Materials Research Innovations

ISSN: 1432-8917 (Print) 1433-075X (Online) Journal homepage: http://www.tandfonline.com/loi/ymri20

Time dependent effects of various staining agents

on colour of artificial teeth
M. amil Akyil & F. Bayindir
To cite this article: M. amil Akyil & F. Bayindir (2010) Time dependent effects of various
staining agents on colour of artificial teeth, Materials Research Innovations, 14:5, 365-369, DOI:
10.1179/143307510X12820854748755
To link to this article: http://dx.doi.org/10.1179/143307510X12820854748755

Published online: 18 Jul 2013.

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Date: 11 November 2016, At: 05:53

Time dependent effects of various staining

agents on colour of artificial teeth
M. Samil Akyil* and F. Bayindir
The purpose of this in vitro study was to evaluate the colour changes in six brands of porcelain
and of acrylic teeth after their immersion in tea, filtered coffee and cola for 1 day, 1 week, 2 weeks
and 4 weeks. The study comprised three brands of porcelain and three brands of acrylic teeth.
Five central maxillary incisors from the six types of artificial denture teeth were distributed equally
into four groups (n530) according to the four immersion solutions. Colour measurements on each
tooth were made before their immersion, and repeated after 1 day, 1 week, 2 week and 4 week
immersions in the four solutions using the CIE L*a*b* colour measuring system. The colourimetric
data were converted to National Bureau of Standards units. The data were analysed statistically
by repeated measures analysis of variance (ANOVA), one- and two-way ANOVA, and Tukey
honestly significant difference (HSD) multiple comparison tests. It was found that tea was more
chromogenic than either filtered coffee or cola, and that acrylic teeth that had been immersed in
tea for 4 weeks displayed the greatest colour change when compared to porcelain teeth. Tea is
more chromogenic than filtered coffee and cola. The colour stability of porcelain teeth is greater
than that of acrylic teeth. The degree of discolouration of acrylic and porcelain teeth after their
immersion in tea, filtered coffee and cola is time dependent.
Keywords: Colour stability, Acrylic denture teeth, Porcelain denture teeth

Introduction
Of all artificial teeth, those made from either methacrylate resin based or porcelain have the best esthetics.1
However, the colour stability of methacrylate resin and
porcelain is crucial for maintaining their dental
esthetics.2 The degree of discolouration of artificial teeth
can be affected by a number of intrinsic and extrinsic
factors that include incomplete polymerisation, water
sorption, diet, oral hygiene and photo-oxidation.3,4 The
intrinsic factors are related to the chemical stability and
oxidation of polymer matrices of the material, and causes
of discolouration include accelerated aging, water effects,
ultraviolet irradiation from sunlight, temperature and
environmental humidity.46
The extrinsic factors include diet, oral hygiene and the
adsorption of colourants in beverages.3,7 Beverages,
such as coffee, tea and cola, coloured dental irrigants,
such as chlorhexidine, and nicotine are known to cause
discolouration of oral tissues and dental materials, and
among these, coffee, tea and cola cause the greatest
degree of discolouration.711 Additionally, the degree
of discolouration of artificial teeth that is caused by
coloured dental irrigants is reported to be substantially
greater than that caused by ultraviolet radiation alone.6

Department of Prosthodontics, Faculty of Dentistry, Ataturk University,

Erzurum, Turkey
*Corresponding author, email samilakyil@hotmail.com

W. S. Maney & Son Ltd. 2010

Received 11 August 2009; accepted 6 October 2009
DOI 10.1179/143307510X12820854748755

Acrylic resin teeth have several advantages over porcelain teeth: they weigh less, are less likely to fracture,
and the quality of the bond between the tooth and the
base is better.12 However, they are inferior to porcelain
teeth in maintaining an acceptable esthetic appearance
because they become discoloured more rapidly, and do
not wear well. As a result, their durability and service life
is shorter than those of porcelain teeth.2 Although
porcelain teeth are superior to resin based teeth because
of their better wear resistance properties and esthetic
appearance, porcelain teeth can become discoloured
because of progressive adsorption of colourants on the
porcelain surface and infrequent cleaning.1,2,13
The reflective colours of surfaces can be measured by
tristimulus colour analysers, such as a spectrophotometer
or a colourimeter14,15 using the CIELAB Colour CIE
L*a*b* system which was developed by the Commission
Internationale de lEclairage (CIE).16,17 In this system,
colour perception is designed to approximate human
vision, and changes in colour are reported in three spatial
coordinates, L*, a* and b*, where L* represents the
brightness (value) of a shade, a* represents the amount of
red-green colour and b* represents the amount of yellowblue colour. Using this information, colour differences
for each spatial coordinate can be measured in order to
calculate the overall colour difference DE.
When a material is completely colour stabile, no
colour difference will be detected after exposure of a test
material to the test environment (DE50). Although
different thresholds values of colour difference above

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Colour stability of artificial teeth

Table 1 Types of porcelain and acrylic teeth that were used in this study
Type of
material

Porcelain

Acrylic

Trade name

Manufacturer

Shade and
form

Code

Real
Porcelain Teeth
Vacuum
Natura Vacuum
Major Dent
Midway
Acry Rock

Enta B.V. Brouwerijbaan, Bergen op Zoom, The Netherlands

SMIC Shanghai, Pudong New Area, Shanghai, China

A1, 113
2, 341

R
PT

Zahnfabrik Bad Nauheim, GmbH & Co. Luxor KG, Frankfurt, Germany
Major Prodotti Dentari S.p.A., Moncalieri, Italy
Zahnfabrik Bad Nauheim, GmbH & Co. Luxor KG, Frankfurt, Germany
Dental Manufacturing S.p.A., Via Ca` Mignola Nuova (Ro), Italy

36, 275
1F, 33/A
A1, P2
A1, K10

N
MD
M
AR

which the colour change is perceptible to the human eye

have been reported by various authors,7,1822 a DE value
of 3?7 or less is considered to be visually imperceptible,
as well as being clinically acceptable.14,19,20,23
In the dental literature, there are only a few studies
which have compared the colour change in both porcelain
and acrylic teeth after their exposure to coloured
solutions.1,2,24 Koksal and Dikbas2 and Mutlu-Sagesen et
al.1 compared the colour change in both porcelain and
acrylic teeth after their exposure for 1 day, 1 week,
2 weeks and 4 weeks to tea, cola and coffee in vitro.
They reported that both porcelain and acrylic teeth
became discoloured in coffee after 4 weeks. In view of
increasing consumption of coloured beverages, and the
paucity of information on their potential to cause
discolouration of teeth, more data are needed on the
colour changes in porcelain and acrylic resin teeth after
their exposure to coloured beverages. For these reasons,
the purpose of this in vitro study is to evaluate the colour
change in six brands of porcelain and acrylic teeth after
their immersion in tea, filtered coffee and cola for 1 day,
1 week, 2 weeks and 4 weeks.

Method and materials

Six brands of porcelain and acrylic teeth were used in
this study, and their trade names, manufacturers, shade
and form, and codes are given in Table 1. Five maxillary
central incisors from each of the six brands of removable
partial dentures were distributed equally into four equal
groups (n530) according to the following immersion
solutions: filtered coffee, tea and cola (coloured solutions), and distilled water (control solution).

Preparation of staining solutions

To prepare the filtered coffee solution, 6 g of commercially available filtered coffee (Kraft Foods Deutschland,
GmbH, Bremen, Germany) was added into 300 mL of
boiling distilled water. The tea solution was prepared by
immersing two tea bags that each contained 2 g of tea
(Lipton Yellow Label Tea; Unilever, Istanbul, Turkey)
into 300 mL of boiling distilled water for 10 min. The
filtered coffee and tea solutions were then stirred for 10 s
every 15 min until the temperature of the solution was
37uC, and then passed through filter paper to remove any
particulate residues. The cola storage solution was
undiluted Coca-Cola (Coca-Cola Co., Istanbul, Turkey).
Each solution was stirred once a day in order to reduce the
precipitation of particles, and replaced daily.

Colour measurements
The colour of each tooth was measured before immersion
in each solution by the CIE L*a*b* system using
a colourimeter (Shade Eye NCC; Shofu Dental
Corporation, Kyoto, Japan).25 Before each measurement,

the colourimeter was calibrated according to the manufacturers recommendations. Each measurement session
comprised three colour measurements that were taken
from the central region of the cervical area of each tooth
(24 mm from the gingival region). The mean values of
the L*, a* and b* measurements were then calculated, and
were used as the baseline measurements. After completing
the baseline colour measurements, the teeth were then
immersed in 300 mL of various immersion solutions (see
later for their preparation) in capped flasks that were
maintained in a temperature controlled water bath (type:
SB1X; Grant Instruments Ltd, Cambridge, England) at
371uC.
The colour measurements for each tooth were repeated
after 1 day, 1 week, 2 weeks and 4 weeks of immersion in
the coloured and control solutions. For these repeated
colour measurements, each tooth was rinsed in distilled
water for 5 min, and then blotted dry with tissue paper
before the colour measurement. Colour was then measured
three times in each tooth in the identical manner that was
described for the baseline colour measurement.
The mean values of the L*, a* and b* measurements
were calculated, and were then used as to calculate the
colour difference DE* from the baseline measurement
for each tooth at each of the four different immersion
times using the formula

1=2
DE  ~ (DL )2 z(Da )2 z(Db )2
where DE is the colour change in all dimensions (L*a*b*),
and DL*, Da* and Db* are the colour changes in each
spatial coordinate.17 In order to relate DE* to the clinical
environment, the data were converted to National Bureau
of Standards (NBS) units1,2 using the equation
NBS units~DE  |0:92
where the specific colour differences are expressed in
terms of NBS units (Table 2).

Statistical analysis
Repeated measures analyses of variance (ANOVA), with
two between unit factors (material and solution) and one
within unit factor (immersion time) in order to identify
Table 2 Critical remarks of colour differences using NBC
grading system
Critical remarks of colour differences

NBS unit

Trace
Slight
Noticeable
Appreciable
Much
Very much

00.5
0.51.5
1.53.0
3.06.0
6.012.0
12.0z

Extremely slight change

Slight change
Perceivable change
Marked change
Extremely marked change
Change to other colour

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Table 3 Colour differences DE, colour differences in each

spatial coordinate and NBS values of porcelain
and acrylic teeth after their immersion in tea for
1 day, 1 week, 2 weeks and 4 weeks: data are
shown as mean colour change at each immersion time relative to baseline measurement for
each tooth type
Time

1 day

1 week

Tooth
code DE
R
PT
N
MD
M
AR
R
PT
N
MD
M
AR

R
PT
2 weeks N
MD
M
AR
R
PT
4 weeks N
MD
M
AR

DL*

Da*

Db*

0.633
0.350
0.000 20.125
1.573
0.950 20.025 21.100
0.891
0.850
0.050
0.150
0.907
0.200
0.050 20.625
1.187
0.900 20.200
0.000
0.641
0.450
0.000 20.325
1.025 20.050
0.375
1.408
2.435
0.150
0.275 20.550
0.679
0.350
0.150
0.125
0.966 20.075
0.250 20.800
0.776
0.400 20.100 20.600
0.675
0.025
0.175 20.625
.
.
1 719
1 350
0.150
0.150
3.028
0.325
0.000
0.000
0.275
0.100
0.100
1.062
3.237
1.075 20.200 20.200
0.955
0.250
0.150
0.150
1.102
0.675
0.325
0.325
1.289
1.175
0.025 20.350
2.482
0.875
0.050 22.425
0.615
0.275
0.150
0.250
3.505
1.200 20.425 22.625
2.250 20.400 21.925
3.163
3.252
1.125
0.000 23.075

NBC
units
0.582
1.447
0.819
0.834
1.092
0.589
1.295
2.240
0.625
0.889
0.714
0.621
1.295
2.240
0.625
0.889
0.714
0.621
1.186
2.283
0.566
3.225
2.910
2.991

the main effects and possible interactions between these

factors, and to evaluate the effects of each type of
storage solution and immersion time on DE* for each
type of artificial tooth. The relationships between tooth
type, storage solution and the onset time of discolouration were assessed using Wilks lambda with an a priori
level of significance of a50?05. Two-way ANOVA was
used to evaluate the effect of the type of storage solution
on DE* for each tooth type at each immersion time.
One-way ANOVA and Tukey honestly significant
difference (HSD) multiple comparison tests were applied
to each between unit factor with the level of a set at 0?05.

Table 4 Colour differences DE, colour differences in each

spatial coordinate and NBS values of porcelain
and acrylic teeth after their immersion in ltered
coffee for 1 day, 1 week, 2 weeks and 4 weeks:
data are shown as mean colour change at each
immersion time relative to baseline measurement
for each tooth type
Time

1 day

1 week

Tooth
code DE
R
PT
N
MD
M
AR
R
PT
N
MD
M
AR

R
PT
2 weeks N
MD
M
AR
R
PT
4 weeks N
MD
M
AR

DL*

Da*

NBC
units

Db*

0.984
0.775 20.050
0.300
0.847
0.575 20.150
0.025
0.581
0.350 20.100 20.050
1.439
1.000
0.000 20.150
0.915
0.750
0.000 20.225
1.281
1.075
0.175 20.500
1.299
1.225 20.125
0.100
0.776
0.675 20.025
0.125
0.568 20.025
0.075
0.025
1.100
0.050
0.200 20.900
1.234
1.125
0.000 20.150
1.842
0.775
0.025 21.075
1.238
1.125
0.175
0.350
0.998
0.825
0.100 20.250
0.573
0.025
0.150
0.125
1.426
0.475
0.250 21.250
1.453
0.825
0.175 21.025
2.661
1.375
0.175 22.225
1.792
1.650
0.075
0.450
1.135
0.850 20.075 20.525
0.805 20.250
0.000
0.025
1.964
0.950
0.075 21.700
2.256
1.225 20.200 21.850
2.489
1.350
0.250 21.925

0.905
0.780
0.534
1.324
0.842
1.179
1.195
0.714
0.523
1.012
1.135
1.695
1.139
0.918
0.527
1.312
1.337
2.448
1.648
1.045
0.740
1.807
2.075
2.290

Table 5 Colour differences DE, colour differences in each

spatial coordinate and NBS values of porcelain
and acrylic teeth after their immersion in cola for
1 day, 1 week, 2 weeks and 4 weeks: data are
shown as mean colour change at each immersion time relative to baseline measurement for
each tooth type
Time

1 day

Results
The colour differences of porcelain and acrylic teeth
after their immersion in the four solutions for 1 day,
1 week, 2 weeks and 4 weeks are summarised in
Tables 36. There were statistically significant interactions (P,0?001) between tooth type, solution type and
the duration of the immersion. Of the three coloured
solutions, tea was found to be more chromogenic than
either filtered coffee or cola whose chromogenic effects
were not significantly different from each other.
Immersion in distilled water for 4 weeks did not cause
any discolouration to the porcelain and acrylic teeth.
When the NBS grading system was used to assess
colour change, it was found that tea caused a perceivable colour difference in the Porcelain Teeth
Vacuum porcelain teeth and the Midway and Acry
Rock acrylic teeth, and a marked colour difference in
the Major Dent acrylic teeth after immersion for
4 weeks (Table 4). Filtered coffee caused perceivable

Colour stability of artificial teeth

1 week

Tooth
code DE
R
PT
N
MD
M
AR
R
PT
N
MD
M
AR

R
PT
2 weeks N
MD
M
AR
R
PT
4 weeks N
MD
M
AR

1.066
1.805
0.683
0.645
1.117
0.593
1.291
0.754
1.517
1.213
1.424
0.717
2.174
0.770
1.162
1.019
1.132
0.882
0.789
1.024
1.315
1.266
1.190
0.746

DL*

Da*

NBC
units

Db*

0.850
0.125
0.500
1.475 20.075 20.525
0.225
0.075
0.000
0.300
0.275
0.100
0.475 20.100 20.100
20.150
0.150 20.350
.
0 750
0.075
0.950
0.325
0.000 20.175
20.675
0.125
0.350
20.725
0.250 20.200
0.750
0.400
0.825
20.150
0.200
0.250
1.350
0.100
1.500
0.350
0.175
0.075
0.350
0.475
20.700
20.675
0.400
0.125
0.100
0.325
0.625
20.175
0.100
0.075
20.050
0.325
0.650
0.600
0.275
0.300
0.400
0.325
0.625
0.225
0.475
0.400
20.175
0.225
0.250
20.150
0.325
0.175

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1.661
0.628
0.593
1.028
0.545
1.188
0.693
1.395
1.116
1.310
0.660
2.000
0.708
1.069
0.937
1.041
0.812
0.726
0.942
1.210
1.165
1.095
0.686

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Table 6 Colour differences DE, colour differences in each

spatial coordinate and NBS values of porcelain
and acrylic teeth after their immersion in distilled
water for 1 day, 1 week, 2 weeks and 4 weeks:
data are shown as mean colour change at each
immersion time relative to baseline measurement
for each tooth type
Time

1 day

1 week

Tooth
code DE
R
PT
N
MD
M
AR
R
PT
N
MD
M
AR

R
PT
2 weeks N
MD
M
AR
R
PT
4 weeks N
MD
M
AR

0.265
0.192
0.162
0.159
0.187
0.157
0.305
0.222
0.258
0.182
0.194
0.211
0.575
0.251
0.275
0.210
0.234
0.226
0.315
0.257
0.287
0.237
0.249
0.236

DL*

Da*

Db*

0.925
0.125
0.425
20.275
0.175 20.175
0.275 20.025
0.050
20.300
0.125 20.025
20.675 20.050
0.050
20.050
0.125
0.075
1.175
0.300
0.950
0.350
0.250
0.725
0.750
0.150
0.775
20.425
0.500
0.550
0.125
0.100
0.875
20.075
0.250
0.575
0.825
0.550
1.250
20.500
0.475
0.600
20.075
0.550
0.700
20.675
0.650
0.750
21.375
0.475
0.900
20.500
0.500
0.775
0.675
0.500
1.550
20.475
0.475
0.750
20.575
0.400
0.650
20.600
0.725
0.825
21.100
0.275
0.575
20.700
0.400
0.600

NBC
units
0.243
0.176
0.149
0.146
0.172
0.145
0.281
0.204
0.237
0.168
0.178
0.195
0.529
0.231
0.253
0.193
0.215
0.208
0.290
0.237
0.264
0.218
0.229
0.217

colour changes in all acrylic teeth and the Real porcelain

teeth only after immersion for 4 weeks (Table 5).
Further, the degree of discolouration was dependent
upon the immersion time for these coloured beverages:
the longer the immersion time, the greater the degree of
discolouration. There was no discolouration in any of
the teeth that were immersed in cola after 4 weeks using
this rating system (Tables 7 and 8).

Discussion
In the present study, it was found that the tea caused
more discolouration to artificial teeth than either filtered
coffee or cola, and the degree of discolouration increased with immersion time. In addition, it was found
that porcelain teeth were more resistant to discolouration than acrylic teeth.
Although instruments, such as spectrophotometers
and colourimeters, and visual assessments can be used to

Colour stability of artificial teeth

Table 8 Differences between each type of porcelain and

acrylic teeth after their immersion for four weeks
in various solutions
R
S

PT
D* S

DW a
Cola a,
b
Tea a,
b
FC b

N
D* S

MD
D* S

DW a
Cola a

DW
Tea

a
a,
b
b

FC

FC

Tea

Cola c

M
D* S

AR
D* S

D*

DW a
Cola a,
b
FC b

DW a
Cola a

DW a
Cola a

FC

FC

Tea

Tea

Tea

S: solution; D: differences according to the results of the Tukey

honestly significant difference (HSD) multiple comparison test;
DW: distilled water; FC: filtered coffee.
*Different letters indicate dissimilarity of groups (P,0?05).

measure the extent of discolouration of dental materials,2 instrumental measurements are preferred because
the measurements are not compromised by the subjective interpretation of visual assessments.7,26 When
these instruments use the CIELAB Colour CIE L*a*b*
system to measure colour, they report colour changes in
three spatial coordinates in order to calculate DE.16 The
authors used such a system to measure the colour
difference DE after immersing artificial teeth in filtered
coffee, tea and cola. Additionally, the NBS developed a
clinical classification system for comparing colour
differences in dental materials using NBS units.24 In
this measuring system, an observer can report on his/her
perception of the colour change.27
In this study, the authors used the CIELAB Colour
CIE L*a*b* and NBS systems to assess colour
differences of artificial teeth after their immersion in
tea, filtered coffee and cola. It was found that the highest
NBS unit value was 3?2, a value which describes the
colour change as a marked change according to the
NBS system. Using the CIELAB Colour CIE L*a*b*
system, it was found that the highest DE value was 3?5,
and this value is lower than the acceptable upper DE
limit of 3?7 when using this system.14,19,20,23
Mutlu-Sagesen et al.1 commented that it is difficult to
create an in vitro experimental environment in order to
mimic the in vivo oral environment. The aim of our
study was to assess the effect of three different staining
solutions on the degree of discolouration of artificial
teeth for 4 weeks in a simulated in vivo oral environment.
For this purpose, the immersion solutions were maintained at a constant temperature of 37uC and these
experimental conditions have been used by other
investigators.13,9,10,2830 The duration of the immersion

Table 7 Comparison of colour change in each type of articial teeth after 4 week immersion in each solution
Tea

Filtered coffee

Cola

Distilled water

Tooth code

D*

Tooth code

D*

Tooth code

D*

Tooth code

D*

N
R
PT
M
AR
MD

a
a, b
a, b, c
b, c
c
c

N
PT
R
MD
M
AR

a
a, b
a, b, c
b, c
b, c
c

AR
R
PT
M
MD
N

a
a
a
a
a
a

AR
MD
M
PT
N
R

a
a
a
a
a
a

D: differences according to the results of the Tukey honestly significant difference (HSD) multiple comparison test.
*Different letters indicate dissimilarity of the groups (P,0?05).

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for such studies is a source of contention. Some

investigators have suggested that 4 weeks should be
minimal immersion time in order to assess the effect of a
coloured solution on the degree of discolouration,
whereas others have commented that 4 weeks is too
long.1,2,4,7,14,31,32 In the authors study, the authors
chose 4 weeks as the duration of the immersion period
which is considered to be the minimal in order to
measure a cumulative staining effect.
In this study, it was found that tea caused more
discolouration of the artificial teeth than filtered coffee
and cola. Moreover, this action was time dependent
because the degree of discolouration increased with longer
immersion time. The authors findings are in agreement
with those of previous in vitro studies that reported that tea
caused a greater degree of discolouration of polymeric
dental materials than coffee or cola.7,8,11 They suggest that
the discolouration of acrylic teeth that was caused by tea
was probably due to both adsorption and absorption of
polar colourants in the tea at the surface of acrylic teeth.
Perceivable colour changes were observed in the three
brands of porcelain teeth, and the Midway and Acry
Rock brands of acrylic teeth, and a marked colour
change was observed the Major Dent acrylic teeth after
a 4 week immersion in tea according to the NBS rating
system. Perceivable colour changes were observed also
in the three brands of acrylic teeth, and in Real brand of
porcelain teeth after a 4 week immersion in filtered
coffee. Slight or extremely slight colour changes in all
the artificial teeth were observed after 4 week immersion
in cola. Several investigators reported that coffee was
more chromogenic than tea and cola.1,2,10,30 This
contrasts with the authors findings where it was found
that filtered coffee was less chromogenic than tea, and in
particular for acrylic teeth. The authors suggest that the
difference between the authors results and those of
others could be due to differences in the methods of
preparing the tea and filtered coffee solutions.
It was found that porcelain teeth were less susceptible
than acrylic teeth to the staining action of tea, filtered coffee
and cola, and this result is consistent with those of
previously published studies.1,2,13 While the authors did
not investigate the underlying mechanism for this difference
in susceptibility to colour change, they suggest that the
water sorption properties of acrylic and porcelain may
account for this difference. The penetrability of water
soluble stains is lower in porcelain teeth than in acrylic teeth
because the stains are adsorbed on the porcelain surface.
Compared to filtered coffee and cola, it was found
also that the tea was the most chromogenic solution, and
the degree of discolouration increased with increasing
immersion time, although the DE values were within the
clinical acceptable limit (DE,3?7).14,19,20,23 Although
discolouration of porcelain and acrylic teeth occurred
after their immersion in tea, filtered coffee and cola, the
most discolouration occurred after their immersion in
tea. Additionally, it was found that the porcelain teeth
were more colour stabile than acrylic teeth. Therefore,
wearers of removable partial dentures should be warned
that the degree of discolouration of acrylic and porcelain
teeth is dependent upon their dietary habits.

Conclusions
Within the limitations of the authors in vitro study, the
authors concluded that:

Colour stability of artificial teeth

1. Tea was more chromogenic than filtered coffee and

cola.
2. The colour stability of porcelain teeth was greater
than that of acrylic teeth.
3. The degree of discolouration of acrylic and
porcelain teeth after their immersion in tea, filtered
coffee and cola was time dependent.

Acknowledgement
This research is supported financially by the Department
of Scientific Research Projects of Ataturk University
(Project No. 2003/158).

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