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                   DENTAL MATERIALS
                   TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
Original Article
                   FRACTOGRAPHIC ANALYSIS
                   Brendan M. Angus1a*, John J. Mecholsky Jr.1b, Nader Abdulhameed2c
                   1
                       Materials Science and Engineering Department, College of Engineering, University of Florida, Gainesville FL, USA
                   2
                       College of Dentistry, University of Florida, Gainesville FL, USA

                   a
                     BS, Research Assistant
                   b
                     PhD, Professor and Associate Chair of the Materials Science and Engineering Department
                   c
                    BDS, MS, PhD Student, Clinical Assistant Professor of Restorative Dental Science


                   ABSTRACT                                               DOI: 10.25241/stomaeduj.2018.5(1).art.1
                   Objective: To outline a procedure to determine the fracture toughness of direct resin                                          OPEN ACCESS This is an Open Access
                   composites failing from “natural” flaws.                                                                                       article under the CC BY-NC 4.0 license.

                   Methodology: Tensile (hour glass) tests (n = 30) of a conventional hybrid dental                                               Peer-Reviewed Article

                   composite (Tetric EvoCeram, Ivoclar Vivadent) were fabricated and fractured in uniaxial                                    Citation: Angus BM, Mecholsky Jr JJ,
                   tension loaded at a crosshead speed of 1 mm/min (≥ 10 MPa/s). The fracture toughness                                       Abdulhameed N. Toughness measurement in
                                                                                                                                              direct resin composites using quantitative fracto-
                   of the material was then calculated using the stress at failure and measurement of the                                     graphic analysis. Stoma Edu J. 2018;5(1):18-23.
                   crack size from fractographic analysis using SEM. Hardness (H) measurements were                                           Academic Editor: Nicoleta Ilie, Dipl. Eng,
                   taken using a Vickers pyramidal diamond indenter. Elastic modulus (E) was calculated                                       PhD, Professor, University Hospital, Ludwig-
                                                                                                                                              Maximilians-Universität München, Munich, Germany
                   from the E/H ratio using a Knoop indenter.
                   Results: The values for fracture toughness found were similar to other Bis-GMA based                                       Received: January 09 ,2018
                                                                                                                                              Revised: February 04, 2018
                   dental composites 0.5 ±0.2 MPa       . The Vickers Hardness was 509 ± 27 MPa and the                                       Acccepted: February 22, 2018
                   Knoop Hardness was 495 ± 14 MPa using 0.5 kg/30 s, while the elastic modulus was                                           Published: February 26, 2018

                   9.5 ±1.4 GPa.                                                                                                              *Corresponding author: Brendan M. Angus,
                   Conclusion: The differences found in fracture toughness between this study and                                             BS, Research Assistant, Materials Science and
                                                                                                                                              Engineering Department, College of Engineering,
                   previous published studies are most likely due to variation in technique and material.                                     University of Florida, 1724 Gale Lemerand Dr,
                                                                                                                                              Gainesville, FL 32603, USA, Tel: (561) 927-8584,
                   Quantitative fractographic analysis offers a different method to evaluate the toughness                                    e-mail: BrendanAngus@ufl.edu
                   of direct resin composites.
                                                                                                                                              Copyright: © 2018 the Editorial Council for the
                   Keywords: fracture toughness, resin composites, fractography, dental materials.                                            Stomatology Edu Journal.




                   1. Introduction                                                                    be time dependent. Under a rapid stressing rate, the
                   Dental composites are a mixture of polymers and                                    stress-strain response will be primarily linearly elastic.
                   glass particles used in dental restorations to mimic the                           Under a slow stressing rate, the stress-strain response
                   appearance and performance of teeth and are often                                  will be viscoelastic [8]. The presence of filler also has
                   used to repair damaged teeth [1]. Their mechanical                                 a high impact on the mechanical properties [9]. The
                   properties have improved over the last years and                                   greater the amount of fillers, the greater the modulus
                   consequently a lot of research has been performed to                               of elasticity. The combination of the viscous matrix
                   assess these properties and how they are affected by                               and greater modulus reinforcement leads to a tougher
                   variations in particle size, polymerization depth, and                             composite [10]. The main concern with the increase
                   viscosity [2-4].                                                                   in fracture toughness of the restorative material is
                   In one longitudinal study it was found that out of 926                             maintaining or improving the lifetime service in the oral
                   restorations investigated, 8% failed by fracture. This                             environment while maintaining the esthetic value. The
                   number increases to 18% when considering the failure                               mechanical properties of dental composites have been
                   of only resin composites restorations [5]. In a review                             highly improved in the last few years [11]. Even though
                   of prospective studies, it was found that fracture of                              there are many tests done to correlate in vitro data with
                   dental restorations is the most common cause of                                    the clinical behavior of dental composites, there still is a
                   restoration failures in the first 5 years. [6] Therefore                           need to improve these methods to be more realistic and
                   fracture toughness is a property that has received a lot                           comparable to material behavior while in service [12].
                   of attention in dental composites. Fracture toughness is                           There are several ways to measure fracture toughness
                   a property that represents the ability of some materials                           such as the single edge notch test, compact tension
                   to resist crack propagation [7]. The load continuously                             test, or double torsion test [13]. However, the tests for
                   applied in different directions with temperature and                               toughness, in almost all cases for resin composites,
                   humidity variation leads to the progressive degradation                            involve large crack techniques. Resin composites mostly
                   and failure of the restoration, mainly due to the crack                            fail from small cracks so it is important to develop small
                   propagation. The introduction of imperfections in the                              crack techniques to determine fracture toughness.
                   material during processing, finishing, and/or in service                           The quantitative fractography method offers the
                   has a high impact on the restoration failure probability.                          advantage of using flaw sizes of those encountered
                   The organic matrix of dental composites has viscoelastic                           in service, i.e., small cracks. There are two approaches
                   properties, which means that the response to stress will                           when using fractographic procedures to determine



   18                                                                                Stoma Edu J. 2018;5(1): 18-23.                       http://www.stomaeduj.com
                                                        TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
                                                                                                   FRACTOGRAPHIC ANALYSIS


toughness: controlled crack techniques [14] and direct




                                                                                                                                                            Original Article
observation of “natural” flaws or cracks [15]. “Natural”                                                                          (1)
here means cracks or processing defects caused by                              where A is the cross section within the narrow region
fabrication and handling of the material before testing.                       (gauge section) of the specimen (3 mm). Any sample
It was not possible to develop controlled cracks in the                        that did not break in the narrow cross section was
material so the controlled crack technique could not                           discarded and not used for the data presented. Weibull
be used. This result of difficulty in forming controlled                       parameters were calculated by maximum likelihood
cracks agrees with a similar observation in a previous                         estimation according to ASTM C1239 – 13[18].
study by other authors [16]. Using the “natural” crack
means that an assessment of the fracture toughness                              Table 1. Composition and physical properties of the Tetric Evoceram
of the material as used in clinical practice can be                            Dental Composite.
found. Finishing operations will yield cracks of size                                              Standard – Composition (in weight %)
on the order of “natural” cracks. The advantage of this
                                                                                   Bis-GMA, Urethane dimethacrylate, Ethoxylated Bis-EMA        16.8
technique over others is that it provides a tool for
forensic analysis. Once the toughness is determined                                Barium glass filler, Ytterbium trifluoride, Mixed oxide      48.5
from flaws of the size considered in this work, any                                Prepolymers                                                  34.0
strength from field failures of the same material will be                          Aditives                                                       0.4
able to be determined.
                                                                                   Catalysts and Stabilizers                                      0.3
There are limited studies in the field of dental
composites using quantitative fractographic analysis.                              Pigments                                                     <0.1
Therefore, the aim of the study was to outline a                                                                Physical Properties
procedure to determine the fracture toughness of                                   Flexural Strength (Mpa)                                       120
direct resin composites failing from “natural” flaws. The
                                                                                   Flexural Modulus (Mpa)                                     10,000
materials used in this study are compared to those
in analogous studies using different materials and                                 Compressive Strength (Mpa)                                    250
fabrication techniques.                                                            Vickers Hardness HV 0.5/30 (Mpa)                              580
                                                                                   Density (g/cm3)                                              2.10

2. Methodology                                                                 Fracture toughness was calculated using the
The material used in this study was a hybrid                                   quantitative fractographic analysis. The method uses
conventional dental composite (Tetric EvoCeram,                                optical and scanning electron microscopy to locate and
Ivoclar Vivadent)1. The Tetric EvoCeram composite is a                         measure the size of the origin of the fracture for each
light cured resin composite. The standard composition                          specimen [13]. Once the flaw, or crack, at the origin
and physical properties of Tetric EvoCeram are listed                          starts to propagate it travels with increasing speed
in Table 1 as given by the manufacturer [17]. Tensile                          spreading out in all directions. As the speed increases,
“hour glass” samples with average cross-sectional                              the surface increases in roughness. The origin of the
dimensions of 1.76 mm by 1.51 mm and a 3 mm gauge                              fracture can be determined by the observation of
length were made by filling a mold with the resin and                          the characteristic markings surrounding the fracture
curing the samples for 10 seconds each. The mold was                           origin on the fracture surface. Generally surrounding
covered with a thin Mylar strip to ensure a flat surface.                      the fracture origin there is a relatively smooth region,
The curing process was done using an LED light curing                          sometimes called the “mirror” region, that transitions
unit (Bluephase Style, Ivoclar Vivadent) which emits                           to a slightly rougher region, sometimes termed the
light with an approximate intensity of 1000 mW/cm2.                            “mist” region. These regions and other markings, such
The light cure unit was calibrated prior to use by means                       as twist hackle, can be used to identify the location of
of a dental radiometer (BluePhase meter II, Ivoclar                            the failure origin [13, 15]. The fracture origin is situated
Vivadent). The tip of the light cure unit was positioned                       approximately at the center of the surrounding
directly on top of the Mylar strip and stabilized with                         topography. All surface cracks were treated as elliptical
the plastic tip. Once the samples were cured they were                         cracks for calculating the fracture toughness. Images
polished with very light pressure to ensure that the                           were taken using a scanning electron micrograph
corners were smooth. This was done using Sof-Lex2                              SEM4. Once the crack sizes were obtained the fracture
extra thin polishing discs of medium grit followed by                          toughness was calculated using equation 2 where σ is the
fine grit at 6000-10000 rpm.                                                   stress at failure, a the crack size, and Y is a geometric factor
The polished samples were then broken in tension                               of loading, the crack shape, and location. Y was calculated
using a universal tensile testing machine3 loaded at a                         using the solutions of Newman and Raju for locations at
crosshead speed of 1 mm/min (≥ 10MPa/s) using an                               the surface of the crack or internal cracks [19]:
anti-torsion parallel holder, and the load at failure, P,
was recorded for each sample. The load-displacement                                                                                                   (2)
graphs were linear until there was fracture with little                        The hardness, H, was determined in a conventional
or no non-linear behavior before fracture. The fracture                        manner using a Vickers pyramidal diamond with an
stress, σ, was calculated from the load at failure and the                     indentation load of 0.5 kg at a loading and unloading
dimensions of each specimen using equation 1:                                  time of 30 s [20]. The Vickers diamond was used for
1
  Lot Number V23426, Exp. 2020-5, Ivoclar Vivadent AG, Schaan, Liechtenstein   hardness because it offers an equi-axed diamond
2
  3M, 3M Center St. Paul, MN 55144
3
  Instron, 825 University Ave, Norwood, MA, 02062                              4
                                                                                   Phenom Pro SEM, Phenom World, Eindhoven, Netherlands




Stomatology Edu Journal                                                                                                                                        19
                   TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
                   FRACTOGRAPHIC ANALYSIS

Original Article

                    Figure 1. Optical Micrograph of Knoop Indentation Demonstrating the
                   Measurement for Elastic Modulus.




                                                                                                     Figure 3. Example of a corner crack. The lines indicate the dimensions of
                                                                                                   the crack at the fracture origin.




                    Figure 2. Example of an internal crack. The arrow points to fracture origin.

                   and thus increases the number of measurements and
                   increases precision. For completeness, the Knoop
                   hardness value was also determined at 0.5 kg at a
                   loading and unloading time of 30 s.
                   The elastic modulus was determined using a technique
                   developed by Marshall [21] and Conway [22]. The
                   method used the geometry of the Knoop indenter,
                   i.e., due to the asymmetrical shape of the indenter,
                   one direction of the impression is elongated and
                   the transverse direction is considerably shortened.
                                                                                                     Figure 4. Example of a surface crack. Yellow lines indicate the width and
                   Upon loading, the geometry of the impression will be
                                                                                                   depth of the crack at the fracture origin. Black arrows indicate direction of
                   determined by the shape of the diamond (cf. Figure                              crack propagation away from the crack origin. White arrows indicate twist
                   1). Upon unloading, the shorter direction (2b*) will                            hackle marks on the fracture surface.
                   contract (2bR) due to the elasticity of the material. The
                   elongated end (2a*) will not be measurably changed                               Table 2. Average values of obtained data.
                   because of the length. Thus, the difference between the                          Physical Property                                Standard Deviation
                   original measurement of the diagonals (from the shape
                   of the diamond) and the impression on the material                               Fracture toughness (MPa           )       0.5                         0.2
                   will provide a measure of the elasticity of the material.
                                                                                                    Vickers Hardness (MPa)                   509                           27
                   The E/H ratio can be calculated from the measurement
                   of the diagonals as shown in equation 3 [22]:                                    Y (geometric constant)                  1.28                         0.04
                                                                                                    Elastic Modulus (GPa)                      10                         1.7
                   		                                                                        (3)                                              90% Confidence Interval
                                                                                                    Unbiased Weibull Modulus                  4.4                   3.4 - 5.6
                   where H is the Knoop hardness, ν is Poisson’s ratio (0.3),
                   γ = 75 (the average half angle of the Knoop indenter),                           Characteristic Strength (MPa)              26                     24 - 28
                   b* is half the minor diagonal at maximum load, and bR
                   is half the residual minor diagonal that is measured. The                       7.11a*, where a* is half the major diagonal, assumed to
                   value of b* can be calculated for the Knoop indenter                            be the same before and after indentation.
                   because it is related to the major diameter, i.e., b* =



   20                                                                              Stoma Edu J. 2018;5(1): 18-23.                     http://www.stomaeduj.com
                                  TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
                                                                             FRACTOGRAPHIC ANALYSIS




                                                                                                                               Original Article
3. Results
The average values of toughness, hardness, Y, elastic
modulus, Weibull modulus, and characteristic strength
can be found in Table 2. The detailed strength and
toughness data obtained are presented in Table A-1
in the Appendix. The average fracture toughness for
this material was found to be 0.5 ± 0.2 MPa . Of the
30 samples investigated, most cracks originated at
the surface of the material, often at a corner that was
polished. Only 3 of the 30 samples had internal crack
origins. An example of an internal origin is shown in
Figure 2. Figures 3 and 4 show the more common edge
and corner cracks at the surface of the samples. They
are also representative of the measurement technique.
Figure 3 also illustrates the presence of voids in various
samples often found near crack origins. The Vickers
Hardness was 509 ± 27 MPa using 0.5 kg/30 s, while the
elastic modulus was 10 ±1.7 GPa.
A Weibull graph for the data is presented in Figure 5.
The unbiased Weibull modulus and characteristic
strength were calculated using MATLAB and found to
be 4.4 (90% confidence intervals as per [16]: 3.4 - 5.6)
and 26 MPa (90% confidence intervals as per [16]: 24
MPa - 28 MPa) respectively. The locations of the fracture
origins are also depicted on the Weibull graph. All
origins appear to be uniformly distributed.                      Figure 5. Weibull graph of the composite strengths.

                                                                26] and determination of toughness values for resin
4. Discussion                                                   composites [27, 28], to our knowledge there is no record
While the values for fracture toughness could not be            of toughness values for direct resin composites measured
found from the manufacturer, the value obtained agrees          using the quantitative fractographic technique used
with other Bis-GMA based dental resin composites [23].          here. Thus, we provide useful information for use in in
Our value is less than the value of 1.11 MPa found by           vitro analysis because the size of the cracks are those
Cho et al. for the same material [24] and less than the         expected in clinical failures. The results here and from
value of 1.1 MPa        found by Quinn et al. for materials     Quinn et al. suggest that the fractographic technique
that are resin based, but manufactured in a different way       may be used to determine differences in manufacturing
[16]. Note that a different technique was used by Cho et        techniques as well as differences in particle loading.
al. to measure the fracture toughness. The notched bend         Further research in this area should be pursued.
test is noted for producing increased values of fracture        The unbiased Weibull modulus was 4 for this specific
toughness unless the notch is artificially sharpened [13].      material, which is less than the value of 8 found by
In the present study, as well as the one in Quinn et al., we    Quinn et al. for their material [16]. Of course, the Weibull
were not able to produce a sharp crack artificially due to      modulus is just an indication of the distribution of the
the viscoelastic nature of the material [16]. The condition     values of strength obtained. This distribution is related
at the crack tip can explain the difference in the              to the uniformity of the flaws in the material which,
numerical values between the notched bend test and              in turn, is related to manufacturing procedures and
the “natural” flaws. The material used in Quinn et al. [16]     handling. Thus, both values found in the two studies
is an indirect resin composite block (Paradigm, 3M ESPE,        are relatively low, indicating a wide spread of flaw sizes
MN) used for indirect restorations. The composition of          and locations. As observed in the Weibull graph, there
the indirect material used in their research contains a         does not appear to be an effect of the location of flaws
high fraction of filler particles (85 wt% ultrafine zirconia-   as to the strength of the material. The characteristic
silica ceramic to reinforce a highly crosslinked polymeric      strength was 26 ± 2 MPa. Since the fracture initiating
matrix). Thus, as the authors state, this material is closer    flaws were “natural”, they were not controlled except by
to ceramic behavior. The materials used in this research        the fabrication and finishing procedure. The sizes should
is a direct dental composite material which contains 40-        be comparable to those observed in clinical procedures.
48 wt% Baria-aluminosilicate glass filler as well as 34.0%      Better control of the fabrication procedures could result
pre-polymer fillers. In addition, the sample preparation        in greater toughness values, but most likely not greater
was different in the two studies. The present study used        than ~ 1 MPa , and thus, in greater strengths for the
a prefabricated mold followed by a light cure and then          same size flaws.
shaped for tensile specimens, while in the Quinn et al.         The method used to determine the elastic modulus in
article, a hard block was used and it was sectioned to          this work is relatively straightforward and unique for
get the desired shape for flexural tests. Thus, we should       resin composites. Since the value agrees with the value
not expect the values to be comparable. While there             provided by the manufacturer for flexural modulus,
are many fractographic studies of resin composites [25,         we think this is encouraging in that this presents



Stomatology Edu Journal                                                                                                           21
                   TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
                   FRACTOGRAPHIC ANALYSIS


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   22                                                                        Stoma Edu J. 2018;5(1): 18-23                  http://www.stomaeduj.com
                                 TOUGHNESS MEASUREMENT IN DIRECT RESIN COMPOSITES USING QUANTITATIVE
                                                                            FRACTOGRAPHIC ANALYSIS




                                                                                                                              Original Article
                                                                             Brendan M. ANGUS
                                                                                BS, Research Assistant
                                                        Materials Science and Engineering Department
                                                          College of Engineering, University of Florida
                                                                                   Gainesville, FL, USA



CV
Brendan Angus is a Masters Student at the University of Florida pursuing a degree in Materials Science and Engineering. He
earned his Bachelor’s degree in Materials Science and Engineering at the University of Florida in May of 2017. His research
focuses on the fractography of dental composites.




Questions
1. The fracture toughness of the resin composites was measured using:
qa.      Single edge notch test;
qb.      Compact tension test;
qc.      Quantitative fractography;
qd.      Double torsion test.

2. The elastic modulus was calculated using:
qa.      The slope of the stress-strain curve;
qb.      The sonic modulus technique;
qc.      Knoop indentation;
qd.      Vickers indentation.

3. The value for the fracture toughness found was:
qa.      In agreement with comparable studies;
qb.      Lower than values found in comparable studies;
qc.      Greater than values found in comparable studies;
qd.      Not compared to values found in other studies.
4. Quantitative fractography uses what measurements to calculate fracture
toughness?
qa.      Crack size and stress at failure;
qb.      Crack size and elastic modulus;
qc.      Elastic modulus and stress at failure;
qd.      Stress at failure and Vickers hardness.




                              http://prosthodontics.conferenceseries.com/scientific-program




Stomatology Edu Journal                                                                                                          23