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Strain Engineering for 2D Ferroelectricity in Lead
Chalcogenides
Tao Xu,* Xiaoyuan Wang, Jiawei Mai, Jingtong Zhang, Jie Wang, and Tong-Yi Zhang*
The quest for new 2D ferroelectric materials continues to arouse interest.
Based on first-principles calculations, here, 2D ferroelectric properties in
lead chalcogenides PbXs (X = S, Se, and Te) with a thickness of two atomic
layers via strain engineering is demonstrated. Although these materials
are stable in a rocksalt-type cubic structure and are intrinsically non­
ferroelectric materials, an appropriate mechanical strain can readily activate
a paraelectric to ferroelectric phase transition and induce in-plane electric
polarization in these atomic layers. The induced polarization magnitude
can be as large as 1.90 × 10−10 C m−1 at a biaxial strain of ε = 4.0%, which is
comparable in magnitude to that of ultrathin ferroelectric SnTe. The Curie
temperature Tc of the materials is also estimated using effective Hamilto-
nian simulations. The origin of the emerged ferroelectric phase is attributed
to softening of the polar mode with applied strain. In addition, the band
gaps of the crystals are found to be tunable with applied strain, which can
be adjusted to the ideal value of 1.3 eV for photovoltaic applications. The
results not only provide a new route to explore ferroelectricity in 2D mate-
rials but also suggest promising semiconducting ferroelectrics for solar
applications.
1. Introduction
Ferroelectrics, such as the perovskite PbTiO3 and its solid solu-
tions, are a typical class of functional materials that possess
not only switchable electric polarization but also superior func-
tionalities, including a large piezoelectric response and a high
dielectric permittivity.[1] These fascinating functionalities are
widely exploited for applications, including sensors, nonvolatile
Dr. T. Xu, J. Mai, Prof. T.-Y. Zhang
Materials Genome Institute
Shanghai University
Shanghai 200444, China
E-mail: xutao6313@shu.edu.cn; zhangty@shu.edu.cn
Dr. X. Wang
Key Laboratory of Pressure Systems and Safety
Ministry of Education, East China University of Science and Technology
Shanghai 200237, China
J. Zhang, Prof. J. Wang
Department of Engineering Mechanics
School of Aeronautics and Astronautics
Zhejiang University
Hangzhou 310027, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/aelm.201900932.
DOI: 10.1002/aelm.201900932
Adv. Electron. Mater. 2020, 6, 1900932 1900932  (1 of 7)
random-access memory (FeRAM), and
electromechanical devices.[2,3] Achieving
ferroelectric properties in low-dimensional
materials is of great importance for the
development of miniaturized, integrated
electronic devices as well as for the fun-
damental science attributed to the exotic
physical properties and the emergence of
unusual ferroic patterns.[4–7] However, the
ferroelectric order is inevitably destroyed
below the critical thickness in conven-
tional ferroelectrics, for example, 3–5 nm
for BaTiO3 nanostructures,[8,9] due to the
significantly enhanced depolarization
field and finite size effects at nanoscale
dimensions.
The rise of 2D materials opens a new
avenue for the discovery of atomic-scale
ferroelectrics.[10,11] From theoretical calcu-
lations, several 2D ferroelectric materials,
including compounds[12–14] and elemental
materials,[15,16] have been recently pro-
posed. In experiments, 2D ferroelectrics
were first established in two atomic layer
(AL)-thick SnTe,[17] which subsequently
stimulated research on the ferroelectricity (or ferroelasticity)
of other 2D SnTe analogues MXs (M = Si, Ge, Sn; X = S,
Se, Te).[12,13,18,19] Nevertheless, the lead chalcogenide PbX (X = S,
Se, and Te) atomic layers are intrinsically non­ferroelectric mate-
rials, although their corresponding bulk materials share the
same space group (Fm3m) as bulk SnTe at room temperature.
The discovery of new 2D ferroelectric materials and the under-
lying mechanism will not only provide a better understanding
of the physical mechanism behind the low-dimensional ferro-
electricity but also may facilitate the application of nanoscale
ferroelectric devices.
On the other hand, 2D materials are normally fabricated on
a substrate in practice, in which lattice mismatch and resulting
misfit strain are inevitably present. Strain engineering has been
proven to be a powerful tool in the control and modulation of
the structural, electronic, optical, and magnetic properties of 2D
materials.[20–23] In perovskite oxides, elastic strain has been rec-
ognized as a viable means to modify the structural instabilities
and induce ferroelectricity.[24] In this paper, we demonstrate, by
using first-principles calculations, that appropriate mechanical
strain can activate a paraelectric to ferroelectric phase transi-
tion in 2 AL-thick PbX films and modulate the resulting fer-
roelectric properties. The present results provide a prospective
means of achieving 2D ferroelectric materials in otherwise non­
ferroelectric materials and designing nanoscale devices.
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2. Results and Discussion
The initial configurations of the 2 AL PbXs were cleaved along
the (001) plane from the bulk PbXs. Due to the breaking of the
mirror symmetry along the [001] direction, the 2 AL PbXs are
reduced to P4/nmm space group from the Fm3m space group
of bulk materials. As illustrated in Figure  1a, the crystals con-
sist of two flat atomic layers with two Pb atoms and two X
atoms in a primitive unit cell in a square lattice. The primitive
cells of 2 AL PbXs were adopted to investigate their structural
properties. The optimized lattice constants, as illustrated by the
dashed black line, are a0  =  b0  = 4.23 Å, a0  =  b0  = 4.40 Å, and
a0  =  b0  = 4.64 Å for PbS, PbSe, and PbTe, in good agreement
with previous reports.[25,26] Furthermore, the PbX bond length
increases from PbS through PbSe to PbTe, consistent with the
growing atomic radius. These structures are different from
the closely related bi-layer SnTe (space group Pmn21), which
contains a relative in-plane displacement between Sn and Te
atoms.[18]
We then investigated the stability of the 2 AL PbX films. The
cohesive energies of the crystals, defined as Ec  = EPbX – EPb –
EX, were calculated, where EPbX is the total energy of 2 AL PbXs,
and EPb and EX are the energies of free Pb and X atoms, respec-
tively. The calculated cohesive energies are collected in Table 1.
Negative values indicate that formation of the atomic layers
is energetically favorable. The independent elastic constants
of the studied materials are also summarized in Table 1, in
which all three crystals meet the Born criteria for 2D materials:
C11C22 –C122 > 0 and C11, C22, C44 > 0.[27] This result indicates
that they can be mechanically stable. Furthermore, we also
verified the dynamic stabilities of these structures by calcu-
lating their phonon dispersions, and the results are provided in
Figure 1b and Figure S1, Supporting Information. It is notice-
able that the studied crystals are free of any imaginary phonon
modes within the Brillouin zone, indicating that all of them are
kinetically stable. Finally, AIMD simulations were performed
at 300 K to examine the thermal stability of the crystals. As
illustrated in Figure S2, Supporting Information, a snapshot of
the equilibrium structure indicates that the PbS atomic layer
remains nearly unchanged after a 5 ps simulation, and the total
energy of the simulation system only slightly fluctuates around
Figure 1.  a) Top view and side view of 2 AL PbX film. The dashed square denotes the primitive cell. The two basis vectors are denoted as a0 and b0.
b) Phonon dispersion curves of 2 AL PbS film.
Adv. Electron. Mater. 2020, 6, 1900932 1900932  (2 of 7)
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Table 1.  Calculated results of the lattice parameters, elastic constants,
and cohesive energies of 2 AL PbX films.
a0 = b0 [Å] C11 = C22 [GPa] C12 [GPa] C44 [GPa] Ec [eV]
PbS 4.23 25.8 13.7 17.1 −7.17
PbSe 4.40 19.3 6.1 9.8 −6.58
PbTe 4.64 18.8 10.8 17.1 −5.88
a constant value. All these results ensure the stability and plau-
sibility of the 2 AL PbX films, and these films are expected to
be experimentally fabricated considering that few-atomic-layer
PbXs have been successfully grown.[17,28,29]
Having confirmed the stability of atomic-thick PbXs, we turn
to the investigation of the ferroelectricity of these 2D systems.
Recent experiments have demonstrated strong in-plane ferroe-
lectricity in 2D SnTe,[17] attributed to the relative displacements
between Sn and Te atoms with different electronegativities.
Generally, a larger relative displacement implies a larger value
of the ferroelectric spontaneous polarization. Unlike in the 2D
SnTe material, the centres of the positive and negative charges
in the 2 AL PbXs coincide due to the absence of a relative
atomic displacement between Pb and X atoms. Consequently,
the PbXs preserve the inversion center and are intrinsically
nonferroelectric materials.
Mechanical strain is an effective tool to modulate the struc-
tural properties of 2D materials. We further investigated the
structural properties of 2 AL PbXs with respect to biaxial ten-
sile strain up to 8.0%. With their structures analogous to 2 AL
SnTe, we calculated the strain dependence of the total energy of
2 AL PbS in the centrosymmetric P4/nmm structure (denoted
as phase C) and the distorted Pmn21 structure (denoted as
phase A). The obtained results are depicted in Figure  2 and
Figure S3, Supporting Information. We can see that the A phase
is unstable and spontaneously relaxes to the C phase in all
three crystals without strain. However, for tensile strains larger
than 1.5%, the non-centrosymmetric A phase becomes energet-
ically favorable in PbS, indicating the transformation from the
C phase into the A phase. The A phase of PbS becomes notably
more stable with increasing strain. An analogous trend is also
observed in 2 AL PbSe and PbTe with the application of biaxial
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no appreciable imaginary-frequency modes are observed over

Figure 2.  Total energy of C and A phases versus biaxial strain in 2 AL
PbS film. The insets show the atomic structures of the C and A phases.
strain, as demonstrated in Figure S3, Supporting Informa-
tion, although the critical strains for this transition are larger
(i.e., ≈2.0% and 3.0% for PbSe and PbTe, respectively). We fur-
ther explicitly computed the full phonon dispersion curves of
the strained PbX atomic layers. As shown in Figure S4, Sup-
porting Information, for PbS under 4.0% strain as an example,
the entire Brillouin zone in the polar phase, which confirms
that the distorted structure is indeed the ground state. More-
over, our AIMD simulations also demonstrate that the strained
films remain intact at finite temperature, as illustrated in Figure
S5, Supporting Information. Therefore, the biaxial strain leads
to breaking of the structural centrosymmetry, which is the nec-
essary condition for spontaneous polarization.
The lattice distortion of crystals was quantified by the vector
d, defined as the off-center displacement of the Pb atom, that
is, the relative in-plane displacement between neighboring Pb
and S atoms, as illustrated in Figure 3a. The centrosymmetric
C phase corresponds to d  = 0 with four equivalent in-plane
PbS bonds, which forbids the formation of ferroelectricity,
while the A phase has a nonzero value of d, and the two cova-
lent PbS bonds denoted by white lines are strengthened,
leading to breaking of the inversion symmetry. Upon reversion,
the A phase can transform to the energy degenerate ground-
state A′ phase with opposite d. As a result, the A and A′ phases
are expected to have opposite polarizations. The evolution of
the atomic distortion of 2 AL PbS with applied strain is shown
in Figure 3b. It is evident that the distortion displacement
increases as a function of strain. Similar behaviors can also be
found in PbSe and PbTe films (see Figure S6, Supporting Infor-
mation), in which the induced polar distortions are slightly

Figure 3.  a) Top view of the atomic structures and charge density distributions of two energy-degenerated distorted phases (A and A´) and the cen-
trosymmetric C phase. The arrows and white lines indicate the directions of electric polarization and the covalent Pb–S bonds, respectively. b) Polar dis-
tortions of 2 AL PbS as a function of biaxial strain. c) Double-well potential of 4.0% strained 2 AL PbS film along the normalized distortion displacement.

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Figure 4.  a) Polarization of 2 AL PbS film versus biaxial strain. b) Minimum energy pathway and activation barrier for the transformation between two
ferroelectric phases (A and A´) in the 2 AL PbS film with 4.0% strain.
smaller than the corresponding values in PbS under an equiva-
lent strain amplitude. The variation in the energy of strained
2 AL PbS (ε = 4.0%) with respect to the normalized distortion
displacement was also calculated, and the results are plotted in
Figure 3c, which clearly shows double well potential character-
istics. This result further suggests the existence of ferroelectric
polarization.
The spontaneous polarization of the strained films was
confirmed and evaluated using the modern Berry phase
method,[30,31] which takes into account the electronic and ionic
contributions. We find that the distorted (A and A′) phases
have opposite spontaneous polarizations along the in-plane
(100) direction. The evolution of the calculated polarization of
2 AL PbS with biaxial strain is depicted in Figure  4a, which
increases with increasing applied strain. Specifically, 2 AL PbS
has a large spontaneous polarization of 1.90 × 10−10 C m−1
at a strain of ε  = 4.0%. This value is comparable to those in
ultrathin ferroelectric SnTe (≈10−10 C m−1[18]) and GeSe (1.6 ×
10−10 C m−1[32]). PbSe and PbTe films under this strain also
exhibit polarization with the same order of magnitude. The
activated ferroelectric polarization is expected to be detected in
experiments, as has been done for the 2D ferroelectric SnTe,
due to their comparable polarizations. Furthermore, to evaluate
the feasibility of polarization conversion, the nudged elastic
band (NEB) method[33] was used to compute the minimum
energy pathway and the activation barrier in the ferroelectric
transition of PbS film, in which the initial and final structures
were set as the A and A′ phases, respectively (see Figure 4b).
The calculated energy barrier is approximately 23 meV per
unit cell, which is close to that in SnTe[18] and comparable to
that of the conventional ferroelectric BaTiO3 (18 meV/f.u.).[34]
Similarly, we obtain energy barriers of 22 and 16 meV for PbSe
and PbTe films at a strain of 4.0%. These small values indi-
cate that polarization reversal can be easily achieved under an
external electric field, which is beneficial for energy efficient
ferroelectric devices. It is worth mentioning that ferroelectric
grain boundaries can further decrease the transition barrier
and make the polarization switching easier due to the disconti-
nuity in the polarization and the depolarizing field induced by
the boundaries.[35]
To assess the stability of the emerging ferroelectricity, we fur-
ther employed the Monte Carlo (MC) method to estimate the
Curie transition temperature Tc of 2 AL PbS, above which elec-
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tric polarization vanishes. Following the approach in previous
studies,[18,19,36] we constructed the free energy of the PbS super-
cell expressed in the Landau–Ginzburg expansion in terms of
the polarization:
E = ∑ i ( Api2 + Bpi4 + Cpix2 piy2 ) + ∑ ijαβ J ijαβ piα p jβ (1)
Here, pi is the polar distortion of the local unit cell i including
components of pix and piy, and A, B and C are constant param-
eters. The first three energy terms represent the anharmonic
double-well potential, as shown in Figure 3c. The last term
describes the coupling effect between the nearest-neighbor
local modes i and j, in which interaction parameter Jijαβ (i and
j represent the local modes, and α and β represent directions)
can be derived by fitting the DFT results using mean-field
theory.[37] Taking PbS at strains of 4.0% and 8.0% as examples,
we fitted all the related coefficients and list them in Table S1,
Supporting Information. With the established effective Hamil-
tonian model, we then performed MC simulations to investi-
gate the ferroelectric phase transition. As illustrated in Figure
S7, Supporting Information, the Tc of 2 AL PbS with 4% strain
is estimated to be ≈130 K and is increased to about 300 K with
8% strain. These values are larger than the result predicted in
defect-free 2 AL SnTe film (i.e., 30 K),[38] which suggests the fer-
roelectric state is more stable in the 2D PbX structures.
We now discuss the origin of the ferroelectric polarization
in the 2 AL PbXs with biaxial strain. The ferroelectricity in con-
ventional perovskite ferroelectrics with the displacive transition
is usually associated with softening of the polar optical modes
in the undistorted paraelectric structure.[39] The polar optical
modes become unstable in the high-symmetry paraelectric
phase and are condensed due to their imaginary frequencies,
which causes ferroelectric distortion. Taking the 2 AL PbS at
a strain of ε = 3.0% as an example, we plot the phonon disper-
sion curve of its centrosymmetric structure in Figure  5a. One
can see that this undistorted structure exhibits pronounced
structural instability around the Γ point, as denoted by the
imaginary (negative) frequency. This unstable mode has a
doubly degenerate Eu symmetry. Its real-space eigendisplace-
ment manifests as a relative displacement between adjacent
Pb and S atoms along the [100] or [010] directions, thus corre-
sponding to the ferroelectric soft mode. This soft mode tends to
break the structural centrosymmetry and yields the ferroelectric
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Figure 5.  a) Phonon dispersion curves of centrosymmetric 2 AL PbS film at 3.0% strain. The inset shows the real-space eigendisplacements of the
doubly degenerate unstable mode in the zone centre. b) Frequency of the polar distortion of 2 AL PbS film versus biaxial strain.

ground state in the strained PbS film. Note that there is a pro- 2 AL PbS without strain is shown in Figure S10, Supporting
nounced imaginary frequency at the R point, which is associ- Information, which shows semiconductor characters with a
ated with antiferroelectric (AFE) distortion. However, the AFE band gap of about 1.22 eV. This value is consistent with pre-
state is metastable and higher in energy (e.g., 20.5 meV at a vious reports[45,46] and is larger than that of its bulk counter-
strain of 4.0%) than the ferroelectric ground state. The frequen- part (i.e., about 0.5 eV[47]). The variation of the band gaps of
cies of the polar mode in 2 AL PbS versus strain are depicted PbS, PbSe, and PbTe versus biaxial strain are also shown in
in Figure 5b. We clearly see that the frequencies are strongly Figure  6. It is well known that the traditional ferroelectric
strain dependent and that the onset of softening occurs at a photovoltaic materials suffer from large band gap and thus
critical strain of ≈ε = 1.5%, which produces the structural phase have low energy conversion efficiency. Surprisingly, the band
transition from the paraelectric C phase to the ferroelectric A gaps of PbX films in the current study are generally close to
(or A′) phase. This phonon mode is increasingly softened with 1.0 eV and are increased by the application of biaxial strain.
increasing strain such that the polar distortion is increasingly In particular, the PbS film with 4.0% strain has a band gap of
preferred. A similar strain-induced soft polar mode is also 1.35 eV, which is the ideal value of band gap for photovoltaic
observed in PbSe and PbTe films. applications. Since ferroelectric polarization and suitable band
The above results thus demonstrate that biaxial strain gap are two key properties in photovoltaic devices, our strategy
can trigger the paraelectric to ferroelectric transition due of strain engineering in lead chalcogenides further provides
to the frozen of the polar mode and effectively modulate the a means for excellent 2D ferroelectric photovoltaic materials.
ferroelectric properties in 2 AL PbXs. Note that 2D materials Despite the challenge in the synthesis of 2D group IV chal-
have superior mechanical flexibility and can sustain much cogenides at this moment, 2 AL SnTe film and few-atomic-
higher strain than their bulk counterparts, for example, ≥25% layer PbXs have been successfully grown in experiments.[17,29]
in some 2D materials.[40] The biaxial strain in the present study We hope that our prediction can stimulate further experi-
can be introduced by choosing suitable substrates, such as Si mental work on this class of crystals to design atomic scale
and Ni,[41] in practice. It can also be intentionally imposed and ferroelectrics and high-efficiency ferroelectric photovoltaic
controlled by defects,[42] functional wrapping,[43] or even direct nanodevices.
mechanical application.[44] In addition to under biaxial strain,
the paraelectric to ferroelectric phase transition in 2 AL PbX
films can also occur in different strain states. The [100] uniaxial
strain above a certain level, for instance, also breaks the original
P4/nmm symmetry of PbX films and leads to the ferroelectric
Pmn21 phase with polarization along the [100] direction. As
illustrated in Figure S8, Supporting Information, the critical
uniaxial strains for the ferroelectric phase transitions are ≈2.5%,
3.0%, and 4.0% for PbS, PbSe, and PbTe, respectively. The polar-
ization of the films versus uniaxial strain was also calculated,
and the results are shown in Figure S9, Supporting Informa-
tion. For instance, the ferroelectric polarization of 2 AL PbS at
a uniaxial strain of 4.0% is 1.42 × 10−10 C m−1, which is slightly
smaller than the corresponding value of 1.90 × 10−10 C m−1
at the same biaxial strain. All these results demonstrate the
effective tuning of ferroelectricity by the application of strain
engineering.
To further improve the understanding of the electronic
properties of the thin films, we calculated the electronic den-
sity of states (DOS) of all the investigated crystals. The DOS of Figure 6.  Band gaps of 2 AL PbX films versus biaxial strain.

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3. Conclusion
In summary, we have proposed a strain engineering approach
for realizing 2D ferroelectricity in nonferroelectric 2 AL PbX
films based on DFT calculations. The atomic structures and
physical properties of the crystals were explored, and their sta-
bilities were confirmed by cohesive energy calculations, ab initio
molecular dynamics simulations, and phonon-spectrum calcula-
tions. The strain-free atomic layers are characterized by a par-
aelectric P4/nmm structure. As the applied strain is increased,
PbS, PbSe, and PbTe in turn transform into a ferroelectric phase
with in-plane electric polarization. The emerging ferroelectricity
is enhanced with increasing strain. The strain dependence of
phonon modes in 2 AL PbXs was also studied to clarify the origin
of the electric polarization. Moreover, our work also reveals that
the strained PbX films are promising ferroelectric photovoltaic
(PV) materials because of their notable ferroelectric polarization
and suitable band gap. The present results provide great oppor-
tunities for realizing a ferroelectric phase in low-dimensional
materials and designing multifunctional nanoscale devices.
4. Experimental Section
The first-principles calculations were conducted based on density
functional theory (DFT), as implemented in the Vienna Ab initio
Simulation Package.[48,49] The generalized gradient approximation
(GGA)[50] of the Perdew–Burke–Ernzerhof (PBE)[51] form was employed
for the exchange-correlation functional. The kinetic energy cutoff was set
to 400 eV, and the Monkhorst–Pack k-point scheme[52] with a size of 12
× 12 × 1 was used for the Brillouin zone integrations. To avoid spurious
interactions due to the periodic boundary condition, a vacuum space of
20 Å normal to the layer plane was applied. The atomic positions were
fully optimized until the Hellmann–Feynman force on each atom was
less than 0.001 eV Å−1. The phonon dispersion was studied using the
finite displacement method implemented in the Phonopy package,[53]
and the ferroelectric polarization was calculated by the Berry phase
approach.[30,31] A 7 × 7 × 1 supercell containing 196 atoms and k-mesh
grids of 1 × 1 × 1 were used in the phonon spectra calculations. Ab
initio molecular dynamics (AIMD) simulations with the NVT ensemble
and Nosé–Hoover thermostat were carried out to assess the thermal
stability of the crystals. For the modeling of epitaxial 2 AL PbX films, a
biaxial strain, defined as ε11 =  ε22 = (a–a0)/a0 = (b–b0)/b0, was imposed
by constraining the in-plane lattice parameters a and b, where a0 and b0
are the equilibrium lattice constants.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
The authors acknowledge the financial support from the National
Natural Science Foundation of China (Grant No. 11802169 and No.
11602252) and Fundamental Research Funds for the Central Universities
(Grant No. 50321071915017).
Conflict of Interest
The authors declare no conflict of interest.
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Author Contributions
T.X. and X.Y.W. contributed equally to this work. T.X. conceived the
project, designed and directed computational experiments, and wrote
the entire manuscript. X.Y.W. and J.W.M. supported the calculations and
discussed the results. J.T.Z. and J.W. conducted the MC calculations and
discussed the results. T.Y.Z. supervised the work and provided critical
feedback on the manuscript. All authors read and commented on the
manuscript.
Keywords
2D materials, ferroelectric photovoltaic materials, ferroelectricity, strain
engineering
Received: August 30, 2019
Revised: September 30, 2019
Published online: November 18, 2019
[1] M. E. Lines, A. M. Glass, Principles and Applications of Ferroelectrics
and Related Materials, Clarendon Press, Oxford, UK 1979.
[2] R. Ramesh, Thin Film Ferroelectric Materials and Devices, Kluwer Aca-
demic, Boston, MA 1997.
[3] J. F. Scott, Ferroelectric Memories, Springer, Berlin, Germany 2000.
[4] T. Shimada, T. Xu, Y. Uratani, J. Wang, K. Kitamura, Nano Lett. 2016,
16, 6774.
[5] Y. Nahas, S. Prokhorenko, L. Louis, Z. Gui, I. Kornev, L. Bellaiche,
Nat. Commun. 2015, 6, 8542.
[6] R. Mazumder, D. P. Sujatha, D. Bhattacharya, P. Choudhury, A. Sen,
M. Raja, Appl. Phys. Lett. 2007, 91, 062510.
[7] J. Liu, Y. Ji, S. Yuan, L. Ding, W. Chen, Y. Zheng, npj Comput. Mater.
2018, 4, 78.
[8] M. J. Polking, M.-G. Han, A. Yourdkhani, V. Petkov, C. F. Kisielowski,
V. V. Volkov, Y. Zhu, G. Caruntu, A. P. Alivisatos, R. Ramesh, Nat.
Mater. 2012, 11, 700.
[9] I. I. Naumov, L. Bellaiche, H. Fu, Nature 2004, 432, 737.
[10] C. Cui, F. Xue, W.-J. Hu, L.-J. Li, npj 2D Mater. Appl. 2018, 2, 1.
[11] M. Wu, P. Jena, Wiley Interdiscip. Rev.: Comput. Mol. Sci. 2018, 8,
e1365.
[12] M. Wu, X. C. Zeng, Nano Lett. 2016, 16, 3236.
[13] H. Wang, X. Qian, 2D Mater. 2017, 4, 015042.
[14] S. Shen, C. Liu, Y. Ma, B. Huang, Y. Dai, Nanoscale 2019, 11,
11864.
[15] C. Xiao, Adv. Funct. Mater. 2018, 28, 1707383.
[16] Y. Wang, C. Xiao, M. Chen, C. Hua, J. Zou, C. Wu, J. Jiang,
S. A. Yang, Y. Lu, W. Ji, Mater. Horiz. 2018, 5, 521.
[17] K. Chang, J. Liu, H. Lin, Na. Wang, K. Zhao, A. Zhang, F. Jin,
Y. Zhong, X. Hu, W. Duan, Q. Zhang, L. Fu, Q.-K. Xue, X. Chen,
S.-H. Ji, Science 2016, 353, 274.
[18] W. Wan, C. Liu, W. Xiao, Y. Yao, Appl. Phys. Lett. 2017, 111, 132904.
[19] R. Fei, W. Kang, L. Yang, Phys. Rev. Lett. 2016, 117, 097601.
[20] M. Wu, H. Fu, L. Zhou, K. Yao, X. C. Zeng, Nano Lett. 2015, 15,
3557.
[21] D.-B. Zhang, S.-H. Wei, npj Comput. Mater. 2017, 3, 32.
[22] I. Niehues, R. Schmidt, M. Drüppel, P. Marauhn, D. Christiansen,
M. Selig, G. Berghäuser, D. Wigger, R. Schneider, L. Braasch,
R. Koch, A. Castellanos-Gomez, T. Kuhn, A. Knorr, E. Malic,
M. Rohlfing, S. M. de Vasconcellos, R. Bratschitsch, Nano Lett.
2018, 18, 1751.
[23] C. Long, Y. Dai, Z.-R. Gong, H. Jin, Phys. Rev. B 2019, 99, 115316.
[24] D. G. Schlom, L.-Q. Chen, C. J. Fennie, V. Gopalan, D. A. Muller,
X. Pan, R. Ramesh, R. Uecker, MRS Bull. 2014, 39, 118.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
[25] X.-B. Li, P. Guo, Y.-N. Zhang, R.-F. Peng, H. Zhang, L.-M. Liu,
J. Mater. Chem. C 2015, 3, 6284.
[26] X. Zhang, Z. Yang, Y. Chen, J. Appl. Phys. 2017, 122, 064101.
[27] M. Born, K. Huang, Dynamical Theory of Crystal Lattices, Clarendon
Press, Oxford, UK 1954.
[28] G. B. Bhandari, K. Subedi, Y. He, Z. Jiang, M. Leopold, N. Reilly,
H. P. Lu, A. T. Zayak, L. Sun, Chem. Mater. 2014, 26, 5433.
[29] S. Khan, Z. Jiang, S. M. Premathilka, A. Antu, J. Hu, A. A. Voevodin,
P. J. Roland, R. J. Ellingson, L. Sun, Chem. Mater. 2016, 28, 5342.
[30] R. D. King-Smith, D. Vanderbilt, Phys. Rev. B 1993, 47, 1651.
[31] R. Resta, Rev. Mod. Phys. 1994, 66, 899.
[32] S. Guan, C. Liu, Y. Lu, Y. Yao, S. A. Yang, Phys. Rev. B 2018, 97, 144104.
[33] G. Henkelman, B. P. Uberuaga, H. Jónsson, J. Chem. Phys. 2000,
113, 9901.
[34] R. E. Cohen, Nature 1992, 358, 136.
[35] W. Shu, J. Wang, TY. Zhang, J. Appl. Phys. 2012, 112, 064108.
[36] W. Zhong, D. Vanderbilt, K. M. Rabe, Phys. Rev. Lett. 1994, 73,
1861.
[37] W. Zhong, D. Vanderbilt, K. M. Rabe, Phys. Rev. B 1995, 52, 6301.
[38] K. Liu, J. L. Lu, S. Picozzi, L. Bellaiche, H. J. Xiang, Phys. Rev. Lett.
2018, 121, 027601.
Adv. Electron. Mater. 2020, 6, 1900932 1900932  (7 of 7)
www.advelectronicmat.de
[39] H. Uwe, T. Sakudo, Phys. Rev. B 1976, 13, 271.
[40] K. S. Kim, Y. Zhao, H. Jang, S. Y. Lee, J. M. Kim, K. S. Kim, J.-H. Ahn,
P. Kim, J.-Y. Choi, B. H. Hong, Nature 2009, 457, 706.
[41] Z. Fu, M. Liu, Z. Yang, Phys. Rev. B 2019, 99, 205425.
[42] L. Seravalli, M. Minelli, P. Frigeri, P. Allegri, V. Avanzini, S. Franchi,
Appl. Phys. Lett. 2003, 82, 2341.
[43] X. L. Wu, F. S. Xue, Appl. Phys. Lett. 2004, 84, 2808.
[44] Y. G. Wang, Q. L. Zhang, T. H. Wang, W. Han, S. X. Zhou, J. Phys. D:
Appl. Phys. 2011, 44, 125301.
[45] W. Wan, Y. Yao, L. Sun, C.C. Liu, F. Zhang, Adv. Mater. 2017, 29,
1604788.
[46] X. B. Li, P. Guo, Y. N. Zhang, R. F. Peng, H. Zhang, L. M. Liu,
J. Mater. Chem. C 2015, 3, 6284.
[47] W. Li, Q. Y. He, Y. Z. Wang, T. Wang, Chem. Phys. Lett. 2017, 687,
101.
[48] G. Kresse, J. Hafner, Phys. Rev. B 1993, 47, 558.
[49] G. Kresse, J. Furthmüller, Phys. Rev. B 1996, 54, 11169.
[50] S. Grimme, J. Comput. Chem. 2006, 27, 1787.
[51] M. Ernzerhof, G. E. Scuseria, J. Chem. Phys. 1999, 110, 5029.
[52] H. J. Monkhorst, J. D. Pack, Phys. Rev. B 1976, 13, 5188.
[53] A. Togo, F. Oba, I. Tanaka, Phys. Rev. B 2008, 78, 134106.
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim