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Semi-analytical atomic-level uncertainty quantication for the elastic properties

of 2D materials

Article · May 2021

DOI: 10.1016/j.mtnano.2021.100126

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 Semi-analytical atomic-level uncertainty quantication for the
elastic properties of 2D materials
M. C. Trinha , T. Mukhopadhyayb,∗
a Division of Mechanical System Engineering, Jeonbuk National University, Jeonju, Republic of Korea
b Department of Aerospace Engineering, Indian Institute of Technology Kanpur, Kanpur, India

Abstract
Inherent stochasticity in the nano-structural geometry and molecular mechanics properties
of lattice-like two-dimensional (2D) materials can signicantly deviate the predicted elastic
properties that are widely reported in a deterministic framework. Such uncertainties can
be attributed to inevitable fabrication uncertainties and random error in parameterizing the
atomic-level constants depending on the accuracy of highly complicated nano-scale experi-
ments. Generalized high-delity analytical models are developed in this article to quantify
the inuence of these source-uncertainties on the basis of rst and second order perturbation
theories coupled with nano-scale continuum mechanics. The proposed stochastic mechanics
based analytical framework is further validated using the baseline Monte Carlo simulation
assisted probabilistic approach. To provide comprehensive numerical insights, four dierent
2D materials with uniform and non-uniform atomic distributions are considered covering
the mono-planar as well as multi-planar nano-structural congurations (graphene, hexago-
nal boron nitride, stanene and molybdenum disulde). The perturbation based approach is
further extended to quantify the relative sensitivity of dierent nano-structural and molec-
ular mechanics parameters on the elastic moduli of 2D materials. The proposed analytical
approach leads to a signicant level of computational eciency by alleviating the necessity
of carrying out thousands of molecular dynamics simulations in order to obtain deep compu-
tational insights concerning uncertainty quantication and sensitivity analysis, which would
assume a crucial role to ensure robust analysis and design of technologically demanding
multi-functional devices and systems across the length-scales.
Keywords: Uncertainty quantication of 2D materials, Perturbation theory, Sensitivity
analysis of 2D materials, Monte Carlo simulation, Probabilistic analysis

∗
Corresponding author: Tanmoy Mukhopadhyay (Email address: tanmoy@iitk.ac.in)

Preprint submitted to Materials Today Nano May 23, 2021

1. Introduction
After the feasibility of isolating a single layer of carbon atoms, known as graphene that
possesses a range of unprecedented and fascinating properties [16], a signicant scientic
endeavor has been initiated in exploration of other potential two-dimensional (2D) and quasi-
two dimensional (quasi-2D) nanomaterials that could have excellent mechanical, chemical,
thermal, optical, and electronic properties [716]. The last decade has witnessed a remark-
able expansion in research interest concerning such 2D nanomaterials with mono-plannar
(where the constituent atoms lie in a single plane like hBN, graphene oxides, and BCN) and
multi-planar (where the constituent atoms lie in dierent planes like stanene, chalcogenides
(MoSe2 and MoS2 ), borophene, sermanene, silicene and phosphorene) [1725] structural con-
gurations. Among these materials, the hexagonal form is prominent from a top-view [8, 26]
(refer to gure 1), which from the viewpoint of atomic distribution, can further be catego-
rized into uniform (where the material is formed by an array of single atom such as graphene
and stanene) and non-uniform (where the material is formed by dierent atoms such as
hBN and MoS2 ) nanostructures [27]. The eective elastic moduli of these 2D materials,
which depend on the nano-structural conguration and molecular mechanics parameters of
the atomic bonds, are of utmost importance to characterize their applicability as structural
elements in various multi-functional devices and systems.
A plenty of research has been reported in the deterministic framework concerning dier-
ent elastic properties of 2D materials (such as eective Young's modulus, shear modulus and
Poisson's ratios) using molecular mechanics [27, 28], molecular dynamics [29], rst principle
studies/ ab-initio [3032] and experimental investigation [33]. However, inherent stochas-
ticity in the nano-structural geometry and molecular mechanics properties of lattice-like
2D materials can signicantly deviate the eective elastic properties (computationally pre-
dicted) that are widely reported following the deterministic framework. Such uncertainties
can be attributed to inevitable fabrication uncertainties and random error in parametriz-
ing the molecular mechanics constants depending on the accuracy of complex nano-scale
experiments. To ensure an adequate level of reliability in the performance of various 2D
material based nanoelectromechanical systems, it is imperative to develop a robust and in-
clusive predictive framework, where the eect of source-uncertainty can be quantied. The
traditional approach of uncertainty quantication is to follow direct Monte Carlo simulation

2
Figure 1: Atomic-level uncertainty quantication of 2D materials. (A) Three dimensional view,
top view and side view of a generic 2D material nanostructure (B) Top and side views of monoplanar 2D
materials with uniform atomic distribution (such as graphene) (C) Top and side views of monoplanar 2D
materials with non-uniform atomic distribution (such as hBN, BCN) (D) Top and side views of multiplanar
2D materials with uniform atomic distribution (such as stanene, silicene, borophene) (E) Top and side
views of multiplanar 2D materials with non-uniform atomic distribution (such as MoS2 , MoSe2 , WS2 ) (F)
Top and side views of a generic nanostructure showing the in-plane and out-of-plane angles, where ψ =
90◦ − θ/2. The parameter θ is referred as bond angle. (G  I) Deformation mechanism of bond stretching,
in-plane (i.e. 1-2 plane) angle variation and out-of-plane (i.e. normal to the 1-2 plane) angle variation (J)
Schematic representation of axial and shear stresses (K) Schematic representation of the computational
mapping between source-uncertainties of the input parameters (xi ) and the uncertainty associated with the
system responses (y ). Here ςi and ςe are symbolic representation of the associated degree of uncertainties to
the input and output quantities, respectively. In the present study the random atomic-level input variables
are the molecular mechanics and nanostructural parameters (stochastic in nature), while the system responses
are the eective elastic moduli of 2D materials.

3
where thousands of realizations are necessary to be carried out using molecular dynamics
simulation (or ab-initio calculations) [3438]. However, considering that molecular dynamics
simulations (or ab-initio calculations) are computationally expensive, it becomes practically
impossible to carry out thousands of such simulations for the comprehensive probabilistic
characterization.
In this paper, we aim to develop a generic computationally ecient analytical framework
for characterizing the eect of source-uncertainties on the elastic moduli of 2D materials.
High-delity analytical models would be developed on the basis of rst and second order per-
turbation theories coupled with nano-scale continuum mechanics. The proposed stochastic
mechanics based analytical framework would further be validated using the baseline Monte
Carlo simulation assisted probabilistic approach. To provide comprehensive numerical in-
sights, four dierent 2D materials with uniform and non-uniform atomic distributions would
be considered in this study covering the mono-planar as well as multi-planar nano-structural
congurations (graphene, hexagonal boron nitride, stanene and molybdenum disulde). The
perturbation based approach would further be extended to quantify the relative sensitivity
of dierent nano-structural and molecular mechanics parameters on the elastic moduli of
2D materials. This paper hereafter is organized as follows: a brief theoretical background
behind the molecular mechanics based closed-form formulae for the eective elastic mod-
uli of 2D materials is presented in subsection 2.1; uncertainty quantication and sensitivity
analysis for the elastic moduli of 2D materials based on rst-order and second-order pertur-
bation theories are discussed in subsection 2.2; a detailed numerical investigation following
deterministic and stochastic approaches for the elastic moduli of 2D materials belonging to
dierent classes is presented in section 3 considering various degrees of source-uncertainty;
and nally concluding remarks and a perspective of this paper are presented in section 5.

2. Atomic-level uncertainty quantication of 2D materials

2.1. Derivation of elastic moduli based on the mechanical equivalence of atomic bonds
Although hexagonal lattice-like monolayer 2D nanostructures can be categorized in four
classes as discussed in the preceding section, only two classes in terms of structural cong-
uration namely monoplanar and multiplanar are sucient to recognize for the derivation of
closed-form analytical formulae of the eective elastic moduli. This is because of the fact

4
that the mechanical equivalence of the atomic bonds are required to be considered between
two adjacent atoms, where it does not make any dierence whether the two adjacent atoms
are same or dierent (i.e. uniform and non-uniform atomic distribution). Top and side views
of monoplanar 2D nanomaterials (such as graphene and hBN) and multiplanar 2D nanoma-
terials (such as stanene and MoS2 ) are illustrated in gure 1(B-E). It can be noted that the
multiplanar conguration can be converted to the monoplanar conguration when the out-
of-plane inclination angle vanishes (i.e. α = 0). In other words, the monoplanar hexagonal
conguration can be considered as a special case of the multiplanar hexagonal conguration.
In this section we would provide a brief description of the mechanical equivalence of the
atomic bonds rst, followed by the derivation of eective elastic moduli for the lattice-like
2D materials using the equivalent bond properties.
For atomic-scale mechanics, bonding and non-bonding interactions contribute to the ef-
fective interatomic potential energy of a 2D nanomaterial. Bonding interactions such as
torsion, stretching, and bending have corresponding torsional energy (Et ), stretching energy
(Es ), and bending energy (Eb ). Non-bonding energies (Enb ) are associated with the coulom-
bic force eld, the core repulsions, and the van der Waals attraction. It can be noted in
case of small deformation that the contribution of bending and stretching eects are pre-
dominant among all constituents of the eective interatomic potential energy [39, 40]. The
strain energy associated to the bending eect in multiplanar nanomaterials such as stanene
and MoS2 can be considered as the compound eect of in-plane bending strain energy (EbI )
and out-of-plane bending strain energy (EbO ). Deformation mechanisms of the predominant
eects including stretching, in-plane bending, and out-of-plane bending for a typical generic
atomic bond of the multiplanar nanostructure are shown in gure 1(GI). For monoplanar
nanostructures such as graphane and hBN, the strain energy component caused by the out-
of-plane bending disappears as all the constitutive atoms lie in a single plane. The total
inter-atomic potential energy (E ) for a generic multiplanar nanostructure can be presented
as
E = Es + EbI + EbO
1

1 1
 (1)
2 2 2
= kr (∆l) + kθ (∆θ) + kθ (∆α)
2 2 2
Here ∆l, ∆θ and ∆α are the variations in bond length (l), in-plane angle (θ), and out-of-

5
plane angle (α) respectively, as depicted in gure 1(GI). The parameters kr and kθ denote
the stretching and bending stinesses of atomic bonds which can be expressed as structural
equivalence of a beam deformation, as reported in [41].
From a solid mechanics point of view, the application of an axial force N to a beam with
Young's modulus E , length l, uniform circular cross-sectional area A, and second moment
of area I can generate the following strain energy.
1 L N2 1 N 2l
Z
1 EA
Ua = dl = = (∆l)2 (2)
2 0 EA 2 EA 2 l
Similarly, the application of a pure bending moment M causing a slope of ∆φ at the beam
ends [27] can produce the following strain energy.
1 L M2
Z
1 EI
Ub = dl = (2∆φ)2 (3)
2 0 EI 2 l
The molecular mechanics parameter associated with the stretching of an atomic bond can
EA
be obtained by comparing Equation 2 to the rst term of Equation 1, as kr = . In case
l
of the bending of an atomic bond, the in-plane bond angle ∆θ and out-of-plane bond angle
∆α are assumed equivalent to the slope 2∆φ caused by the pure bending moment [27]. Thus
the molecular mechanics parameter associated with the bending of an atomic bond can be
EI
obtained by comparing Equation 3 to the second and third terms of Equation 1, as kθ = .
l
From these established relations between structural mechanics parameters (EA and EI )
and molecular mechanics parameters (kr and kθ ), the generalized closed-form expressions for
eective elastic moduli of hexagonal lattice-like single layer two-dimensional nanostructures
(Young's moduli, Poisson's ratios, and in-plane shear modulus for both the monoplanar and
multiplanar structural congurations) can be obtained using the concept of unit cells [4248].
The elastic moduli of an entire hexagonal periodic nanostructure can be derived by con-
sidering the stress and strain elds of single hexagonal unit, often referred as representative
volume element (RVE) or unit cell. The nanostructural congurations and the loading direc-
tions (unidirectional and shear) are shown in gure 1. It can be noted that gure 1(A) shows
the most generalized multiplanar nanostructure, the closed-form formulae corresponding to
which can be used for the four dierent classes of 2D materials (refer to gure 1(BE)) by
assuming the molecular mechanics and nanostructural parameters appropriately. For a gen-
eralized multi-planar nanostructure, the in-plane strain components can be expressed as a
function of uniaxial stresses as (refer to section 1 of the supplementary material for detailed

6
derivation) [27]
cos2 α cos2 ψ l2
 
σ1 t(sin ψ + 1) 2 2 2
(4)


11 = + cos ψ sin α + sin ψ
cos ψ kr 12kθ

σ1 tl2 cos2 α sin ψ cos ψ

12 = − (5)
12kθ

cos2 α l2
 
σ2 t cos ψ
sin2 ψ + 2 + cos2 ψ + sin2 α(sin2 ψ + 2) (6)



22 =
sin ψ + 1 kr 12kθ

σ2 tl2 cos2 α sin ψ cos ψ

21 = − (7)
12kθ
In the above expressions, ij represents the strain components in the direction j due to the
application of stress in direction i. The stress component σi represent the stress eld in
direction i. The directions i and j (where i, j = 1, 2) are mutually perpendicular. The
geometric parameters l, α, ψ and t denote the bond length, out-of-plane angle, in-plane
angle and single-layer thickness, respectively. From the above expressions, it can be noted in
a stochastic environment that the strain corresponding to a deterministic value of stress will
not be deterministic due to the inherent uncertainties of the molecular mechanics parameters.
Subsequently, the elastic moduli will be in stochastic in nature. Young's moduli in direction-
1 (E1 ) and direction-2 (E2 ) can be obtained from the in-plane stress components (i.e. σ1 and
σ1
σ2 ) and in-plane strain components (i.e. 11 and 22 ) based on the basic denitions (E1 =
11
σ2
and E2 = )
22
cos ψ
E1 =  2 2 (8)
l2

cos α cos ψ 2 2 2


t(sin ψ + 1) + cos ψ sin α + sin ψ
kr 12kθ
sin ψ + 1
E2 = 2 (9)
l2
 
cos α 2


2 2 2


t cos ψ sin ψ + 2 + cos ψ + sin α(sin ψ + 2)
kr 12kθ
12 21
Similarly, from the denition of Poisson's ratios (ν12 = − and ν21 = − ), we have
11 22
2 2 2
cos α sin ψ cos ψl
ν12 =  2 (10)
cos α cos2 ψ l2

2 2


12kθ (sin ψ + 1) + cos2 ψ sin α + sin ψ
kr 12kθ

7
 cos2 α sin ψ (sin ψ + 1) l2
ν21 = (11)
cos2 α l2
 
2 2 2



12kθ sin ψ + 2 + cos2 ψ + sin α(sin ψ + 2)
kr 12kθ
The total shear strain of an entire hexagonal unit under the application of shear stress τ can
be obtained as [49]
l3 (cos α + 2)
 
sin ψl(sin ψ + 1)
γ = τ cos α sin α cos ψ + (12)
6kθ (sin ψ + 1) cos α kr cos2 ψ
τ
Using the denition of shear stress as G12 = , we can obtain
γ
cos ψ(sin ψ + 1)kr kθ
G12 =  2  (13)
kr l 2 2
t cos ψ(cos α + 2) + kθ sin ψ(sin ψ + 1) cos α
6
The expressions of Young's moduli (E1 and E2 ), Poisson's ratios (ν12 and ν21 ) and shear
modulus (G12 ) presented in this section can be used for any 2D material (as shown in
gure 1(BE)) to obtain the elastic moduli in a deterministic framework. The parameters
required to evaluate these expressions are well-documented in material science literature.
Note that it is shown later in this paper (refer to Table 1 to Table 3) that these expressions
are able to obtain the elastic moduli readily, wherein the values are quite close to that
reported in literature. In the following section, we utilize these closed-form expressions of
the elastic moduli to quantify the eect of source-uncertainty based on perturbation theory.
In such analyses, the molecular mechanics and nanostructural parameters would be treated
as stochastic variables.

2.2. Uncertainty quantication and sensitivity analysis of 2D materials

Elastic properties of 2D materials as presented in the preceding section depend on their
geometric parameters (ψ , α, t, and l) and the molecular mechanics parameters (kr and
kθ ). Determining the accurate values of these parameters for 2D material nano-structures is
extremely challenging. The reported values of these parameters are often susceptible to un-
certainties depending on the adopted degree of quality control. Thus quantifying the source-
uncertainties associated with nanostructural and molecular mechanics parameters and their
eect on the elastic moduli of 2D materials are always of high interest not only in academia
but also in the industrial sector for ensuring robust and sustainable performance in various
potential applications. The aim of this section is to present semi-analytical frameworks for

8
quantifying the uncertainty associated with the elastic properties of single-layer 2D materi-
als with monoplanar and multiplanar congurations. In other words, the objective stands
to be establishing an ecient computational mapping between the uncertainties associated
with the elastic moduli of the 2D materials and the source-uncertainties of their atomic-level
parameters.
Having the closed-form expressions for the ve in-plane elastic moduli as presented in
the preceding section, two dierent approaches of uncertainty quantication are adopted in
this section. In the rst approach, a perturbation based intrinsic uncertainty propagation
algorithm is coupled with the closed-form expressions of the elastic moduli to obtain the cor-
responding mean and standard deviation due to stochastic variation in the input parameters
(i.e. source uncertainty). This approach is computationally quite ecient since the entire
process could be accomplished through an analytical framework. The second approach is
to adopt a sampling based method like Monte Carlo simulation (MCS), where thousands of
realizations are carried out using the closed-form expressions to obtain the elastic moduli
corresponding to dierent random combinations of the set of stochastic input parameters.
The complete probabilistic description of the response quantities (i.e. the elastic moduli) can
be obtained using MCS and subsequently, the mean and standard deviations can be calcu-
lated from the set of random output data. Since this is a semi-analytical method requiring a
large number of function evaluations, normally it is computationally more intensive. In the
current paper, we mainly focus on uncertainty quantication using the perturbation based
approach, the results of which are further cross-validated using the Monte Carlo simulation
approach. A brief description of these two uncertainty quantication approaches is provided
in the following paragraphs.
Monte Carlo simulation is a widely popular uncertainty propagation technique for in-
vestigating the probabilistic characteristics of a physical quantity as an output in terms of
dierent random input parameters. Based on the law of large number, MCS requires a large
number (∼ 104 ) of pseudorandom samples to guarantee its necessary convergence. Its results
are often considered as the ground truth for validating other methods. The mean (µ) and
standard deviation (σ ) are two important characteristics of both random input and uncertain
output parameters. In this study, ψ , α, l, kr and kθ are random input parameters. The mean
and standard deviation of these input parameters are assumed to be related as σ = µ × s0 ,

9
where s0 (= ςi , i = 1, 2, 3, ..., 5) is referred as the degree of stochasticity. Note that we have
considered same degree of stochasticity for each of the input parameters for obtaining all
the numerical results in this paper. As the actual distribution type of these random input
parameters is often unknown, it is reasonable to assume their normal distribution [50]. It
is noted that the uncertain output parameters for Young's modulus in direction-1 (E1 ) and
direction-2 (E2 ), and the in-plane shear modulus (G12 ) are normally reported in literature
for convenience as Ē1 = E1 × t, Ē2 = E2 × t, and G¯12 = G12 × t, respectively. Thus the single
layer thickness t is not considered as a random parameter in the current study, meaning
that we would quantify the uncertainties associated with Ē1 , Ē2 , G¯12 , ν12 and ν21 . In a
mathematical form, the Monte Carlo simulation based uncertainty quantication approach
can be expressed as

X(ςe ) = Φ{ψ(ς1 ), α(ς2 ), l(ς3 ), kr (ς4 ), kθ (ς5 )} (14)

where X represents the uncertain output quantities of interest i.e. Ē1 , Ē2 , G¯12 , ν12 and ν21 .
The parameter Φ denotes the Monte Carlo simulation operator which entails N0 number
of simulations corresponding to dierent random combinations of the stochastic input pa-
rameters. ςi (i = 1, 2, ..., 5) and ςe represent the degree of stochasticity associated with the
ve input parameters and the response quantity of interest (i.e. the eective elastic moduli),
respectively. Essentially in this study, we aim to establish a computational mapping between
ςi (i = 1, 2, , 5) and ςe .
In this paragraph, we briey describe the perturbation based technique for uncertainty
quantication. As each elastic moduli (X , which could be any of the elastic moduli among
Ē1 , Ē2 , G¯12 , ν12 and ν21 ) of hexagonal lattice-like single layer 2D materials is a function of
random input parameters listed in s = {ψ, α, l, kr , kθ }, its equivalent closed-form formulation
is the following Taylor series expansion derived around the mean point of each variable
µs = {µψ , µα , µl , µkr , µkθ }.
5  !
X∂X 
X(s) = X(µs ) + (si − µsi )
i=1
∂si s=µs
5 X 5
! (15)
2

1 X ∂ X  

+ (s i − µ s i
) s j − µ s j
+ Π (s)
2 i=1 j=1 ∂si ∂sj s=µs
where Π (s) represents the higher-order terms that are often omitted due to the trade-o
between the solution accuracy and computation eorts required. Based on the Taylor series

10
expansion, perturbation techniques are demonstrated to acquire the probabilistic character-
istics of each elastic moduli. In the rst-order perturbation technique (FOPT), the mean
(µI ) and standard deviation (σ I ) of the Young moduli (X ) are presented in Equation 16 and
Equation 17 as
µI {X(s)} = X (µs ) (16)

5
5 X  !  !
2 X ∂X  ∂X 
I
(17)

σ {X(s)} = Cov (si , sj )
i=1 j=1
∂si s=µs ∂sj s=µs

where Cov (si , sj ) is the covariance between random variables si and sj such that Cov (si , sj ) =
(σsi )2 when i = j and Cov (si , sj ) = 0 when the two variables are uncorrelated. Equation 16
can be directly evaluated in closed-form using Equation 4 - 11 and 13. The components of
Equation 17 can be readily obtained in closed-form using the expressions of the elastic mod-
uli (refer to Equation 4 - 11, 13). Such explicit expressions obtained using the perturbation
based method would allow a rapid and exact quantication of uncertainty and sensitivity
associated with the atomic-level input parameters of 2D materials. For illustration, one of
the components for E1 is given below (expressions for rest of the components are given in
section 2 of the supplementary material)
l2 2 2
2


∂ Ē1 cos
12kθ2
ψ sin ψ + cos ψsin α
= 2 (18)
∂kθ
 2 2
l2 2 2 ψsin2 α + cos ψcos α


(1 + sin ψ) 12k θ
sin ψ + cos kr

In the second-order perturbation technique (SOPT), the closed-form formulation for

mean (µII ) and standard deviation (σ II ) of a physical quantity is more complex and time-
consuming [51]. Following SOPT, the mean and standard deviation of the Young moduli
X(s) are presented in Equation 19 and Equation 20 as
5 5
!
∂ 2 X 

1 XX
µII {X(s)} = X(µs ) + Cov (si , sj ) (19)
2 i=1 j=1 ∂si ∂sj s=µs

5
!2 5
!2
2
 
2 X ∂X  X 1 ∂ X
E (si − µsi )4
 II 
σs2i +
 
σ {X(s)} = 
2 
∂si s=µs
 4 ∂si s=µs
i=1
!
i=1
! (20)
5
∂ 2 X 
 
X ∂X 
E (si − µsi )3
 
+ 2 
i=1
∂si s=µs
 ∂si s=µs
where E is the mathematical expectation operator in probability theory. It can be noted
that, similar to the case of FOPT, closed-form expressions for the components of Equation 19

11
and 20 can also be obtained readily, leading to an accurate and ecient symbolic calculation
of the atomic-level uncertainties.
Based on the expressions of standard deviation and mean, obtained using the perturbation
technique, sensitivity of each of the random input parameter on an elastic modulus X can
be quantied as  
σi
µi
Si = 5   (21)
P σi
i=1 µi
5
where Si = 1. Here Si represents the sensitivity of ith input parameter. The parameters σi
P
i=1
and µi denote the standard deviation and mean of the elastic moduli when only the ith input
parameter is considered as stochastic, while all other input parameters are assumed to take
their respective deterministic nominal values. Note that besides the standard deviation and
mean obtained using either FOPT or SOPT, MCS can also be used in the above expression
depending on the desired level of accuracy and computational eciency.

3. Results and discussion

Here we focus on presenting comprehensive numerical results based on the theoretical

framework of uncertainty quantication and sensitivity analysis described in the preceding
section. Four dierent hexagonal lattice-like single layer 2D materials are investigated be-
longing to the monoplanar and multiplanar nanostructural congurations with uniform and
nonuniform atomic distributions (graphene - monoplanar nanostructure and uniform atomic
distribution, hBN - monoplanar nanostructure and nonuniform atomic distribution, stanene
- multiplanar nanostructure and uniform atomic distribution, MoS2 - multiplanar nanos-
tructure and nonuniform atomic distribution), as depicted in gure 1(BE). Note here that
graphene is made of only C atoms where all the atoms lie in a single plane. A single layer
of hBN is made of two dierent atoms B and N, where these two atoms lie in a single plane
too. Stanene is made of only Sn atoms where the atoms lie in dierent planes. A single layer
of MoS2 is made of two dierent atoms Mo and S, where these two atoms lie in dierent
planes.
First we present the deterministic values of the ve elastic moduli for four dierent
classes of 2D materials, as described above. The results obtained using equations 8, 9, 10,

12
Table 1: Young's moduli (deterministic) of hexagonal lattice-like single layer 2D materials. Here the results
are presented as E¯1 = E1 × t and E¯2 = E2 × t (unit TPa-nm), where t is the single-layer thickness. The
Young's moduli of each material (E1 and E2 in TPa) can be obtained via dividing the presented values (E¯1
and E¯2 ) by the respective single layer thickness (t in nm). Four dierent materials are considered here with
both the monoplanar (graphene, hBN) and multiplanar (stanene and MoS2 ) congurations.

Present Results
Material Reference results from literature (Ē1 = Ē2 ) (TPa-nm)
(TPa-nm)

Graphene Ē1 = 0.3542 0.34 ± 0.034 [52], 0.2720.306 [53], 0.350 [54], 0.357
(Monoplanar) [31], 0.377 [55], 0.364 [56], 0.357 [57], 0.343 ±0.01 [58],
Ē2 = 0.3542 0.354 [39], 0.3604 [59]

Ē1 = 0.2659
hBN 0.251 ± 0.015 [60], 0.271 [61], 0.272 [62], 0.236 [63],
(Monoplanar) Ē2 = 0.2659 0.278 [64], 0.269 [65], 0.322 [66]

Stanene Ē1 = 0.0545

(Multiplanar) 0.0528 [67]
Ē2 = 0.0643

MoS2 Ē1 = 0.1073 0.211±0.012 [33], 0.1629±0.0603 [68], 0.141 [69], 0.262
(Multiplanar) Ē2 = 0.2141 [70], 0.150 [71]

11 and 13 are shown in Table 1 - 3, wherein the current deterministic values are compared
with published literature covering both experimental and computational investigations. The
deterministic values of the molecular mechanics and nanostructural parameters (ψ , α, l, kr
and kθ ), based on which the closed-form expressions of elastic moduli are evaluated, are
provided in section 3 of the supplementary material. A good agreement of the deterministic
results with published literature corroborates the validity of the present molecular mechanics
based analytical framework (subsection 2.1) and renders adequate condence to use it for
subsequent uncertainty quantication and sensitivity analysis. The closed-form expressions
for obtaining deterministic values of the elastic moduli, as presented in subsection 2.1, are
generalized in nature and these can be used for a wide range of 2D materials with hexagonal
lattice-like nanostructural forms by providing the respective molecular mechanics parameters
as input. These molecular mechanics parameters are well-documented for various types of
atomic bonds in the literature of materials science. The deterministic results reveal that

13
Table 2: Poisson's ratios (deterministic) of hexagonal lattice-like single layer 2D materials. Four dierent
materials are considered here with both the monoplanar (graphene, hBN) and multiplanar (stanene and
MoS2 ) congurations.

Material Present Results Reference results from literature (ν12 = ν21 )

Graphene ν12 = 0.2942 0.165 [72], 0.120.16 [73], 0.186 [74], 0.34 [75], 0.17
(Monoplanar) [76], 0.41 [77], 0.110.12 [78], 0.195 [79], 0.6530.848
ν21 = 0.2942 [80], 1.1291.1441 [81]

hBN ν12 = 0.2901 0.20.3 [82], 0.211 [83], 0.2-0.24 [82], 0.13-0.16 [84],
(Monoplanar) 0.3840.389 [85], 0.4000.405 [85], 0.3840.389 [85],
ν21 = 0.2901 0.211 [85], 0.053 [85], 0.20.4 [86]

Stanene ν12 = 0.1394

0.14 − 0.16 [27], 0.36 − 0.42 [87]
(Multiplanar) ν21 = 0.1645

MoS2 ν12 = 0.0690

(Multiplanar) 0.21 [88], 0.29 [89]
ν21 = 0.1376

the reciprocal theorem is numerically satised for all the four considered materials. It is
noticed that for graphene and hBN (monoplanar), Ē1 = Ē2 and ν12 = ν21 , while for stanene
and MoS2 (multiplanar), Ē1 < Ē2 and ν12 < ν21 . In a broader sense, 2D materials with
monoplanar structural forms (i.e. θ = 120◦ and α = 0◦ ) have equal values of elastic modulus
in the two perpendicular directions. However, for 2D materials with multiplanar structural
forms, the elastic modulus for direction-2 is greater than that of direction-1 [27, 90].
After presenting the deterministic results of the elastic moduli, we focus on the stochastic
characterization and uncertainty quantication (refer to subsection 2.2) in rest of this pa-
per. The uncertainties are accounted for in the atomic level parameters of the 2D material
nanostructures. The uncertain atomic-level geometric parameters considered here are: bond
lengths (l), in-plane and out-of-plane bond angles (ψ and α). In addition, uncertainty in the
molecular mechanics parameters of the atomic bonds is considered in the form of stochastic
stretching and bending stinesses of the atomic bonds (kr and kθ ). Note that the molecular
mechanics parameters (kr and kθ ) are representative of the corresponding force elds and
these can be obtained by using AMBER force eld for graphene, DREIDING force model

14
Table 3: In-plane shear modulus (deterministic) of hexagonal lattice-like single layer 2D materials. Here the
results are presented as G¯12 = G12 × t (unit TPa-nm), where t is the single-layer thickness of a particular
nano-material. The actual value of the in-plane shear moduli (G12 in TPa) can be obtained from the
presented results via dividing these values (G¯12 ) by the respective single layer thickness (t in nm). Four
dierent materials are considered here with both the monoplanar (graphene, hBN) and multiplanar (stanene
and MoS2 ) congurations.

Material Present Results Reference results from literature (TPa-nm)

(TPa-nm)

Graphene
G¯12 = 0.1254 0.07240.0741 [81], 0.1676 [91] 0.0952±0.0122 [92]
(Monoplanar)

hBN
G¯12 = 0.0951 0.0951 [65], 0.105 [93], 0.165 [94]
(Monoplanar)

Stanene
G¯12 = 0.0325 0.0325 [49]
(Multiplanar)

MoS2
G¯12 = 0.0719 0.079 [49]
(Multiplanar)

for hBN, and so on (refer to the supplementary material). Thus, the uncertainties in the
force-eld parameters have been considered in terms of kr and kθ in the present analysis.
Subsequently, the inuence of the compound eects of these atomic-level uncertainties are
investigated on the eective elastic properties of the 2D materials (refer to gure 1(K)). In
essence, the aim of this article is to establish a mapping between the source-uncertainties of
the atomic-level input parameters and the uncertainty in the elastic moduli. Here, we would
investigate the performance of FOPT and SOPT compared to direct MCS rst, and thereby
further numerical results will be presented following a `validated' SOPT based approach,
unless otherwise mentioned. The scenario of compound stochasticity (with same degree of
uncertainty in all the input parameters i.e. ςi = s0 , for all i) would be considered, except for
the results presented in gure 8 - 11 where the inuence of the individual stochastic eects
are investigated.
The comparative performance of the three aforementioned uncertainty quantication

15
 Legend:

Solid: 
Dashed: 

Figure 2: Comparative performance of the Monte Carlo simulation (MCS), rst-order pertur-
bation technique (FOPT), and second-order perturbation technique (SOPT) in the uncertainty
quantication of graphene. (A) Mean and standard deviation corresponding to dierent level of source-
uncertainty for the Young's modulus in direction-1 E¯1 (B) Mean and standard deviation corresponding
to dierent level of source-uncertainty for the Young's modulus in direction-2 E¯2 (C) Mean and standard
deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν12 (D) Mean and
standard deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν21 (E) Mean
and standard deviation corresponding to dierent level of source-uncertainty for the shear modulus G¯12 .

frameworks (FOPT, SOPT and MCS) on the ve elastic moduli of studied 2D materials is
presented in gure 2 for graphene, gure 3 for hBN, gure 4 for stanene, and gure 5 for

16
 Legend:

Solid: 
Dashed: 

Figure 3: Comparative performance of the Monte Carlo simulation (MCS), rst-order per-
turbation technique (FOPT), and second-order perturbation technique (SOPT) in the un-
certainty quantication of hBN. (A) Mean and standard deviation corresponding to dierent level of
source-uncertainty for the Young's modulus in direction-1 E¯1 (B) Mean and standard deviation correspond-
ing to dierent level of source-uncertainty for the Young's modulus in direction-2 E¯2 (C) Mean and standard
deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν12 (D) Mean and
standard deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν21 (E) Mean
and standard deviation corresponding to dierent level of source-uncertainty for the shear modulus G¯12 .

MoS2 . In terms of standard deviation, both the FOPT and SOPT perform well compared
to the baseline results of MCS, even for a high value of the degree of source-uncertainty

17
 Legend:

Solid: 
Dashed: 

Figure 4: Comparative performance of the Monte Carlo simulation (MCS), rst-order pertur-
bation technique (FOPT), and second-order perturbation technique (SOPT) in the uncertainty
quantication of stanene. (A) Mean and standard deviation corresponding to dierent level of source-
uncertainty for the Young's modulus in direction-1 E¯1 (B) Mean and standard deviation corresponding
to dierent level of source-uncertainty for the Young's modulus in direction-2 E¯2 (C) Mean and standard
deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν12 (D) Mean and
standard deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν21 (E) Mean
and standard deviation corresponding to dierent level of source-uncertainty for the shear modulus G¯12 .

s0 = 0.1. It is noted that the mean of each uncertain elastic modulus obtained from the
SOPT is in good agreement with the MCS results up to high degrees of source-uncertainty.

18
 Legend:

Solid: 
Dashed: 

Figure 5: Comparative performance of the Monte Carlo simulation (MCS), rst-order per-
turbation technique (FOPT), and second-order perturbation technique (SOPT) in the uncer-
tainty quantication of MoS2 . (A) Mean and standard deviation corresponding to dierent level of
source-uncertainty for the Young's modulus in direction-1 E¯1 (B) Mean and standard deviation correspond-
ing to dierent level of source-uncertainty for the Young's modulus in direction-2 E¯2 (C) Mean and standard
deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν12 (D) Mean and
standard deviation corresponding to dierent level of source-uncertainty for the Poisson's ratio ν21 (E) Mean
and standard deviation corresponding to dierent level of source-uncertainty for the shear modulus G¯12 .

In the same vein, the accuracy of the FOPT deteriorates with the increase in degree of
stochasticity s0 . The standard deviation of all the elastic moduli increases with increasing

19
 Legend:

Solid: 
Dashed: 

Figure 6: Number of iterations (N0 ) required to achieve converged numerical values of mean
and standard deviation for graphene using Monte Carlo simulation (MCS), rst-order pertur-
bation technique (FOPT), and second-order perturbation technique (SOPT). (A) Convergence
considering s0 = 0.1 for the Young's modulus in direction-1 E¯1 (B) Convergence considering s0 = 0.1 for
the Young's modulus in direction-2 E¯2 (C) Convergence considering s0 = 0.1 for the Poisson's ratio ν12 (D)
Convergence considering s0 = 0.1 for the Poisson's ratio ν21 (E) Convergence considering s0 = 0.1 for the
shear modulus G¯12 .

degree of source-uncertainty, while the trend of mean values depends on the particular elastic
modulus and the 2D material under consideration. Considering a Gaussian distribution for
the elastic properties (which is veried to be true later in gure 12), it can be shown that

20
the elastic properties could deviate more than 50% with respect to their deterministic values
that are normally considered in the analysis and design of various nano-scale devises and
systems. Moreover, the mean of the elastic moduli may also increase or decrease signicantly
from the deterministic values depending on the elastic moduli and the 2D material under
consideration. It can be noted from the results that the trend of variation in mean depends
on the nanostructural congurations (monoplannar or multiplanar), rather than atomistic
distribution (uniform or nonuniform). The monoplanar structures of graphene and hBN
show similar trends, while the multiplanar structures of stanene and MoS2 show dierent
trends due to their bi-planar and tri-planar congurations, respectively. In general, from
the above discussions, it becomes imperative to take into account the stochastic deviations
in the values of elastic moduli for an inclusive and sustainable design paradigm, wherein
the proposed perturbation based molecular mechanics approach could readily be adopted for
ecient numerical quantication of a wide range of 2D materials.
We have further investigated the computational resources required for carrying out un-
certainty quantication following MCS, FOPT and SOPT. For this purpose, the number of
iterations necessary to obtain converged mean and standard deviations are reported consid-
ering a monoplanar (graphene) and a multiplanar (MoS2 ) 2D material. The results presented
in gure 6 of the main paper and gure 4 of the supplementary material show that while
FOPT and SOPT take only a few samples to converge, the MCS takes ∼104 samples. In this
context, it may be noted that the derivatives in the FOPT and SOPT based expressions of
mean and standard deviations (refer to Equations 16, 17, 19 and 20) can be obtained either
in closed form, or numerically when the dierentiation becomes too complex. However, as
shown in the convergence results here, the number of iterations required to evaluate the
FOPT and SOPT based mean and standard deviations is quite low in the current analyses.
This leads to a signicant degree of computational eciency in perturbation method based
uncertainty quantication of 2D materials. Further, it is interesting to notice that the re-
sults of MCS converge close to results of SOPT, indicating that SOPT yields more accurate
results compared to FOPT. Note that a converged MCS is regarded as the most authentic
result in stochastic analyses.
After establishing that SOPT is capable of obtaining both the mean and standard devi-
ations accurately up to a signicantly large degree of source-uncertainty, further computa-

21
 Legend:

Figure 7: Relative inuence of compound source-uncertainties on the elastic moduli of dier-

ent classes of 2D materials. (A) graphene (monoplanar nanostructure and uniform atomic distribution)
(B) hBN (monoplanar nanostructure and nonuniform atomic distribution) (C) stanene (multiplanar nanos-
tructure and uniform atomic distribution) (D) MoS2 (multiplanar nanostructure and nonuniform atomic
distribution). Here the eect of source uncertainties (with dierent degree) are investigated on Young's
modulus in direction-1 E¯1 , Young's modulus in direction-2 E¯2 , Poisson's ratio ν12 , Poisson's ratio ν21 , and
in-plane shear modulus G¯12 using the SOPT.

tional insights are presented here based on this ecient uncertainty quantication approach.
Figure 7 presents a measure as to how sensitive dierent eective elastic moduli are towards
source uncertainty, wherein the respective coecient of variations are presented considering
the compound eect of dierent degrees of source-uncertainty. For all the four dierent
classes of 2D materials, ν12 is found to be most sensitive towards source uncertainties. How-

22
 Legend:

Figure 8: Individual inuence and sensitivity of the source-uncertainties for graphene. Relative
inuence of the source-uncertainty associated with individual stochastic parameters (ψ , α, l, kr , and kθ ) and
their corresponding sensitivity (shown using insets) are plotted considering dierent degree of uncertainty.
SOPT is used to obtain the results presented here. (A) Young's modulus in direction-1 E¯1 (B) Young's
modulus in direction-2 E¯2 (C) Poisson's ratio ν12 (D) Poisson's ratio ν21 (E) In-plane shear modulus G¯12 .

ever, depending on the monoplanar or multiplanar congurations, the Young's moduli and
the shear modulus are found to be least sensitive to uncertainties.
Sensitivity of dierent individual eects of the random input parameters (ψ , α, l, kr ,
and kθ ) are investigated further to access their relative importance in the elastic moduli

23
 Legend:

Figure 9: Individual inuence and sensitivity of the source-uncertainties for hBN. Relative
inuence of the source-uncertainty associated with individual stochastic parameters (ψ , α, l, kr , and kθ ) and
their corresponding sensitivity (shown using insets) are plotted considering dierent degree of uncertainty.
SOPT is used to obtain the results presented here. (A) Young's modulus in direction-1 E¯1 (B) Young's
modulus in direction-2 E¯2 (C) Poisson's ratio ν12 (D) Poisson's ratio ν21 (E) In-plane shear modulus G¯12 .

of the dierent classes of 2D materials. Figures 8 - 11 present the coecient of variation

corresponding to dierent degree of uncertainty in the individual parameters, while keep-
ing rest of the parameters constant. Sensitivity of the input parameters on dierent elastic
moduli is also explicitly quantied considering dierent values of the source uncertainties,

24
 Legend:

Figure 10: Individual inuence and sensitivity of the source-uncertainties for stanene. Relative
inuence of the source-uncertainty associated with individual stochastic parameters (ψ , α, l, kr , and kθ ) and
their corresponding sensitivity (shown using insets) are plotted considering dierent degree of uncertainty.
SOPT is used to obtain the results presented here. (A) Young's modulus in direction-1 E¯1 (B) Young's
modulus in direction-2 E¯2 (C) Poisson's ratio ν12 (D) Poisson's ratio ν21 (E) In-plane shear modulus G¯12 .

as presented in the insets. It can be noted that in case of graphene and hBN (monoplanar
conguration), there is no out-of-plane inclination angle (α = 0). Thus, this input param-
eter causes no stochastic eect on the uncertainty of the elastic moduli of monoplanar 2D
materials. Subsequently, the corresponding sensitivity of α also comes out to be zero. In

25
 Legend:

Figure 11: Individual inuence and sensitivity of the source-uncertainties for MoS2 . Relative
inuence of the source-uncertainty associated with individual stochastic parameters (ψ , α, l, kr , and kθ ) and
their corresponding sensitivity (shown using insets) are plotted considering dierent degree of uncertainty.
SOPT is used to obtain the results presented here. (A) Young's modulus in direction-1 E¯1 (B) Young's
modulus in direction-2 E¯2 (C) Poisson's ratio ν12 (D) Poisson's ratio ν21 (E) In-plane shear modulus G¯12 .

case of the monoplanar structural congurations (graphene and hBN), the Young's moduli
are found to be most sensitive to ψ and kr , while the Poisson's ratios and the shear modulus
are most sensitive to l. In case of the bi-planar stanene structure, kr is most sensitive to
the Young's moduli and l is most sensitive to the Poisson's ratios and shear modulus. For

26
 Legend:

Figure 12: Complete probabilistic characterization of the elastic moduli. Monte Carlo simulation
based complete probabilistic descriptions of the elastic moduli (Young's modulus in direction-1 E¯1 , Young's
modulus in direction-2 E¯2 , Poisson's ratio ν12 , Poisson's ratio ν21 , and in-plane shear modulus G¯12 ) are
presented for various classes of 2D materials considering a compound eect of uncertainty with s0 = 0.05.
(A) graphene (monoplanar nanostructure and uniform atomic distribution) (B) hBN (monoplanar nanos-
tructure and nonuniform atomic distribution) (C) stanene (multiplanar nanostructure and uniform atomic
distribution) (D) MoS2 (multiplanar nanostructure and nonuniform atomic distribution).

the tri-planar MoS2 structure, l and ψ are most sensitive to the Young's moduli, while α, ψ
and l are most sensitive to the Poisson's ratios and the shear modulus. The results further
reveal that degree of source-uncertainty in the individual input parameters does not have
any eect on their sensitivity.
So far in this paper, we have concentrated on quantifying the eect of source-uncertainties
using the mean and standard deviation of the elastic moduli. The ecient perturbation based
techniques (FOPT and SOPT) are ideal for this purpose. However, when the complete
probabilistic descriptions of the stochastic elastic moduli are required, the Monte Carlo

27
simulation is the best approach. Here we investigate the complete probabilistic descriptions
of the elastic moduli considering a compound eect of source uncertainty with the degree
of stochasticity as s0 = 0.05. The probabilistic distributions, obtained using Monte Carlo
simulations coupled with the closed-form expressions of elastic moduli, are presented in
gure 12 for graphene, hBN, stanene, and MoS2 . All the probabilistic descriptions follow
Gaussian distribution, wherein the stochastic bounds of dierent elastic moduli are found to
be in accordance with their respective sensitivities (as presented in the preceding gures).
It can be noted that we have shown typical probability density functions for s0 = 0.05 here;
however, similar characterization of the complete probabilistic descriptions corresponding to
other values of the degree of stochasticity can be readily obtained following the proposed
framework.

4. Summary and perspective

As discussed in the preceding sections, there are two sets of uncertainties involved in the
current analysis: I. source-uncertainty of the stochastic input parameters (ςi , i = 1, 2, ..., 5),
and II. uncertainty of the eective elastic moduli of the 2D materials (ςe ). We have proposed
an ecient framework for mapping ςe in terms of ςi (where i = 1, 2, ..., 5) i.e. developing
the capability of predicting the expected uncertainty associated with the elastic moduli for
dierent degree of stochasticity of the atomic-level sources of uncertainty. Thus, degree of
stochasticity of the input sources of uncertainty (l, ψ , α, kr and kθ ) refers here to the extent
of their variability with respect to the corresponding mean values. Such variability of the
input sources could be attributed to inevitable fabrication uncertainties and random error in
parameterizing the atomic-level constants depending on the accuracy of highly complicated
nano-scale experiments. In reality, the actual value of the degree of stochasticity (ςi ) is often
unknown and depends on the condence of the input parameters (i.e. quality of experimental
characterization and parameterizations). Thus, a wide range of its value (ςi = s0 ∼ [0 0.1])
is considered to investigate the eect of source uncertainties comprehensively on the elastic
moduli of 2D materials. In the current numerical investigation, we have considered ςi = s0 ,
for all the ve input parameters i.e. i = 1, 2, 3, ..., 5 unless otherwise mentioned. However,
dierent values of ςi for the ve stochastic sources of uncertainties (i.e. ς1 6= ς2 6= ς3 6= ς4 6= ς5 )
can also be considered in the current framework, if required.

28
 The uncertainty involved in the elastic moduli depends on the compound eect of all
the source uncertainties, which is quantied in the current article following two dierent
approaches (perturbation based method and Monte Carlo simulation based method). In this
context, it can be noted that the variation of the mean of the elastic moduli comes out to be
highly nonlinear, while that of the standard deviations is almost linear (the uncertainty of the
elastic moduli is quantied primarily using the rst two statistical moments). Interestingly,
we note that the elastic moduli could vary up to as high as 50% corresponding to the
degree of stochasticity of 0.1. Moreover, the mean of the elastic moduli may also increase
or decrease signicantly from the deterministic values depending on the elastic moduli and
the 2D material under consideration. Thus, the mapping of stochasticity, as undertaken in
the current investigation, is not straightforward, rather dependent on the intrinsic stochastic
physics involved in the system. An explicit quantication of the expected level of stochastic
deviation of the eective elastic moduli would lead to inclusive analysis and design of nano-
scale devices and systems where 2D materials can be used.
This paper investigates four dierent 2D materials (graphene, hBN, stanene and MoS2 )
that belong to four dierent structural classes (i.e. uniform, non-uniform, mono-planar,
and multi-planar atomic structures). We noted that the stochastic elastic moduli depend
strongly on these structural congurations. The stochastic results for one class of materials
can not represent the other class. This aspect is appropriately highlighted in the preceding
section of numerical results. Moreover, we have investigated ve dierent elastic moduli (two
Young's moduli, two Poisson's ratios and shear modulus) for each of these four classes of 2D
materials. The inuence of stochasticity varies considerably for dierent elastic moduli even
for the same 2D material.
It can be noted that the analytical framework for uncertainty quantication of the elas-
tic moduli presented in this paper can serve as an ecient reference for any nano-scale
lattice-like material (monoplanar and multiplanar). Even though results are shown in this
paper considering only four dierent materials (belonging to four dierent classes as per the
nanostructural conguration and atomic distribution), the uncertainty quantication and
sensitivity analysis frameworks can be used for various other 2D materials. The current fo-
cus of this paper is on hexagonal nanostructures of 2D materials. In fact, a large number of
the 2D materials beyond the four considered examples have hexagonal lattice-like structure

29
(refer to [95]). The current formulations are directly applicable to all such hexagonal 2D
and quasi-2D materials. Note that, the hexagonal lattice could be converted to rectangular
and rhombus shapes by taking the in-plane angle and length of the bond angles parallel
to direction-1 as zero, respectively [96]. The corresponding elastic moduli can be readily
obtained by introducing slight changes in the geometry in the mechanics-based derivation
of the supplementary material. As a matter of fact, a similar mechanics-based approach
considering the bond properties and lattice geometry could be potentially extended to any
lattice forms of dierent 2D materials by appropriately choosing the unit cell. Noteworthy
feature of the current framework of uncertainty quantication is the computational eciency
and cost-eectiveness compared to performing molecular dynamics simulation or nano-scale
experiments. Otherwise, it would have been practically impossible to perform a large number
(∼ 104 ) of function evaluations for Monte Carlo simulation based uncertainty quantication
and sensitivity analysis.

5. Conclusions

A generic analytical framework is proposed in this article to obtain deep computational

insights eciently for a wide range of 2D materials concerning uncertainty quantication
and sensitivity analysis of the eective elastic properties. First and second order pertur-
bation theories are coupled with an atomic-level continuum mechanics based approach for
quantifying the inevitable inuence of source uncertainties, which can be attributed to dif-
ferent level of fabrication irregularities and random error in parametrizing the atomic-level
constants depending on the accuracy of complex nano-scale experiments. It is shown that
the perturbation based approach can characterize the eect of source-uncertainties quite
eciently compared to the baseline direct Monte Carlo simulation approach. Following a
variance-based framework, the perturbation based approach is further extended to quantify
the relative sensitivity of dierent nano-structural and molecular mechanics parameters on
the elastic moduli of 2D materials, wherein it is noticed that the sensitivity of dierent pa-
rameters depends on the elastic moduli as well as the type of 2D material under consideration.
Such explicit quantication of sensitivity, as presented in this article, could provide a clear
perspective on the degree of accuracy and quality control required for dierent nano-scale
parameters to minimize the error and uncertainty in predicted eective elastic properties.

30
 To provide comprehensive numerical insights, four dierent classes of 2D materials with
uniform and non-uniform atomic distributions are considered covering the mono-planar
as well as multi-planar nano-structural congurations (graphene, hexagonal boron nitride,
stanene and molybdenum disulde). The results reveal that SOPT obtains more accurate
results compared to FOPT, wherein the mean and standard deviation of the elastic moduli
are found to deviate from the nominal deterministic values signicantly. The compound ef-
fect of source-uncertainties with a standard deviation up to 0.1 could lead to more than 50%
deviation in the deterministic values of elastic moduli, essentially corroborating the necessity
of developing an inclusive analysis and design framework for 2D materials considering the
inuence of uncertainties. The presented analytical framework for stochastic characteriza-
tion of the elastic moduli can be regarded as an ecient reference for the entire spectrum
of 2D materials with lattice-like structural forms. It can be noted in this context that such
a comprehensive stochastic characterization would have been practically impossible from
the computational viewpoint following a direct Monte Carlo simulation approach with the
conventional molecular dynamics simulations.
In summary, this paper presents a generic and ecient, yet insightful mapping between
the uncertainties associated with elastic moduli of 2D materials and the individual source-
uncertainties concerning the nano-structural and molecular mechanics parameters. As the
elastic moduli are of utmost importance for utilizing the 2D materials as structural elements
in various nanoelectromechanical systems and devices, robust characterization of these elastic
moduli towards inevitable source-uncertainties would be pivotal in ensuring a reliable and
sustainable performance.

Acknowledgements
TM acknowledges the Initiation Grant received from IIT Kanpur during the period of
this research work. MCT is thankful to Dr. Hyungmin Jun (CSDL, Jeonbuk National
University) for his support via the Basic Science Research Program through the National
Research Foundation of Korea (NRF). The authors would like to thank Mr. Ritam Paul
(SURGE, IIT Kanpur) for supporting the initial numerical analyses.

Competing interests
The authors declare no competing nancial interests.

31
Data availability

All data used to generate these results is available in the main text or Supplementary In-
formation. Further details could be obtained from the corresponding author upon reasonable
request.

References

[1] Lee, H. C., Liu, W.-W., Chai, S.-P., Mohamed, A. R., Aziz, A., Khe, C.-S., Hidayah, N.
M. S., and Hashim, U. Review of the synthesis, transfer, characterization and growth
mechanisms of single and multilayer graphene. RSC Adv., 7:1564415693, 2017.
[2] Li, Y., Wei, A., and Datta, D. Thermal characteristics of graphene nanoribbons endorsed
by surface functionalization. Carbon, 113:274  282, 2017.
[3] Gupta, K. K., Mukhopadhyay, T., Roy, A., and Dey, S. Probing the compound eect
of spatially varying intrinsic defects and doping on mechanical properties of hybrid
graphene monolayers. Journal of Materials Science & Technology, 50:4458, 2020.
[4] Lin, P., Pan, C., and Wang, Z. Two-dimensional nanomaterials for novel piezotronics
and piezophototronics. Materials Today Nano, 4:17  31, 2018.
[5] Mukhopadhyay, T., Mahata, A., Naskar, S., and Adhikari, S. Probing the ef-
fective young's modulus of `magic angle' inspired multi-functional twisted nano-
heterostructures. Advanced Theory and Simulations, 3(10):2000129, 2020.
[6] Roy, A., Gupta, K., Naskar, S., Mukhopadhyay, T., and Dey, S. Compound inuence of
topological defects and heteroatomic inclusions on the mechanical properties of swcnts.
Materials Today Communications, 26:102021, 2021.
[7] Balendhran, S., Walia, S., Nili, H., Sriram, S., and Bhaskaran, M. Elemental analogues
of graphene: silicene, germanene, stanene, and phosphorene. Small, 11(6):640652,
2015.
[8] Xu, M., Liang, T., Shi, M., and Chen, H. Graphenelike twodimensional materials.
Chemical Reviews, 113(5):37663798, 2013.
[9] Das, S., Robinson, J. A., Dubey, M., Terrones, H., and Terrones, M. Beyond graphene:
Progress in novel two-dimensional materials and van der waals solids. Annual Review
of Materials Research, 45:127, 2015.

32
[10] Ghatak, K., Kang, K. N., Yang, E.-H., and Datta, D. Controlled edge dependent stack-
ing of ws2-ws2 homo-and ws2-wse2 hetero-structures: A computational study. Scientic
reports, 10(1):111, 2020.
[11] Chakraborty, P., Das, T., Nafday, D., Boeri, L., and Saha-Dasgupta, T. Manipulating
the mechanical properties of ti2 C mxene: Eect of substitutional doping. Phys. Rev. B,
95:184106, 2017.
[12] Zhou, N., Yang, R., and Zhai, T. Two-dimensional non-layered materials. Materials
Today Nano, 8:100051, 2019.
[13] Wang, H., Feng, H., and Li, J. Graphene and graphene-like layered transition metal
dichalcogenides in energy conversion and storage. Small, 10(11):21652181, 2014.
[14] Hua, C., Li, S., Xu, Z.-A., Zheng, Y., Yang, S. A., and Lu, Y. Tunable topological
energy bands in 2d dialkali-metal monoxides. Advanced Science, 7(4):1901939, 2020.
[15] Hua, C., Sheng, F., Hu, Q., Xu, Z.-A., Lu, Y., and Zheng, Y. Dialkali-metal monochalco-
genide semiconductors with high mobility and tunable magnetism. The journal of phys-
ical chemistry letters, 9(23):66956701, 2018.
[16] Bai, H., Wang, X., Wu, W., He, P., Xu, Z., Yang, S. A., and Lu, Y. Nonvolatile
ferroelectric control of topological states in two-dimensional heterostructures. Phys.
Rev. B, 102:235403, 2020.
[17] Geim, A. K. and Grigorieva, I. V. Van der waals heterostructures. Nature, 499(7459):
419425, 2013.
[18] Zhang, Y. J., Yoshida, M., Suzuki, R., and Iwasa, Y. 2d crystals of transition metal
dichalcogenide and their iontronic functionalities. 2D Materials, 2(4):044004, 2015.
[19] van den Broek, B., Houssa, M., Lu, A., Pourtois, G., Afanas'ev, V., and Stesmans, A.
Silicene nanoribbons on transition metal dichalcogenide substrates: Eects on electronic
structure and ballistic transport. Nano Research, 9(11):33943406, 2016.
[20] Houssa, M., van den Broek, B., Iordanidou, K., Lu, A. K. A., Pourtois, G., Locquet,
J.-P., Afanas'ev, V., and Stesmans, A. Topological to trivial insulating phase transition
in stanene. Nano Research, 9(3):774778, 2016.
[21] Shi, Z. and Singh, C. V. The ideal strength of two-dimensional stanene may reach or
exceed the grith strength estimate. Nanoscale, 9:70557062, 2017.
[22] Mahata, A. and Mukhopadhyay, T. Probing the chirality-dependent elastic properties

33
 and crack propagation behavior of single and bilayer stanene. Phys. Chem. Chem. Phys.,
20:2276822782, 2018.
[23] Rehman, M. U., Hua, C., and Lu, Y. Topology and ferroelectricity in group-v mono-
layers. Chinese Physics B, 29(5):057304, 2020.
[24] Wang, X., Xiao, C., Yang, C., Chen, M., Yang, S. A., Hu, J., Ren, Z., Pan, H., Zhu, W.,
Xu, Z.-A., and Lu, Y. Ferroelectric control of single-molecule magnetism in 2d limit.
Science Bulletin, 65(15):12521259, 2020.
[25] Chandra, Y., Mukhopadhyay, T., Adhikari, S., and Figiel, F. Size-dependent dynamic
characteristics of graphene based multi-layer nano hetero-structures. Nanotechnology,
31:145705, 2020.
[26] Ersan, F., Cahangirov, S., Göko§lu, G., Rubio, A., and Aktürk, E. Stable monolayer
honeycomb-like structures of RuX2 (x = S, Se). Phys. Rev. B, 94:155415, 2016.
[27] Mukhopadhyay, T., Mahata, A., Adhikari, S., and Zaeem, M. A. Eective elastic prop-
erties of two dimensional multiplanar hexagonal nanostructures. 2D Materials, 4(2):
025006, 2017.
[28] Chandra, Y., Adhikari, S., and Flores, E. S. Advances in nite element modelling
of graphene and associated nanostructures. Materials Science and Engineering: R:
Reports, 140:100544, 2020.
[29] Grantab, R., Shenoy, V. B., and Ruo, R. S. Anomalous strength characteristics of tilt
grain boundaries in graphene. Science, 330(6006):946948, 2010.
[30] Lorenz, T., Joswig, J.-O., and Seifert, G. Stretching and breaking of monolayer mos2 
an atomistic simulation. 2D Materials, 1(1):011007, 2014.
[31] Liu, F., Ming, P., and Li, J. Ab initio calculation of ideal strength and phonon instability
of graphene under tension. Physical Review B, 76(6):064120, 2007.
[32] Lebègue, S. and Eriksson, O. Electronic structure of two-dimensional crystals from ab
initio theory. Phys. Rev. B, 79:115409, 2009.
[33] Castellanos-Gomez, A., Poot, M., Steele, G. A., van der Zant, H. S., Agraït, N., and
Rubio-Bollinger, G. Elastic properties of freely suspended mos2 nanosheets. Advanced
Materials, 24(6):772775, 2012.
[34] Wan, S., Sinclair, R. C., and Coveney, P. V. Uncertainty quantication in classical
molecular dynamics. Philosophical Transactions of the Royal Society A: Mathematical,

34
 Physical and Engineering Sciences, 379(2197):20200082, 2021.
[35] Mukhopadhyay, T., Mahata, A., Dey, S., and Adhikari, S. Probabilistic analysis and
design of hcp nanowires: An ecient surrogate based molecular dynamics simulation
approach. Journal of Materials Science & Technology, 32(12):13451351, 2016.
[36] Mahata, A., Mukhopadhyay, T., and Adhikari, S. A polynomial chaos expansion based
molecular dynamics study for probabilistic strength analysis of nano-twinned copper.
Materials Research Express, 3(3):036501, 2016.
[37] Dhaliwal, G., Nair, P. B., and Singh, C. V. Uncertainty analysis and estimation of
robust airebo parameters for graphene. Carbon, 142:300310, 2019.
[38] Mukhopadhyay, T., Mahata, A., Adhikari, S., and Zaeem, M. A. Eective mechanical
properties of multilayer nano-heterostructures. Scientic reports, 7(1):15818, 2017.
[39] Shokrieh, M. M. and Raee, R. Prediction of young's modulus of graphene sheets and
carbon nanotubes using nanoscale continuum mechanics approach. Materials & Design,
31:790795, 2010.
[40] Gelin, B. R. Molecular Modeling of Polymer Structures and Properties. Hanser Gardner
Publications, 1994.
[41] Li, C. and Chou, T. W. A structural mechanics approach for the analysis of carbon
nanotubes. International Journal of Solids and Structures, 40(10):2487  2499, 2003.
[42] Gibson, L. and Ashby, M. F. Cellular Solids Structure and Properties. Cambridge
University Press, Cambridge, UK, 1999.
[43] Singh, A., Mukhopadhyay, T., Adhikari, S., and Bhattacharya, B. Voltage-dependent
modulation of elastic moduli in lattice metamaterials: Emergence of a programmable
state-transition capability. International Journal of Solids and Structures, 208-209:31
48, 2021.
[44] Mukhopadhyay, T., Naskar, S., and Adhikari, S. Anisotropy tailoring in geometrically
isotropic multi-material lattices. Extreme Mechanics Letters, 40:100934, 2020.
[45] Adhikari, S., Mukhopadhyay, T., Shaw, A., and Lavery, N. Apparent negative values of
young’s moduli of lattice materials under dynamic conditions. International Journal
of Engineering Science, 150:103231, 2020.
[46] Mukhopadhyay, T., Adhikari, S., and Alu, A. Theoretical limits for negative elastic
moduli in subacoustic lattice materials. Phys. Rev. B, 99:094108, 2019.

35
[47] Mukhopadhyay, T. and Adhikari, S. Eective in-plane elastic moduli of quasi-random
spatially irregular hexagonal lattices. International Journal of Engineering Science, 119:
142  179, 2017.
[48] Mukhopadhyay, T., Adhikari, S., and Alu, A. Probing the frequency-dependent elastic
moduli of lattice materials. Acta Materialia, 165:654  665, 2019.
[49] Mukhopadhyay, T., Mahata, A., Adhikari, S., and Asle Zaeem, M. Probing the
shear modulus of two-dimensional multiplanar nanostructures and heterostructures.
Nanoscale, 10:52805294, 2018.
[50] Lyon, A. Why are normal distributions normal? The British Journal for the Philosophy
of Science, 65(3):621649, 2014.
[51] Trinh, M. C., Mukhopadhyay, T., and Kim, S. E. A semi-analytical stochastic buckling
quantication of porous functionally graded plates. Aerospace Science and Technology,
page 105928, 2020.
[52] Lee, C., Wei, X., Kysar, J. W., and Hone, J. Measurement of the elastic properties and
intrinsic strength of monolayer graphene. Science, 321(5887):385388, 2008.
[53] Demczyk, B., Wang, Y., Cumings, J., Hetman, M., Han, W., Zettl, A., and Ritchie,
R. Direct mechanical measurement of the tensile strength and elastic modulus of mul-
tiwalled carbon nanotubes. Materials Science and Engineering: A, 334(1–2):173 
178, 2002.
[54] Kudin, K. N., Scuseria, G. E., and Yakobson, B. I. C 2 f, bn, and c nanoshell elasticity
from ab initio computations. Physical Review B, 64(23):235406, 2001.
[55] Lier, G. V., Alsenoy, C. V., Doren, V. V., and Geerlings, P. Ab initio study of the
elastic properties of single-walled carbon nanotubes and graphene. Chemical Physics
Letters, 326(1–2):181  185, 2000.
[56] Sánchez-Portal, D., Artacho, E., Soler, J. M., Rubio, A., and Ordejón, P. Ab initio
structural, elastic, and vibrational properties of carbon nanotubes. Phys. Rev. B, 59:
1267812688, 1999.
[57] Jiang, J.-W., Wang, J.-S., and Li, B. Young's modulus of graphene: A molecular
dynamics study. Phys. Rev. B, 80:113405, 2009.
[58] Zhao, H., Min, K., and Aluru, N. Size and chirality dependent elastic properties of
graphene nanoribbons under uniaxial tension. Nano letters, 9(8):30123015, 2009.

36
[59] Chang, T. and Gao, H. Size-dependent elastic properties of a single-walled carbon
nanotube via a molecular mechanics model. Journal of the Mechanics and Physics of
Solids, 51(6):10591074, 2003.
[60] Song, L., Ci, L., Lu, H., Sorokin, P. B., Jin, C., Ni, J., Kvashnin, A. G., Kvashnin, D. G.,
Lou, J., Yakobson, B. I., and Ajayan, P. M. Large scale growth and characterization of
atomic hexagonal boron nitride layers. Nano Letters, 10(8):32093215, 2010.
[61] Kudin, K. N., Scuseria, G. E., and Yakobson, B. I. c2 F, bn, and c nanoshell elasticity
from ab initio computations. Phys. Rev. B, 64:235406, 2001.
[62] Peng, Q., Ji, W., and De, S. Mechanical properties of the hexagonal boron nitride
monolayer: Ab initio study. Computational Materials Science, 56:11  17, 2012.
[63] Zhao, S. and Xue, J. Mechanical properties of hybrid graphene and hexagonal boron
nitride sheets as revealed by molecular dynamic simulations. Journal of Physics D:
Applied Physics, 46(13):135303, 2013.
[64] Le, M.-Q. Young's modulus prediction of hexagonal nanosheets and nanotubes based
on dimensional analysis and atomistic simulations. Meccanica, 49(7):17091719, 2014.
[65] Jiang, L. and Guo, W. A molecular mechanics study on size-dependent elastic properties
of single-walled boron nitride nanotubes. Journal of the Mechanics and Physics of Solids,
59(6):1204  1213, 2011.
[66] Oh, E. S. Elastic properties of various boron-nitride structures. Metals and Materials
International, 17(1):2127, 2011.
[67] Modarresi, M., Kakoee, A., Mogulkoc, Y., and Roknabadi, M. Eect of external strain
on electronic structure of stanene. Computational Materials Science, 101:164  167,
2015.
[68] Bertolazzi, S., Brivio, J., and Kis, A. Stretching and breaking of ultrathin MoS2 . ACS
Nano, 5(12):97039709, 2011.
[69] Lorenz, T., Teich, D., Joswig, J.-O., and Seifert, G. Theoretical study of the mechanical
behavior of individual TiS2 and MoS2 nanotubes. The Journal of Physical Chemistry
C, 116(21):1171411721, 2012.
[70] Scalise, E., Houssa, M., Pourtois, G., Afanas'ev, V., and Stesmans, A. Strain-induced
semiconductor to metal transition in the two-dimensional honeycomb structure of mos2.
Nano Research, 5(1):4348, 2012.

37
[71] Jiang, J.-W., Qi, Z., Park, H. S., and Rabczuk, T. Elastic bending modulus of single-
layer molybdenum disulde (mos2): nite thickness eect. Nanotechnology, 24(43):
435705, 2013.
[72] Blakslee, O., Proctor, D., Seldin, E., Spence, G., and Weng, T. Elastic constants of
compression-annealed pyrolytic graphite. Journal of Applied Physics, 41(8):33733382,
1970.
[73] Sánchez-Portal, D., Artacho, E., Soler, J. M., Rubio, A., and Ordejón, P. Ab initio
structural, elastic, and vibrational properties of carbon nanotubes. Physical Review B,
59(19):12678, 1999.
[74] Liu, F., Ming, P., and Li, J. Ab initio calculation of ideal strength and phonon instability
of graphene under tension. Phys. Rev. B, 76:064120, 2007.
[75] Tu, Z.-c. and Ou-Yang, Z.-c. Single-walled and multiwalled carbon nanotubes viewed
as elastic tubes with the eective young's moduli dependent on layer number. Phys.
Rev. B, 65:233407, 2002.
[76] Jiang, J.-W., Wang, J.-S., and Li, B. Young's modulus of graphene: A molecular
dynamics study. Phys. Rev. B, 80:113405, Sep 2009.
[77] Brenner, D. W. Empirical potential for hydrocarbons for use in simulating the chemical
vapor deposition of diamond lms. Phys. Rev. B, 42:94589471, 1990.
[78] Alzebdeh, K. Evaluation of the in-plane eective elastic moduli of single-layered
graphene sheet. International Journal of Mechanics and Materials in Design, 8(3):
269278, 2012. doi: 10.1007/s10999-012-9193-7.
[79] Alzebdeh, K. I. An atomistic-based continuum approach for calculation of elastic prop-
erties of single-layered graphene sheet. Solid State Communications, 177:25  28, 2014.
[80] Scarpa, F., Adhikari, S., and Phani, A. S. Eective elastic mechanical properties of
single layer graphene sheets. Nanotechnology, 20(6):065709, 2009.
[81] Sakhaee-Pour, A. Elastic properties of single layered graphene sheet. Solid State Com-
munications, 149:9195, 2009.
[82] Akdim, B., Pachter, R., Duan, X., and Adams, W. W. Comparative theoretical study
of single-wall carbon and boron-nitride nanotubes. Phys. Rev. B, 67:245404, 2003.
[83] Kudin, K. N., Scuseria, G. E., and Yakobson, B. I. c2 F, bn, and c nanoshell elasticity
from ab initio computations. Phys. Rev. B, 64:235406, 2001.

38
[84] Verma, V., Jindal, V. K., and Dharamvir, K. Elastic moduli of a boron nitride nanotube.
Nanotechnology, 18(43):435711, 2007.
[85] Boldrin, L., Scarpa, F., Chowdhury, R., and Adhikari, S. Eective mechanical properties
of hexagonal boron nitride nanosheets. Nanotechnology, 22(50):505702, 2011.
[86] Oh, E. S. Elastic properties of boron-nitride nanotubes through the continuum lattice
approach. Materials Letters, 64(7):859  862, 2010.
[87] Mortazavi, B., Rahaman, O., Makaremi, M., Dianat, A., Cuniberti, G., and Rabczuk,
T. First-principles investigation of mechanical properties of silicene, germanene and
stanene. Physica E: Low-dimensional Systems and Nanostructures, 87:228  232, 2017.
[88] Woo, S., Park, H. C., and Son, Y.-W. Poisson's ratio in layered two-dimensional crystals.
Phys. Rev. B, 93:075420, 2016.
[89] Jiang, J.-W., Qi, Z., Park, H. S., and Rabczuk, T. Elastic bending modulus of single-
layer molybdenum disulde (mos 2 ): nite thickness eect. Nanotechnology, 24(43):
435705, 2013.
[90] Li, T. Ideal strength and phonon instability in single-layer mos 2. Physical Review B,
85(23):235407, 2012.
[91] Zakharchenko, K. V., Katsnelson, M. I., and Fasolino, A. Finite temperature lattice
properties of graphene beyond the quasiharmonic approximation. Phys. Rev. Lett., 102:
046808, Jan 2009.
[92] Liu, X., Metcalf, T. H., Robinson, J. T., Houston, B. H., and Scarpa, F. Shear modulus
of monolayer graphene prepared by chemical vapor deposition. Nano Letters, 12(2):
10131017, 2012.
[93] Bosak, A., Serrano, J., Krisch, M., Watanabe, K., Taniguchi, T., and Kanda, H. Elas-
ticity of hexagonal boron nitride: Inelastic x-ray scattering measurements. Phys. Rev.
B, 73:041402, 2006.
[94] Verma, V., Jindal, V. K., and Dharamvir, K. Elastic moduli of a boron nitride nanotube.
Nanotechnology, 18(43):435711, 2007.
[95] Ding, H., Zhen, Z., Imtiaz, H., Guo, W., Zhu, H., and Liu, B. Why are most 2d lattices
hexagonal? the stability of 2d lattices predicted by a simple mechanics model. Extreme
Mechanics Letters, 32:100507, 2019.
[96] Adhikari, S., Mukhopadhyay, T., and Liu, X. Broadband dynamic elastic moduli of hon-

39
 eycomb lattice materials: A generalized analytical approach. Mechanics of Materials,
157:103796, 2021.

40
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