TPH Z100
(Vivadent) (De Trey) (3M)
A2 926797 00852 8ME
A3 A04133 01049 8AA
A3.5 A00347 01047 8TJ
A4 A14685 01176 8FC
B2 A09983 00946 7GC
B3 926347 00386 8FW
531
techniques were used to avoid modification of the
surfaces that may influence the results. The
thickness of the samples was measured with a
50 mm-resolution caliper. Only the samples that
were within this resolution range were involved in
the study. For each shade, five samples were
prepared, for a total of 90 samples. Specimens
were stored in darkness at room temperature for
24 h to allow optimal conversion.
For color measurements, a spectrophotometer
(PSD1000, Ocean Optics, FL, USA) equipped with an
integrating sphere (ISP-REF, Ocean Optics, FL, USA)
with a 10 mm opening was used. The spectropho-
tometer was connected to a computer running
OOILab 1.0 (Ocean Optics, FL, USA) in Lp ap bp system
as color measurement software. D65 illumination
and a 108 standard observation angle were selected.
A 50% gray card (Kodak Co, Rochester, USA) was
used as a neutral background. For the evaluation of
the opacity, as it is defined as the ratio of the
reflectance of a specimen disk when backed by a
black standard to that when backed by a white
standard,11 black and a white cardboard were taken
from color separation scale Q-14 (Kodak Co,
Rochester, USA). After the measurements, the
samples were immersed for 30 days in a water
bath at 60 8C.8 After the immersion, the samples
were measured again both for color and opacity
measurements under the same conditions and using
the same procedures.
By applying the formula DE ¼ ½ðDLp Þ2 þ ðDap Þ2
þðDbp Þ2 1=2 ;14 it was possible to calculate DE and to
compare the values before and after the aging
treatment. Because the ability of the human eye
to appreciate differences in color differs from
individual to individual (as it is a combination of
eye characteristics and skill of the operator), three
different intervals were used for distinguishing
color differences. Values of DE , 1 were regarded
as not appreciable by the human eye. Values 1 ,
DE , 3:3 were considered appreciable by skilled
operators, but considered clinically acceptable,
whilst values of DE . 3:3 were considered appreci-
able also by non-skilled persons and for that reason
clinically not acceptable.11,12,15
ANOVA statistical analysis was performed both
for color and opacity.
Results
Color
All the materials showed a certain degree of
discoloration due to aging in water. Values ranged
532 A. Vichi et al.

ðp , 0:001Þ was found between Spectrum and Tetric

Table 2 Differences in color ðDEÞ after 1 month of water
aging. Ceram/Z100, while between Tetric Ceram and Z100
there was no statistically significant difference. As
Material Shade DE after 1 month for color, there was no evidence of different and
consistent behavior of the clearer and darker
Spectrum TPH A2 12.1
Spectrum TPH A3 15.6
colors, and the A and B based colors.
Spectrum TPH A3.5 11.5
Spectrum TPH A4 6.8
Spectrum TPH B2 9.3
Spectrum TPH B3 4.9 Discussion
Tetric Ceram A2 1.3
Tetric Ceram A3 1.4 It is extremely difficult to measure whether the
Tetric Ceram A3.5 2.2
appearance of restorative materials mimic natural
Tetric Ceram A4 3.2
Tetric Ceram B2 1.8 teeth. In the ideal case, the resin-based composite
Tetric Ceram B3 1.9 has to show the same reflectance, translucence and
Z100 A2 0.8 transparency as tooth structure. A formal definition
Z100 A3 1.4 for translucency is not available in the CIE inter-
Z100 A3.5 4.4
Z100 A4 3.9
national lightning vocabulary16 or in the ASTM
Z100 B2 6.1 standards.17 However, it can be defined as the
Z100 B3 3.6 potential of a material to scatter a portion of the
incoming light, whilst the remaining light is trans-
mitted.18 This property is quite difficult to measure.
from very little (0.76 for Z100 A2) to high shifts
What usually measured is the opacity, which is
(15.60 for Spectrum A3) (Table 2).
commonly defined as the ratio of the reflectance of a
If the value DE . 3:3 is taken as the limit for
specimen disk when backed by a black standard to
clinical appreciation of color variation, Spectrum
that when backed by a white standard.11 The
showed a mismatch for all the selected shades, all
opacity, in the common visual assessment, can be
the shade shifts of Tetric Ceram lay within this
considered as the inverse of translucency. This
limit, whilst 67% of the Z100 samples showed a
property should not be confused with gloss. Gloss
mismatch.
is a property of a surface, which involves specular
ANOVA analysis showed a statistically significant
reflection and is responsible for a lustrous or mirror-
different ðp , 0:001Þ behavior between Spectrum
like appearance. Glossiness is connected with the
and Tetric Ceram/Z100. Between Tetric Ceram and
surface condition, while opacity refers to the diffuse
Z100 no significant difference could be demon-
rather than to the specular aspects of appearance.18
strated, although the overall results were best for
Several laboratory tests have been proposed in
Tetric Ceram. The parameter that was most
order to simulate and accelerate the discoloration
affected was the Lp value, while the ap value was
that takes place under clinical conditions over a
scarcely influenced. The bp values for Tetric and
relatively long time.7,10 Asmussen’s test8 is still the
Z100 decreased only a little, whilst this value for
reference test for such trials, not in the least
Spectrum showed a more perceptible increase (to
because the requirements for the devices are quite
yellow). There was no clear pattern of color shifts
simple.11
between clearer and darker colors, and no unmis-
For this study, the samples were stored for 24 h
takable differences were noted between A and B
at room temperature and then measured for color
based colors.
determination. No polishing techniques were used
in this phase because great attention was given in
Opacity order to have samples as similar as possible to each
other, and the polishing technique may modify the
The Opacity of all tested materials increased after surface of the samples.
water aging, but Tetric Ceram B3 showed a In order to properly measure the optical proper-
decrease. As the value was very low, it may be ties of the materials, the spectrophotometer was
due to the tolerance of the measuring instrument. equipped with an integrating sphere. This configur-
Some values were particularly high, especially ation permits good reliability of the results19 better
for Spectrum TPH; the A2 shade showed an increase than visual assessment20,21 or other instrumental
in opacity of 29.7%. configurations.18
Once again, the ANOVA statistical analysis An explanation for the shifts in optical proper-
revealed that a statistically significant difference ties due to water exposure might be found in
Color and opacity variations in three different resin-based composite products after water aging 533

the materials’ composition and the way they are
affected by environmental conditions. It is known
from literature that resin-based composites allow
water to penetrate the matrix or filler – matrix
interface.22,23 As it is assumed that the resin
component is the source of discoloration, one
would expect that a high volume fraction of the
resin correlates with a high prospect for discolor-
ation.11 From this study, the amount of matrix resin
could not be directly associated with the degree of
color shift (filler load by volume for Spectrum is 57%,
for Tetric 60% and for Z100 66%). This is in accordance
with observations by Dietschi13 who stated that
relatively small differences in filler-resin ratio
could not explain for variations in water sorption.
The color shifts may well be related to the nature of
the resin matrix (Bis-GMA, Bis-EMA and TEGDMA for
Spectrum, Bis-GMA, UTDMA and TEGDMA for Tetric
and Bis-GMA and TEGDMA for Z100). In fact, it is
known that the uptake of water by TEGDMA is higher
than by UTDMA.24 The presence in the resin matrix of
Tetric Ceram of roughly 40% by weight of UTDMA, not
present in the other two composites, may reduce the
water uptake and, consequently, the color shift
induced by water sorption. Also the increase of the bp
value (to yellow) in the composite that had the
greater discoloration can be connected with this
different nature of the matrix.
Also the size and distribution of the filler
particles seems to correlate directly with the
results; in fact, the resin composite with the higher
filler dimension (Spectrum 0.04 –5 mm with 50% of
the particles larger than 1.48 mm) was shown to be
more susceptible to water aging discoloration,
versus the two resin-based composite systems in
which the overall filler dimension was smaller
(Tetric 0.04 –3 mm with 80% of the particles larger
than 1.5 mm; Z100 0.04 – 3.5 mm with 74% of the
particles smaller than 1.0 mm). This may be
tentatively explained considering that color per-
ception is directly connected with scattering. As
the interface between resin and particles is one of
the weakest points of the composite material, with
a high sensitivity to water sorption,25 it may be
supposed that hydrolytic degradation of this inter-
face can modify the way in which the light is
scattered by the particles. A different dimension of
particles may determine a different degree of water
aging susceptibility correlating with the dimension
of filler particles. This may also explain the fact
that the results on opacity showed a similar pattern
of results as those of color, the hydrolytic degra-
dation of the matrix alters the scattering pattern
and this may lead to mutation in composite opacity.
While for color, the level of clinical acceptability
has been investigated,11,12,15 there is no literature
available for the level of clinical acceptance of
opacity variations.
It has to be emphasized that in this study, the
opacity was evaluated as an intrinsic property of
the material, to be distinguished from gloss, which
is a surface property.
Conclusion
In this study, it has been shown that water acts
as a discoloring agent to varying degrees for all

Table 3 Opacity values and variation after 1 month of water aging.

Material Shade Opacity Opacity Opacity variation

t ¼ 0 (%) t ¼ 1 month (%) t ¼ 0=t ¼ 1 month

Spectrum TPH A2 63.8 93.5 þ 30

Spectrum TPH A3 65.6 75.5 þ 10
Spectrum TPH A3.5 63.0 81.6 þ 19
Spectrum TPH A4 63.6 75.6 þ 12
Spectrum TPH B2 58.6 74.4 þ 16
Spectrum TPH B3 62.9 73.4 þ 11
Tetric Ceram A2 55.0 57.7 þ3
Tetric Ceram A3 56.9 59.3 þ2
Tetric Ceram A3.5 57.1 61.0 þ4
Tetric Ceram A4 67.5 72.6 þ5
Tetric Ceram B2 62.4 64.7 þ2
Tetric Ceram B3 65.6 65.2 þ0
Z100 A2 60.3 61.8 þ2
Z100 A3 66.1 66.9 þ1
Z100 A3.5 61.9 69.6 þ8
Z100 A4 63.8 68.7 þ5
Z100 B2 65.3 75.0 þ 10
Z100 B3 64.2 67.1 þ3
534
the materials selected. Taking the value DE ¼ 3:3
as the limit for clinical acceptability for the
discoloration, one of the three materials selected
for this study performed significantly worse than
the other two. This may be explained by the
different nature of the resin matrix, and also may
be correlated with the dimension distribution of the
filler particles. The smaller the dimension of the
particles the lower the water aging susceptibility.
The results for opacity also showed it to be
influenced by water aging. The pattern of the
results for opacity variation was the same as that
for color (Table 3).
Further studies are necessary in order to better
understand the process of discoloration of resin-
based composites, evaluating the various par-
ameters that affect clinical discoloration.
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