Mechanics of Materials 160 (2021) 103901

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Mechanics of Materials
journal homepage: www.elsevier.com/locate/mechmat

Excluded volume and its relation to the theory of fiber-fiber contacts

Amit Rawal
Department of Textile and Fibre Engineering, Indian Institute of Technology Delhi, Hauz Khas, New Delhi, India

A R T I C L E I N F O A B S T R A C T

Keywords: Contemporary understanding of fiber-fiber contacts is vital in diversifying the applications of fiber networks.
Aspect ratio Various properties of fiber networks rely on the architecture, which essentially requires encapsulating realistic
Excluded volume features arising from excluded volume effects. Herein, an architectural-based interfiber spacing model of
Fiber network
‘generalized’ fiber networks has been proposed by combining the geometrical probability, stochastic, and
Interfiber spacing
Random
excluded volume approaches. The interfiber spacing model features the classical work of excluded volume
approach of Onsager, superimposed on Komori and Makishima’s theory of fiber-fiber contacts. The significance
of the interfiber spacing model relies on its ability to systematically demystify the anomalies in Onsager’s work
for random networks composed of exceedingly low-aspect-ratio fibers. Nevertheless, a good agreement between
the theory and experiments justified that Onsager’s excluded volume approach is sufficiently robust to predict
the interfiber spacing of moderate to high-aspect-ratio fiber networks.

1. Introduction observed as Onsager’s theory (Onsager, 1949) breakdown at a lower

In the 19th century, van der Waals employed a key concept of
excluded volume that formed the basis of generalizing the ideal gas laws.
Maxwell (1874) proliferated the work of van der Waals by describing the
free path of molecules diminished by four times the volume of the
molecules (also called as covolume or half of the excluded volume of the
sphere). In general, the excluded volume is defined as the inaccessible
volume around an object into which the center of another object is de­
nied to avoid the overlapping of the objects on the basis of their possible
center of mass positions and orientations (Balberg et al., 1984; Lazzara
et al., 2000). Over the years, the excluded volume approach has
extended beyond the spherical objects as the significance of random
packings of anisotropic entities emerged in the fields of self-assembly of
nanoparticles, colloidal rods in amorphous sediments, liquid crystals,
glasses, granular processing, fibrous media, and composites, to name a
few (Herzfeld, 1996; Williams and Philipse, 2003; van Roij, 2005;
Chaikin et al., 2006; Otten and van der Schoot, 2009; Kyrylyuk et al.,
2011; Otten and van der Schoot, 2011; Baule et al., 2013; Kale et al.,
2016; Asai et al., 2017). Particularly, the pioneering work of Onsager
(1949) underpins the importance of excluded volume of the colloidal
rods (cylinders and spherocylinders) as a function of their spatial ori­
entations. Strikingly, a first-order phase transition from an isotropic
(orientationally disordered) to a nematic (orientationally ordered)
phase occurs beyond a certain volume fraction of rods (Vroege and
Lekkerkerker, 1992; Frenkel, 2015). Notably, a discrepancy was
aspect ratio of spherocylindrical rods due to the negligence of higher
virial coefficients (Frenkel, 1987). Recently, discrete element
method-based simulations also revealed that a cusp was detected on the
packing density-aspect ratio curve, especially with rods having an aspect
ratio of unity (Gan and Yu, 2020).
Irrefutably, Onsager’s theory (Onsager, 1949) is valid for larger
aspect ratio rods (Frenkel, 1987), which means that it can be readily
applicable to textile fibers that generally have an aspect ratio of more
than 1000. Further, one of the key contributions of Onsager’s work
(Onsager, 1949) was that the excluded volume computed for the cyl­
inders or spherocylinders not only considered the surface-surface in­
teractions but the synergy with end-end and side-end contacts has been
encompassed in a holistic manner. Arguably, the surface-surface in­
teractions of large aspect ratio cylinders are pre-dominant in modulating
the excluded volume (Onsager, 1949). However, as the preferential
alignment in cylinders is augmented, the probability of intersections
with the ends of the cylinder rises simultaneously, reducing the proba­
bility of intersection with the curved surface (Ranganathan and Advani,
1991). This means that in the case of unidirectional fibers or yarns, the
end-end or the side-end intersection is a key factor that maneuvers the
number of fiber-fiber contacts.
In the field of textiles, the seminal work of van Wyk (1946) employed
the excluded area approach and predicted the number of fiber-fiber
contacts in three-dimensional (3D) random fiber networks. Subse­
quently, Komori and Makishima (1977) generalized van Wyk’s work by

E-mail address: arawal@iitd.ac.in.

https://doi.org/10.1016/j.mechmat.2021.103901
Received 21 February 2021; Received in revised form 28 April 2021; Accepted 2 May 2021
Available online 13 May 2021
0167-6636/© 2021 Elsevier Ltd. All rights reserved.
A. Rawal Mechanics of Materials 160 (2021) 103901

considering the anisotropic nature of fiber alignment. One of the key
assumptions of Komori and Makishima’s work relied upon the negli­
gence of the end-to-end or side-to-end interactions of fibers. Accord­
ingly, they consistently emphasized that their theory is not valid for
nonuniform structures that include yarns, slivers, and unidirectional
fibers (Komori and Makishima, 1977; Komori and Itoh, 1994). More­
over, Pan (1993) pointed out that there was an inherent drawback in
Komori and Makishima’s work as the reduction in the probability of
fiber‒fiber contacts with successive contacts has not been accounted.
Subsequently, Komori and Itoh (1994) criticized the modified model
(Pan, 1993) as an error was made in computing the inhibited or
forbidden length brought about by a newly formed contact. This
hand-waving discussion of the theory of fiber-fiber contacts clearly il­
lustrates that there is a need to generalize Komori and Makishima’s work
(Komori and Makishima, 1977) such that it is applicable to a diverse set
of fiber networks.
The importance of fiber-fiber contacts has also been recognized in
the field of short fiber-reinforced composites. Specifically, the prepara­
tion of short fiber-reinforced composites involves the flow of suspen­
sions comprising short fibers infused in a highly viscous fluid. With the
increase in the fiber volume fraction, the fibers flow in close proximity to
each other that affect the flow-induced fiber orientation characteristics.
Ranganathan and Advani (1991) modified Doi and Edward’s model (Doi
and Edwards, 1978) of spacing between rigid rod-like polymer mole­
cules by accounting for the cylindrical fiber ends intersected by the
surrounding fibers. Later, Toll (1993, 1998) corrected the interfiber
were either not applicable or less meaningful to the regularly packed
fiber masses, i.e., yarns or any defined set of unidirectional fibers
(Komori and Makishima, 1977; Komori and Itoh, 1994). Such ambiguity
can be overcome by combining Onsager’s excluded volume approach
(Onsager, 1949) with Komori and Makishima’s work (Komori and
Makishima, 1977). Here, it is assumed that the cylindrical fibers in the
network are of diameter D and length l. Let us consider a fiber element in
a spherical coordinate system such that the orientation of this element
can be defined uniquely by a pair of orientation angles (θ, ϕ) provided
that 0 ≤ θ ≤ π and 0 ≤ ϕ ≤ π, where, the polar and azimuthal angles, θ
and ϕ are formed with the Z and X axes, respectively. Based upon
symmetry, we have only considered half of the unit sphere, as shown in
Fig. 1A.
Considering an infinitesimal region formed on the unit sphere within
the range of θ ∼ θ + dθ and ϕ ∼ ϕ + dϕ, the area occupied by a randomly
placed fiber element would be sinθdθdϕ. In generalized fiber networks,
the probability of finding the orientation of fiber is Ω(θ, ϕ)sinθdθdϕ,
where Ω(θ, ϕ) is the orientation density function (see Fig. 1B). Appar­
ently, the following normalization condition is satisfied based upon the
fact that the sum of the area fractions covered by these fiber elements is
unity. Since half of the unit sphere is being considered, therefore
(Komori and Makishima, 1977),
∫π ∫π
Ω(θ, ϕ)sinθdθdϕ = 1 (1)
0 0

spacing model (Ranganathan and Advani, 1991) by employing the Let us now place a cylindrical fiber A having orientation (θ, ϕ) in a
excluded volume approach. Although the correction made by Toll defined volume (V), and another fiber B of same dimensions but with an
(1993, 1998) is pertinent, it did not account for the interaction of cy­ orientation (θ , ϕ ) is required to be spatially located in this volume.
′ ′

lindrical fibers similar to Onsager’s work (Onsager, 1949) by consid­ Contact between the two fibers is formed when the geometrical center of
ering all possible configurations of fiber interactions based upon the fiber B is brought into the inaccessible or excluded volume of fiber A, as
excluded volume approach. illustrated in Fig. 2. The excluded volume formed around the periphery
In this work, we construct an interfiber spacing model of generalized of cylindrical fiber A (vexcyl ), is given by Onsager (1949),
fiber networks1 by combining the geometrical probability, stochastic, ( )
and excluded volume approaches. Here, the term ‘interfiber spacing’ vcyl = 2Dl + (π/2)D |sinχ | + κlD2
ex 2 3
(2)
refers to the mean distance between the successive fiber-fiber contacts.
Accordingly, section 2 presents an interfiber spacing model for gener­ where κ = (π/2)(1 + |cosχ |) + 2E(sinχ );
[ ]1/2
alized fiber networks based upon the seminal works of Onsager (1949) sinχ = 1 − {cosθcosθ + sinθsinθ cos(ϕ − ϕ ) }2
′ ′ ′
;
and Komori and Makishima (1977) by utilizing the cylinders and
spherocylinders as geometrical entities. The presented interfiber spacing ∫ π /2 ( )1/2
model is a blueprint for a variety of textile materials and short-fiber E(sinχ ) = 1 − sin2 χ sin2 γ dγ (3)
0
reinforced composites. To the best of the author’s knowledge, this is a
first attempt to develop a generalized model that can be utilized for a where χ is the angle formed between the axes of fibers, E(sinχ ) is the
variety of fiber networks spanning several length scales. In section 3, a complete elliptic integral of the second kind.
comparison of the theoretical model with Toll’s model (Toll, 1998) has Thus, the probability that fiber B comes in contact with fiber A, p(θ,
been made for the 2D and 3D random networks comprising
ϕ; θ , ϕ ), is given by,
′ ′

low-aspect-ratio fibers. With the aid of the interfiber spacing model, this
is a first attempt to systematically demystify the anomalies in Onsager’s vex
(4)
′ ′ cyl
p(θ, ϕ; θ , ϕ ) =
work (Onsager, 1949) for random networks composed of exceedingly V
low-aspect-ratio fibers. In this regard, we extend our earlier work Using Komori and Makishima’s (Komori and Makishima, 1977)
(Kumar and Rawal, 2016) pertaining to the prediction of electrical analysis, the average number of the fibers that contact fiber A, n(θ, ϕ)
percolation threshold by combining Onsager’s work (Onsager, 1949) to based upon the fact that N (»1) fibers are present in volume V is,
determine its suitability for lower aspect ratio cylindrical nanofillers ∫π ∫π
(<10) present in a typical nanocomposite system (Yi and Choi, 1999; n(θ, ϕ) = N
′ ′ ′ ′ ′ ′
p(θ, ϕ; θ , ϕ )Ω(θ , ϕ )sinθ dθ dϕ
′
(5)
White et al., 2010). Further, a comparison has been made between the 0 0

theory and experiments based upon the architectural parameters of

where Ω(θ , ϕ ) is the orientation density function of fiber B.
′ ′

stainless-steel fiber network (Tsarouchas and Markaki, 2011).

Combining equations (2)-(5)
[( {( ) } ]
2. Interfiber spacing model )
N 2Dl2 +(π /2)D3 〈|sin χ |〉+ π2 (1+〈|cos χ |〉)+2E(〈sinχ 〉) lD2
n(θ,φ)=
Komori and colleagues consistently emphasized that their models V
(6)
where N is the number of fibers present in volume V and 〈〉 represents
1 ∫π∫π
Here, the generalized fiber networks refer to a variety of textile materials the mean value, 〈|sinχ |〉 = Ω(θ ,ϕ )|sinχ |sinθ dθ dϕ ,
′ ′ ′ ′ ′

0 0
ranging from random (nonwoven) to highly anisotropic (yarn) fibrous
assemblies.

2
A. Rawal Mechanics of Materials 160 (2021) 103901

Fig. 1. Fiber alignment in a 3D space. (A) Schematic of a fiber element occupying surface of sinθdθdϕ on a unit sphere, within the range of θ ∼ θ+ dθ and ϕ ∼ ϕ + dϕ,
where θ and ϕ are the polar and azimuthal angles, respectively in an isotropic fiber network. (B) For generalized fiber networks, the proportion of fibers that occupies
a surface of a unit sphere is Ω(θ, ϕ)sinθdθdϕ, where Ω(θ, ϕ) is the orientation density function.

∫ ∫
where |sinχ | and |cosχ | are the overall mean values of sinχ and cosχ ,
π π
′ ′ ′ ′ ′
〈|cosχ |〉 = Ω(θ , ϕ )|cosχ |sin θ dθ dϕ ∫π ∫π ∫π ∫π
0 0 respectively, i.e., |sinχ | = 0 0 〈|sinχ |〉Ω(θ, ϕ)sinθdθdϕ; |cosχ | = 0 0
By averaging n(θ, ϕ) over the possible values of θ and ϕ would yield 〈|cosχ |〉Ω(θ, ϕ)sinθdθdϕ
an expression for the average number of contacts on a given fiber n, i.e., The average number of fiber-fiber contacts per unit length of a fiber
nl can be computed, as shown below.
∫π ∫π
[( /) {( )( ) } ]
n= n(θ, ϕ)Ω(θ, ϕ)sinθdθdϕ (7) 3 π 2
n N 2Dl + (π/2)D l |sinχ | + 2 1 + |cosχ | + 2E(sinχ ) D
0 0 nl = =
l V
Or, (9)
[( {( )( ) } ]
) The mean distance between the successive contacts comprising cy­
N 2Dl2 +(π/2)D3 |sinχ |+ π2 1+|cosχ | +2E(sinχ ) lD2
n= (8) lindrical fibers, (b)Cyl can be obtained by taking the reciprocal of nl .
V

Fig. 2. Schematic of (A) end-to-end (B) side-to-end

(C) side-to-side contact being formed between the
two fibers when the geometrical center of fiber B with
orientation (θ , ϕ ) is brought into the inaccessible or
′ ′

excluded volume of fiber A having orientation (θ, ϕ).

Here, D is the fiber diameter, and χ is the angle
formed between the axes of fibers. The region created
by ‘2D’ refers to the excluded volume of fiber A
whereby a fiber-fiber contact is to be formed. Note
that the effect of fiber length l in depicting the
excluded volume is not shown schematically but it is
accounted in the calculations.

3
A. Rawal Mechanics of Materials 160 (2021) 103901

( ) 1 V (2D) random, 3D random, and unidirectional fibrous materials. In

b = = [( {( )( ) } ]
Cyl nl N 2Dl+(π/2)D3 /l )|sinχ |+ π 1+|cosχ | +2E(sinχ ) D2 addition, a comparison has been made with the corresponding expres­
2 Toll
sion of (b)Cyl obtained using Toll’s work (Toll, 1998). Table S1 shows the
(10)
magnitudes of |sinχ |, |cosχ | and E(sinχ ) for 2D random, 3D random, and
Now using the elementary definition of fiber volume fraction
( ) unidirectional fibrous materials. Here, the term ’2D random’ refers to
v
Vf = Vcyl = πND
2l
, where vcyl is the volume of the cylinder, the (b)Cyl can the isotropic orientation of fibers created in the planar or in-plane di­
4V
rection by setting θ = 2π.
be expressed as shown below.
( ) 1 πD 3. Results and discussion
b = = ⎡ {( ) }⎤ (11)
Cyl nl ( ) π
2 (1+|cosχ |)+2E(sinχ )
4Vf ⎣ 2 + 2sπ2 |sinχ | + s
⎦ In the past, the fiber volume fraction and aspect ratio curve revealed
a cusp for low-aspect-ratio cylindrical entities (Gan and Yu, 2020).
Therefore, it is pertinent to detect this anomaly in Onsager’s work
where s (=l/D) is the aspect ratio of fiber. (Onsager, 1949), which would determine its applicability on fiber net­
Also, for developing a simple analytical model, the following works specifically formed in short fiber-reinforced composites.
approximate representation for the complete elliptic integral of the (b) (b)
second kind has been adapted (Chatterjee, 2014). Fig. 3A–C shows a relationship between DCyl or DScyl , s and Vf in 2D and
[ ] 3D random fiber networks by considering constituent fibers as cylinders
1 π (4 − π ) (π2 − 2π − 4)
E(sinχ ) ≈ + |sinχ | + π(π − 3)|cosχ | (12) and spherocylinders. There is a marginal difference between DCyl ob­
(b)
π− 2 2 2
tained via Toll’s model (Toll, 1998) and presented work, as shown in
Or, Fig. 3(A) and (B). For lower magnitudes of Vf , both models reveal that
1
[
π (4 − π ) (π2 − 2π − 4)
] number of contacts formed on a given fiber would be significantly higher
E(sinχ ) ≈ + |sinχ | + π(π − 3)|cosχ | (13) in 3D random fiber networks than the corresponding 2D random fiber
π− 2 2 2
network. Similar trends have emerged in 2D random and 3D random
Similarly, the expression of the mean distance between the succes­ networks comprising fibers with spherocylinder geometry, as depicted
( )
sive contacts, b has been obtained by considering the fibers as in Fig. 3 (C).
Scyl
( ) In general, the low-aspect-ratio fibers may tend to form a strong
spherocylinders of diameter D, length l, and volume vScyl = πD6 + πD4 l .
3 2
preferential or pseudo-unidirectional fiber network, which is similar to a
first-order phase transition from isotropic to nematic phase that occurs
In this case, the excluded volume formed around the periphery of beyond a certain volume fraction of rods or short cylinders in discotic
spherocylinders also referred to as capped cylinders by Onsager (1949), suspensions (Vroege and Lekkerkerker, 1992; Frenkel, 2015; Mejia
( )
4 et al., 2012). This is also similar to the unidirectional composites,
vex
Scyl = πD3 + 2πD2 l + 2Dl2 |sinχ | (14) whereby the carbon fibers (CF) with a low aspect ratio (~6) have
3
attained significant high volume fractions (>50%) (Qu and Schubert,
Now applying the same formulation strategy that has been used for 2016). It is worth mentioning that extremely low aspect ratio (s ∼ 1)
deriving the mean distance between the successive contacts comprising fibers approach the geometry of the plate-like particles. In such a sce­
cylindrical fibers. Therefore, nario, Onsager (1949) made a brilliant comment “Where plate-like
( ) particles are concerned, our approximations will introduce more
( ) D 1 + 3s2 serious errors, and we can hardly hope for more than that our result will
b = ( ) (15) describe concentrated solutions of such particles qualitatively rather
Scyl
8Vf 2
3s2
+ 1s + |sinπ χ | than quantitatively.” Thus, exceedingly low-aspect-ratio fibers would
introduce appreciable errors, which is also evident by considering
various combinations of aspect ratio and fiber volume fractions leading
Table 1 shows the expression of (b)Cyl and (b)scyl for two-dimensional

Table 1
Expressions of the mean distance between the successive fiber-fiber contacts and critical volume fractions for 2D random, 3D random, and unidirectional fibrous
materials.
Parameter 2D Random 3D Random Unidirectional

(b)Cyl D D sD
[ ] [ ]
4 1 (π3 − 20π2 + 36π + 16) π (π + 3) 8Vf
4Vf 2 + 2 + Vf 2+ 2 +
π πs 2π (2 − π)s
2 2s s
Toll D D sD
(b)Cyl [ ] [ ]
4
(π + 2) 3 8Vf
4Vf 2 + 2Vf 1 +
π πs s
( ) ( ) ( )
b 2 2 sD
D 1+ D 1+
Scyl 3s 3s 8Vf
[ ] [ ]
2 1 2 1 1 2
8Vf 2 + + 2 8Vf + + 2
π s 3s 4 s 3s
(Vfc )Cyl 1 1 0.174
[ ] [ ]
4
1 (π3 − 20π2 + 36π + 16) π (π + 3)
2.88s + + 0.72s 2 + 2 +
π π s2
2 2π2 (2 − π)s 2s s
( ) ( )
(Vfc )Scyl 2 2 0.174
1+ 1+
3s 3s
[ ] [ ]
2 1 2 1 1 2
5.76s 2 + + 2 5.76s + + 2
π s 3s 4 s 3s

4
A. Rawal Mechanics of Materials 160 (2021) 103901

Fig. 3. Relationship between fiber and architectural parameters of fiber networks. For a range of Vf in (A) 2D random and (B) 3D random cylindrical fiber networks,
Toll

has been computed under the defined magnitudes of s. A comparison has also been made with the corresponding results of obtained via Toll’s model (Toll,
(b)Cyl (b)Cyl
D D

1998). (C) vs. s for a range of Vf in 2D random and 3D random networks comprising fibers with spherocylinder geometry. (D) Comparison between the
(b)Scyl
D
theoretical and experimental results of (Vfc )Cyl by considering 2D random and 3D random cylindrical fiber networks. Here, a comparison has been made between the
theory and the experimental data of low-aspect-ratio carbon fibers (Yi and Choi, 1999) in addition to the simulation and experimental results of well-dispersed silver
nanowires in nanocomposites (White et al., 2010). The theoretical values have been computed based upon the expressions provided in Table 1 for 2D and 3D random
fiber networks.

reasonable agreement between theory and experiments. However, a

to DCyl or DScyl <1 for 2D and 3D random networks. For example, in the
(b) (b)
poor agreement has been observed between the (Vfc )Cyl obtained via
case of 2D and 3D random networks comprising cylinders or spherocy­
theory and experimental work of Yi and Choi (1999). Inevitably, large
linders with s=4 and Vf=0.3, yielded DCyl or DScyl <1. To further analyze
(b) (b)
variation in determining the aspect-ratio of carbon fibers was observed,
Onsager’s work, we identified lower aspect ratio cylindrical nanofillers for example, the measured average aspect ratios (±standard deviations)
(<10) present in a typical nanocomposite system and revisited our were 4.0 (±2.1), 6.9 (±3.2), 8.9 (±4.9) and 10.3 (±6.1) (Yi and Choi,
previous work based upon the interfiber spacing model (Kumar and 1999). Nevertheless, a good agreement between the theoretical results
Rawal, 2016). of 2D random networks comprising low-aspect-ratio fillers and simula­
Previously, we formulated a percolation threshold concept such that tion results of White et al. (2010) was observed, whereas the simulation
the critical volume fraction of cylinders and spherocylinders, (Vfc )Cyl and results converged with 3D random networks for high-aspect-ratio fillers.
(Vfc )Scyl , respectively are realized when percolation probability is 50% Vf and s also have a significant effect on the coordination number z or
the number of touching neighbors per cylindrical fiber. In this study, the
that led to lCyl or lScyl of 0.72 (Kumar and Rawal, 2016; Zheng et al.,
(b) (b)
z can simply be computed as nl that leads to,
2007). Accordingly, various expressions of (Vfc )Cyl and (Vfc )Scyl have been ⎡ {( )( ) l }⎤
4 ( ) π
2 1 + |cosχ | + 2E(sinχ )
provided for 2D random, 3D random and unidirectional fiber networks, π
z = Vf s⎣ 2 + 2 |sinχ | + ⎦ by rear­
as shown in Table 1. Subsequently, we compared the simulation and π 2s s
experimental results of the percolation threshold of carbon fibers (Yi and ranging equation (11). For 3D random networks that have constituent
Choi, 1999) and fairly well-dispersed silver nanowires (White et al., fibers with s≫1, z = 2Vf s, which matches with the expression derived
2010) with aspect ratios varying between 4 and 31. Fig. 3D shows a earlier (Blouwolff and Fraden, 2006). Similarly, z = 16
π2 Vf s for 2D random

5
A. Rawal
method employed in the 3D reconstructed structure obtained via the X-ray nCT technique (Tsarouchas and Markaki, 2011).
fiber networks that have constituent fibers with s≫1. But now the
question arises whether the expression of z holds for short rods and
disks? Blouwolff and Fraden (2006) experimentally observed that the
random contact model (RCM) formulating a relationship between z, Vf ,
vex
cyl and vcyl was not followed for short rods and disks. This again poses a
question on the validity of Onsager’s work (Onsager, 1949) for
( )
extremely low-aspect-ratio fibers. Nevertheless, as s→ ∞, b =
Cyl
( ) ( )Toll
b = b = πD , which matches well with the expression
scyl Cyl 8Vf |sinχ |
deduced by Komori and Makishima (1977). For 3D random network,
Toll D
|sinχ | = 4π , thus, (b)Cyl = (b)scyl = (b)Cyl = 2V f
= π2V
DL, which matches well
with the expression deduced by van Wyk (1946). Here, L (=Nl) is the
total length of fibers in volume V. In this research work, the fiber seg­
ments are considered to be straight, it is anticipated that the waviness is
a function of change of local fiber orientation. Accordingly, the waviness
in the fiber is implicitly in-built via the assembly of tangent lines at all
points on the fiber axes, computed through global orientation parame­
ters, i.e., |sinχ | and |cosχ | (Komori and Makishima, 1977). This is the
reason that Komori and Makishima (1977) inferred that the number of
contacts per unit length remains unaffected by the fibers that are bent or
possess waviness. Future research directions should address the effect of
the degree of fiber waviness on the inter-fiber spacing by comparing
with experiments and other modeling approaches (Drozdov et al.,
2020).
Next, we validate the interfiber spacing model by comparing the
theoretical results with the experimental data of the stainless steel
network made-up of relatively high-aspect-ratio fibers (Tsarouchas and
Markaki, 2011). For validation purposes, we utilized the architectural
parameters of the ferritic stainless-steel fiber network, which were ob­
tained using the X-ray micro-computed tomography (microCT) tech­
nique and then compared with the X-ray nano-computed tomography
(nCT) analysis based upon a variety of image analysis techniques
(Tsarouchas and Markaki, 2011). Tsarouchas and Markaki (2011)
applied various image analysis methods, including global thresholding,
a combination of anisotropic diffusion and global thresholding, and that
of deconvolution and local thresholding, for analyzing the architectural
parameters using the X-ray microCT technique. Subsequently, the ob­
tained results were benchmarked against the local thresholding method
employed in the 3D reconstructed structure obtained via the X-ray nCT
technique. Tsarouchas and Markaki (2011) critically analyzed each of
the image analysis techniques that led to a variation in the determina­
tion of fiber volume fraction, fiber orientation distributions, fiber
diameter and mean distance between the contacts. Although Tsarouchas
and Markaki (2011) claimed that the stainless steel fiber network
6
Mechanics of Materials 160 (2021) 103901
Fig. 4. Mean distance between the contacts in the
stainless steel fiber network. (A) Hypothesized
anisotropic fiber orientation distribution in the
stainless steel fiber network. (B) Comparison between
the theoretical and experimental values (Tsarouchas
and Markaki, 2011) of the mean distance between the
contacts in stainless steel fiber network with hy­
pothesized anisotropic and 2D random fiber orienta­
tion distributions. Here, the theoretical values are
predicted based upon hypothesized anisotropic fiber
orientation distribution. The experimental values of
the mean distance between the contacts have been
obtained via global thresholding (GT), a combination
of anisotropic diffusion and global thresholding (AD
+ GT), and deconvolution and local thresholding (DC
+ LT) using the X-ray microCT technique (Tsarouchas
and Markaki, 2011). In addition, these values were
benchmarked against the local thresholding (LT)
Fig. 5. DCyl of twisted yarn as a function of helix angle, q at s = 1000. A
(b)
comparison has also been made with the corresponding theoretical results of
Pan (1993).
possesses a 2D random structure, it was not clearly evident from the
in-plane stereographic projections using various image analysis
methods. Further, the in-plane stiffness predicted on the basis of
anisotropic2 fiber orientation distribution obtained via the global
thresholding method appears to correlate well with the experimental
results than any other image analysis method (Tsarouchas and Markaki,
2011). Therefore, the anisotropic in-plane fiber orientation distribution
has been hypothesized (see Fig. 4A), and the mean distance between the
contacts was predicted using Eq. (11) on the basis of fiber and archi­
tectural parameters obtained via various image analysis methods
(Tsarouchas and Markaki, 2011), as depicted in Fig. 4B. Table S2 shows
the values of various fiber and structural parameters, which have been
used to predict the mean distance between the contacts in stainless steel
networks. Intriguingly, a good agreement has been obtained between
the theory and experiments by considering the anisotropic fiber
network. Hypothesizing the 2D random fiber network has resulted in a
poor agreement between the theory and experiments. Nonetheless, the
2
Tsarouchas and Markaki (2011) claimed that the material is transversely
isotropic (planar random) when the points are clustered around the periphery
of the stereogram. However, this was not clearly visible for the stereograms of
fiber orientation distributions obtained via the global thresholding, a combi­
nation of anisotropic diffusion and global thresholding, and that of deconvo­
lution and local thresholding methods.
A. Rawal
preferentially aligned fiber network yielded the mean distance between
the contacts that corroborated well with the magnitudes obtained using
all the image analysis methods.
Leveraging the preferential fiber alignment often enhances the
probability of end-end intersections by concurrently reducing the
probability of intersection with the curved surface (Ranganathan and
Advani, 1991). A typical example is a twisted yarn comprising
high-aspect-ratio fibers assembled in a helical direction. Thus, a com­
parison of has been made between the present work and a theo­
(b)Cyl
D Asai, M., Zhao, D., Kumar, S.K., 2017. Role of grafting mechanism on the polymer
retical model developed earlier (Pan, 1993), as depicted in Fig. 5 (see
supplementary information for details).
For a range of Vf , the magnitude of DCyl is overestimated using Pan’s
(b)
work (Pan, 1993), especially for low-twisted yarns possessing low helix
angle (q). In the future, a comparison can be made between the theo­
retical and experimental results of (b)Cyl in twisted yarns possessing a
variety of helix angles. Nevertheless, the present work has clearly
demonstrated that the excluded volume approach evolved from Ons­
ager’s work (Onsager, 1949) has great potential in a variety of fiber
networks.
4. Conclusions
In this research work, an interfiber spacing model of generalized
fiber networks has been proposed that encapsulated the seminal works
of Onsager (1949) and Komori and Makishima (1977) by utilizing the
cylinders and spherocylinders as geometrical entities. The proposed
model has been validated with the architectural parameters of a
stainless-steel fiber network, which were obtained using various image
analysis methods (Tsarouchas and Markaki, 2011). A good agreement
has been obtained between the theory and experiments by hypothesiz­
ing the anisotropic fiber network. Further, we revealed that the previ­
ously developed model (Pan, 1993) had overestimated the interfiber
spacing in a low-twisted yarn. Categorically, we demystified the
breakdown of Onsager’s work (Onsager, 1949) by identifying the
anomalies in predicting the interfiber spacing of random networks made
up of exceptionally low-aspect-ratio fibers. Nevertheless, Onsager’s
work is sufficiently robust to predict the percolation threshold
comprising cylindrical nanofillers with aspect ratios as low as 8 (White
et al., 2010). Altogether, our findings illustrated the importance of
Onsager’s work, which remains obscure in the field of textile and allied
materials. Particularly, Onsager’s work (Onsager, 1949) can be a hall­
mark for designing a family of fiber networks with a range of length
scales, i.e., nonwoven, collagen, buckypapers, electrospun mats, etc. for
any desired application.
Declaration of competing interest
The authors whose names are listed immediately below certify that
they have NO affiliations with or involvement in any organization or
entity with any financial interest (such as honoraria; educational grants;
participation in speakers’ bureaus; membership, employment, consul­
tancies, stock ownership, or other equity interest; and expert testimony
or patent-licensing arrangements), or non-financial interest (such as
personal or professional relationships, affiliations, knowledge or beliefs)
in the subject matter or materials discussed in this manuscript.
Acknowledgment
This work was supported by the Department of Science and Tech­
nology under project no. MTR/2019/000098. Thanks are due to Mr.
7
Mechanics of Materials 160 (2021) 103901
Danvendra Singh for his skillful computational assistance.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.mechmat.2021.103901.
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