Construction and Building Materials 94 (2015) 83–89

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Construction and Building Materials

journal homepage: www.elsevier.com/locate/conbuildmat

Implications of physico–chemical interactions in asphalt mastics on

asphalt microstructure
Chelsea Davis 1, Cassie Castorena ⇑
North Carolina State University, 2501 Stinson Dr., Raleigh, NC 27695, United States

h i g h l i g h t s

 Asphalt mastics are evaluated using Atomic Force Microscopy.

 Physico–chemical interactions in mastics alter asphalt morphology.
 Filler specific surface area affects extent of physico–chemical interaction.
 Physico–chemical interactions alter asphalt mastic rheology.

a r t i c l e i n f o a b s t r a c t

Article history: Asphalt binder and filler blend to form asphalt mastic, which constitutes the effective adhesive film in
Received 7 January 2015 asphalt concrete. Pavement performance can be improved through better engineering of the mastic,
Received in revised form 10 June 2015 which requires a fundamental understanding of the interaction between asphalt and filler. Physico–
Accepted 12 June 2015
chemical interactions result in adsorption of polar fractions of the asphalt onto filler surfaces, leading
to the formation of an interphase layer on the surface of particles and modifying the asphalt binder
matrix. This study seeks to investigate the effects of physico–chemical interaction on binder matrix
Keywords:
microstructure using Atomic Force Microscopy (AFM) and qualitatively relate microstructural findings
Asphalt
Mastic
to macroscopic rheology.
Physico–chemical interaction Ó 2015 Elsevier Ltd. All rights reserved.
Microstructure
Atomic Force Microscopy

1. Introduction fracture resistance, and moisture susceptibility of asphalt concrete

Asphalt concrete is a composite material consisting of aggre-
gates of varying size, asphalt binder, and air voids. Coarse aggre-
gates in asphalt mixtures are effectively coated by a blend of
asphalt binder and filler, termed asphalt mastic [1]. Fillers consist
of particulate matter less than 0.075 mm in diameter [2]. Fillers
used in asphalt concrete include both natural and manufactured
origins [3]. Natural fillers are the dust portion of mineral aggregate.
Manufactured fillers, on the other hand, are produced as
by-products of industrial processes (e.g., fly ash). The mastic
constitutes the weakest phase of asphalt concrete and therefore
performance of asphalt pavements is highly correlated to the prop-
erties of the mastic. It has been demonstrated that filler can signif-
icantly influence constructability, oxidative aging, stiffness,
⇑ Corresponding author.
E-mail addresses: daviscr2@email.appstate.edu (C. Davis), cahintz@ncsu.edu (C.
Castorena).
1
Address: Appalachian State University, 287 Rivers St, Boone, NC 28608, United
States.
[3]. Current Superpave asphalt concrete specifications include pro-
visions for filler only through specifying an allowable range of
mass ratios between filler and effective binder [2]. These specifica-
tions were developed based on empirical observations. While a
great deal of research has been conducted to understand the per-
formance of binders and mixtures, relatively little attention has
been given to the asphalt mastic and correspondingly, filler. An
improved understanding of the interaction between filler and
asphalt binder could lead to improved engineering and specifica-
tions of fillers in asphalt concrete and hence, improved perfor-
mance of pavements.
Various studies have shown there are three primary mecha-
nisms by which fillers reinforce asphalt binder [4–6]: volume fill-
ing, particle structuralization, and physico–chemical interactions.
Volume filling and particle structuralization are both means of
mechanical reinforcement. Volume filling increases asphalt mastic
stiffness simply as a result of the replacement of asphalt binder
volume with rigid particles. Filler particles start to form an inter-
connected network at a filler volumetric concentration of roughly

http://dx.doi.org/10.1016/j.conbuildmat.2015.06.026
0950-0618/Ó 2015 Elsevier Ltd. All rights reserved.
84 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89
40%, leading to a rapid increase in the rate of stiffening with
increasing volume fraction [6–8]. At lower filler concentrations,
particle contact is not established and the mastic will behave as
a dilute suspension, with volume filling constituting the dominant
mechanical reinforcement mechanism. The third type of reinforce-
ment, physico–chemical interaction, involves the adsorption of
polar fractions of the asphalt binder onto the surface of filler parti-
cles [5,9,10]. Physico–chemical interaction is illustrated in Fig. 1.
Physico–chemical interaction leads to formation of an interphase
adsorbed layer of the polar fractions of asphalt on the surface of fil-
ler particles. In addition, loss of certain components of the asphalt
to adsorption modifies the chemistry and morphology of the
non-adsorbed, ‘‘effective’’ binder matrix.
While mechanical reinforcement mechanisms can be readily
inferred from observed mechanical behavior, understanding phy-
sico–chemical interactions is more challenging using macroscopic
measures. Several researchers have inferred physico–chemical
interactive effects through rheological measurements coupled
with micromechanical models assumed to accurately reflect
macroscopic mastic behavior with emphasis on the thickness and
effective properties of the adsorbed layer [11,12]. Others have
inferred physico–chemical effects through thermodynamic
measures. Craus et al. [10] investigated physico–chemical
interactive effects through measuring heat release using a differen-
tial microcalorimeter. In addition, researchers have investigated
changes in glass transition temperatures between binder and mas-
tics of varying concentrations to investigate physico–chemical
interaction effects on matrix properties [5] and adsorbed
interphase layer thickness [13]. The majority of past research
efforts have focused on identifying interphase layer effects with lit-
tle consideration to the modified asphalt matrix characteristics.
Understanding the physico–chemical interaction between asphalt
and filler on the resultant asphalt matrix is critical to enable
improved design of mastics.
Asphalt is comprised of a complex, heterogeneous blend of ali-
phatic and aromatic hydrocarbons with moderate amounts of sul-
fur and trace amounts of oxygen, nitrogen, and other elements
including metals [14]. This complex chemistry gives rise to com-
posite structure in asphalt binders on the order of nanometers to
micrometers. Hence, understanding the effects of physico–chemi-
cal interaction between asphalt binder and filler on the effective
asphalt matrix properties is critical to improved engineering of
mastics. Recently, there has been significant advancement in
understanding asphalt binder microstructure through use of
Atomic Force Microscopy (AFM) [15–18]. AFM is a type of scanning
probe microscopy in which a very fine cantilever tip is rastered
across the surface of a specimen to map the distribution and prop-
erties of constituent phases. The opacity of asphalt does not lend
well to optical microscopy methods, making scanning probe
microscopy an attractive method for studying binder microstruc-
ture. Non-contact or tapping mode, where very small forces are
applied as the cantilever is rastered across a specimen’s surface,
has proven useful in studying soft materials, like asphalt, for
obtaining images of surface topography and phase contrast which
can be used to identify different microstructural phases in a mate-
rial. In addition, spectroscopy mode, in which the cantilever tip
moves vertically into a specimen rather than across its surface,
can be used to perform nanoindentation experiments for measure-
ment of stiffness and adhesive characteristics. Recent research has
shown that asphalt binders consist of a variety of microdomains
[16,17] with varying rheological properties [18].
Limited research has also been conducted to understand the
effect of filler on binder morphology using AFM. Tan and Guo
[19] used AFM to study the interaction between asphalt and filler
by preparing asphalt droplets which were placed in contact with
slices of aggregate. The relative roughness of different aggregate
surfaces along with interfacial region with asphalt was measured
using AFM. It was demonstrated that a 2–5 lm gap existed
between asphalt film and filler which the authors attributed to sur-
face tension between the filler and asphalt. In addition, nanoscale
adhesion tests were conducted which demonstrated an increase
in adhesion with addition of filler up to filler volumetric concentra-
tions ranging from 0.1 to 0.2 at which point subsequent addition of
filler resulted in a decrease in adhesion. However, no AFM experi-
ments were conducted directly on asphalt mastics. Nazzal et al.
[20] studied the dispersion of nanoclay modifiers in asphalt binder
using AFM, which the authors concluded indicated the nanoclay
was well dispersed within the asphalt. Despite no observed differ-
ences in morphology, the inclusion of the nanoclay significantly
altered the adhesive forces of asphalt materials based on nanoin-
dentation experiments. Nanoclay dosages studied were 2% and
4% by weight of binder, which is substantially lower than typical
filler concentrations in asphalt mastics. Also, nanoclay particles
are much finer than typical mineral fillers and thus, further study
of morphology implications of fillers on asphalt binders is needed.
This study seeks to investigate the effects of physico–chemical
interaction between asphalt and filler on ‘‘effective’’ binder matrix
microstructure using AFM and qualitatively relate microstructural
findings to macroscopic rheology.
2. Materials and methods
2.1. Materials
An unmodified binder with a PG grade of 64–22 was used in this study. The bin-
der was mixed with three different fillers: granite, Portland cement (PC), and
hydrated lime to produce mastics. The granite is a natural filler whereas PC and
hydrated lime are both manufactured fillers. The specific gravity and specific sur-
face area (SSA) of each filler are presented in Table 1. Specific surface area was mea-
sured using a Quantachrome Monosorb single-point BET surface area analyzer. The
Brunauer–Emmett–Teller (BET) theory was used as the analysis technique for SSA
measurements. Specific surface area is an important factor governing physico–
chemical interaction intensity as greater specific surface areas indicate greater
opportunity for adsorption [5]. Each filler was blended with binder at a volumetric
concentration of approximately 24%, leading to dust to binder mass ratios ranging
from 0.8 to 1.0, within the specified range in Superpave mix design specifications
[2]. Use of higher concentrations was avoided to minimize reinforcement by
particle-to-particle contact which becomes most prevalent at volume concentra-
tions greater than 40% [6,7].
All of the mastics in this study were mixed with a laboratory stand mixer with
supplemental hand mixing to initially agitate mastics. Before mixing, the binder
and filler were heated at 150 °C for 30 min and then poured into pre-weighed
pint-sized containers. The binder was then transferred to a hot plate to keep the
binder fluid during mixing. The oven-heated filler was slowly poured into the bin-
der while agitating. The mastic containers were then covered to avoid dust contam-
ination and allowed to cool at room temperature. In order to prevent variations in
thermal history the binder sample source was also placed in the oven at 150 °C for
30 min prior to creating test specimens.
2.2. Experimental methods
Each mastic as well as the bulk binder was tested using the Dynamic Shear
Rheometer (DSR) to determine rheological properties. In addition, AFM in
Tapping Mode to investigate microstructural implications of physico–chemical
interactions between filler and binder on the effective binder matrix.
2.2.1. Dynamic Shear Rheometer
Rheological properties of each binder and mastic sample were determined
using an ARG-2 Dynamic Shear Rheometer (DSR) from TA Instruments. Frequency
sweep tests at multiple temperatures were used to generate the dynamic shear
modulus master curve for all binders and mastics. The frequency sweep test applies
cyclic strain at constant amplitude over a range of loading frequencies and temper-
atures. Loading was applied at frequencies ranging from 0.15 Hz to 25 Hz. The fre-
quency sweeps in this experiment were run at 64, 50, 35, 20, and 5 °C. The 8 mm
parallel plate DSR geometry was used for test temperatures of 5, 20, and 35 °C
whereas the 25 mm parallel plate geometry was utilized for testing at 50 and
64 °C. Time–temperature superposition was utilized to construct dynamic shear
modulus master curves.
 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89
Fig. 1. Physico–chemical interaction in asphalt mastics.
Table 1
Filler properties.
Filler type Specific gravity Specific surface area (m2/g)
Baghouse fines (Granite) 2.58 1.639
Portland cement dust 3.15 2.240
Lime 2.30 14.408
2.2.2. Atomic Force Microscopy
To prepare AFM test samples, the binder or mastic was poured into a Pyrex Petri
dish to produce a thickness of approximately 5 mm. Samples were covered and then
stored at room temperature for 24 h prior to testing to allow the sample to anneal,
allowing for the microstructure to form as suggested by Fischer et al. (2013).
A Veeco D3000 Scanning Tip AFM (Fig. 2) with a wafer stage was used in
Tapping Mode to gather height (topographic) and phase contrast images in this
study. In Tapping Mode, the cantilever is oscillated at its resonant frequency. A
piezo drive is altered using feedback control to maintain a constant tip to sample
spacing, termed set point. The amplitude of the resultant oscillation varies with
changes in surface domains, which are converted into a false color image depicting
various heights as a function planar position. In addition, the phase lag between the
piezo signal and cantilever response will vary with surface features and can also be
used to construct a map of surface variations.
In this study, each sample was scanned at three different surface locations. In
addition, multiple samples were scanned to ensure results were representative of
the material. The scanning area at each location was constant at 25 lm by
25 lm. A single crystal silicon cantilever probe with a resonance frequency of
325 kHz and force constant of 40 N/m was used for each sample based on recom-
mendations by Fischer et al. [21]. A scanning rate of 1 Hz and speed of 2 lm per sec-
ond were utilized. The initial data scale for the height image was set to 100 nm and
phase image data scale set to 40° but subject to adjustment based on the range of
roughness of the sample surface. Once all the initial parameters were set, the sur-
face and tip were located and scanning was initiated. The parameters were adjusted
until a clear and detailed image was output. Nanoscope III software was used in
order to view and process images.
Images indicated probing of the binder phase in all samples (i.e., no filler parti-
cles) as all filler particles were coated with asphalt binder. This observation will be
further discussed later. It should be noted that a small amount of filler settlement is
expected and hence, the filler concentration at the surface of the mastics may not be
representative of the bulk volume of the mastic. However, since each mastic sample
experienced the same thermal and storage history, settlement effects are assumed
to be similar among samples.
Qualitative comparison between AFM images from different mastics and bin-
der were used to assess the effects of physico–chemical interaction on effective
binder microstructure. In order to quantify the phase images for further compar-
ison, a combined Matlab – Photoshop CS5 protocol was developed to identify the
relative area of AFM images comprised of the different microdomains. In all
specimens (both mastic and binder) evaluated, three distinct microdomains were
observed, which have also been observed in many asphalts in past studies [16–
18]. These microdomains are termed the Catana (or ‘‘bee’’ phase), the Periphase,
and the Paraphase [16] and are illustrated in Fig. 3. Note that other microdo-
mains have been observed in asphalt binders as well [16,18] but were not pre-
sent in the binder utilized in this study. The ‘‘bee’’ features have been given a
significant amount of attention in past investigations. Pauli et al. [17] demon-
strated that the ‘‘bees’’ form a result of wax crystallization, and are contained
within the saturate and naphthene aromatic fractions of binder. Das et al. [22]
demonstrated that the wax crystallization plays a critical role in fracture resis-
tance as fractures tend to initiate and propagate at the interface between
85
microdomains. In addition, Allen et al. [18] studied the microrheology of the
three microdomains and demonstrated that the paraphase is the stiffest phase
and the periphase is the softests with the ‘‘bee’’ phase having intermediate stiff-
ness and that the stiffness of the periphase and paraphase.
The image processing protocol developed calculated the relative proportion of
each microdomain in terms of area occupied. This was accomplished by isolating
the different microdomains based on color and determining the relative number
of pixels each microdomain occupied. Example output of the developed image pro-
cessing protocol is shown in Fig. 4. The ‘‘bee’’ structures are denoted by the blue
area, paraphrase by the green area, and periphase by the yellow–red area. The
developed image analysis protocol allowed for determining changes in the relative
quantities of the different microstructures as a result of adsorption on filler
surfaces.
3. Results and discussion
3.1. AFM
AFM results are presented in Fig. 5 for the base binder and the
mastics prepared with granite, PC, and lime. Note that for each
material in Fig. 5, the topographic image is shown on the left and
phase image on the right. The bright spots within the topographic
images for granite and lime mastics are speculated to correspond
to points where very fine filler particles are near the surface and
hence, a drastic change in surface topology occurs. However, phase
images on the right do not show these features, indicating they
represent the surface features of the effective binder matrix.
The images in Fig. 5 demonstrate clear identification of the
three microdomains: paraphase, periphase, and bees, previously
discussed. However, it is apparent that the relative proportion
and size of the features changes with the addition of filler and
appears to be filler specific, providing evidence of physico–chemi-
cal interaction induced changes to the effective binder matrix.
Fig. 6 displays the results of image analysis to determine the rela-
tive surface area each microdomain occupies for the materials
studied.
One notable feature in Fig. 5 is that the size decreases and rel-
ative number of bee structures increases with the addition of filler.
It can be seen that the relative change in the size, relative quantity,
and special distribution of bee features is greatest for the mastic
prepared with lime, indicating a higher degree of physico–chemi-
cal interaction intensity. This is expected since the lime filler has
a much higher specific surface area than the other fillers,
(14.408 m2/g compared to 1.639 m2/g and 2.24 m2/g for granite
and PC, respectively), and hence, given the same volume concen-
tration, provides more opportunity for adsorption. Recall, the bee
structures correspond to the crystallization of waxes and thus,
results indicate a change in wax crystallization and spatial distri-
bution with addition of filler. In addition, as polar components of
asphalt are lost to adsorption, an increase in the relative
86 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89
Fig. 2. Veeco D3000 scanning tip AFM.
Fig. 3. Asphalt binder microdomains.
concentration of waxes is expected as waxes are primarily nonpo-
lar [17]. Fig. 6 indicates a slight increase in the relative concentra-
tion of bees for the lime mastic compared to the base binder.
Results in Figs. 5 and 6 also indicate a decrease in the relative
concentration of the paraphase. Note that three replicate AFM
images were collected and analyzed for each material studied.
The largest change in the concentration of the paraphase occurs
in the lime mastic, which is consistent with expectations given
its relatively high specific surface area. However, granite has a
lower specific surface area than PC but leads to a greater reduction
in the concentration of paraphase domain so trends are not
entirely consistent and merit further investigation. No significant
change in the relative concentration of the periphase domain was
observed to occur as a result of physico–chemical interaction.
Note that based on Allen et al.’s [18] study, it was found that the
paraphase is the softest microdomain and the periphase is the stiff-
est. Thus, one might infer that a loss in paraphase concentration
would indicate an overall increase in macroscopic stiffness.
However, one also must consider that the stiffness of each phase
may change as a result of physico–chemical interaction. Changes
in the microrheology of individual microdomains upon oxidative
aging was reported by Allen et al. [18].
3.2. DSR
Dynamic shear modulus master curves for the binder and
three mastics evaluated in this study are presented in Fig. 7. It
can be seen that the mastics all demonstrate higher moduli than
the binder, as expected. It can also be observed that the different
fillers have differing stiffening effects on the binder, despite
being added to the binder in equal volumetric concentrations.
Recall, volumetric concentrations of fillers were relatively low
at 24% and hence not anticipated to lead to particle structural-
ization. Since volumetric concentrations of fillers are consistent
for all mastics, the effects of volume filling on rheology are
anticipated to be equivalent for all three filler types. Hence, dis-
crepancies in stiffening effects of different fillers can largely be
attributed to physico–chemical interaction. Trends in stiffening
effects of the fillers are consistent with microstructural observa-
tions: Lime has the greatest stiffening effect and induced the
greatest change in binder microstructure whereas granite and
PCC show lower stiffening effects (and also have much lower
SSAs). Thus, microstructural findings support the hypothesis that
differences in stiffening effects can be attributed to physico–
chemical interactions. It should be noted that the effective,
non-adsorbed binder matrix is hypothesized to soften as a result
of physico–chemical interaction. Thus, the increase in stiffening
effect with increasing degree of physico–chemical interaction
indicates that the role of the adsorbed layer significantly affects
mastic rheology.
In addition to comparing the master curves of different binders
and mastic, the effect of temperature on the stiffening effect of the
fillers was also investigated through evaluating |G⁄| ratios at each
temperature of frequency sweep testing at a single loading fre-
quency of 10 Hz. |G⁄| ratios are computed as the ratio of the mastic
modulus to the base asphalt. Results are presented in Fig. 8. Results
demonstrate little change in stiffening ratios with temperature for
granite and PC mastics. However, for the lime mastic, the stiffening
ratio is found to increase with temperature, indicating potential
influence of particle structuralization, which could be induced as
a result of an increase in ‘‘effective’’ filler content due the forma-
tion of a nontrivial semi-rigid adsorbed interphase layer on filler
particles, further displaying physico–chemical interaction intensity
compared to other mastics [11].
 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89 87

Fig. 4. Illustration of image processing output.

Binder Granite Mastic

PC Mastic Lime Mastic

Fig. 5. AFM images. For each material, left image corresponds to topographic and right image corresponds to phase.

4. Conclusions & recommendations (3) Changes in binder microstructure provide an indicator of

(1) Effective (i.e., non-adsorbed) binder in mastics has signifi-
cantly different microstructure than the bulk binder as a
result of physico–chemical interactions.
(2) The extent of change in binder microstructure as a result of
physico–chemical interaction is affected by the filler specific
surface area.
physico–chemical interaction intensity. Mastics that exhib-
ited the most significant change in microstructure upon filler
addition also demonstrated the greatest change in rheology.
(4) A greater stiffening effect is observed for fillers which induce
greatest microstructural changes as a result of physico–
chemical interaction. Physico–chemical interaction is antici-
pated to lead to a softening of the effective asphalt binder
88 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89

Fig. 6. Effect of physico–chemical interaction on different microdomains.

Fig. 7. Dynamic shear modulus (|G⁄|) master curves.

Fig. 8. |G⁄| Ratios at 10 Hz loading frequency.

matrix since polar components adsorb to the surface of
the filler. Thus, results suggest the formation of adsorbed
interphase layer plays a more critical role in determining
macroscopic rheology of mastics than softening of the
binder matrix.
(5) It is should be noted that findings of this study are limited to
a single binder blended with three fillers at a single volumet-
ric concentration. It is recommended that findings be con-
firmed by studying additional binder – filler combinations
using a similar methodology. It is also recommended that
 C. Davis, C. Castorena / Construction and Building Materials 94 (2015) 83–89
nanoindentation experiments be performed to determine
the microrheology of the different binder microphases with
and without inclusion of filler to allow for improved under-
standing of the implication of physico–chemical interaction
on the rheology of the modified binder matrix. It is also
recommended that AFM imaging be conducted at varying
temperatures to investigate thermal effects on binder
morphology.
(6) The results of this study were limited to morphological and
linear viscoelastic characterization of asphalt mastics. It is
recommended that future work also address the effects of
physico–chemical interactions between asphalt binder and
filler on chemistry and molecular structure. It is also sug-
gested that performance implications of interactions
between filler and binder further be investigated with
respect to viscoplasticity, fracture resistance, and adhesion
to aggregate.
Acknowledgments
This research was funded by North Carolina State University’s
Faculty Research and Professional Development Program (FRPD).
This support is greatly appreciated.
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