Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133

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Physica E: Low-dimensional Systems and Nanostructures

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

Monte Carlo simulation of dieletric properties of the antiferroelectric/ T

ferroelectric BiFeO3/YMnO3 bilayer in the external electric field
Ze-yuan Wang, Wei Wang∗, Qi Li, Ming Tian, Zhong-yue Gao, Ying Liu
School of Science, Shenyang University of Technology, Shenyang, 110870, China

A R T I C LE I N FO A B S T R A C T

Keywords: Monte Carlo simulation has been used to study the dielectric properties of an antiferroelectric/ferroelectric Ising
Antiferroelectric/ferroelectric bilayer bilayer structure which consists of the top layer with spin-5/2 and the bottom layer with spin-2. The effects of
Polarization the crystal-fields, the exchange couplings and the external electric field on the polarization, the dielectric sus-
Dielectric susceptibility ceptibility, the internal energy, the specific heat and the blocking temperature of the mixed-spin bilayer system
Blocking temperature
have been examined detailedly. In particular, the phase diagrams of the blocking temperature under the effects
Internal energy
Monte Carlo
of various physical parameters are obtained for the present system. Through a comparison, there is in agreement
between our results obtained and other theoretical studies as well as experimental results.

1. Introduction dielectric and magnetic properties of the multiferroic bilayers in the

In the last decade, the multiferroic bilayer has become the focus of
magnetoelectric materials due to its excellent magnetic and electrical
properties. Among these, the BiFe03/YMn03 bilayer has a higher fer-
roelectric and antiferroelectric transition temperature than room tem-
perature [1–3], which has enlarged its potential prospect in many
fields, such as magnetoelectric read head [4], magnetic field sensors
[5–7], memory devices and so on [8–10].
Experimentally, the exploration of the multiferroic bilayer has re-
ceived great interests. The multiferroic bilayer has been manufactured
by diverse methods at present and many researchers have studied its
physicial properties. By means of magnetron sputtering technique,
Zapata et al. have studied the electric and magnetic properties of the
multiferroic BiFeO3 and YMnO3 thin films [11]. The effects of the de-
position temperature upon the crystalline structure, surface mor-
phology, magnetization, and electrical polarization of BiFeO3 and
YMnO3 thin films have been discussed in detailed. Using the pulsed
laser deposition, Nie et al. have researched the epitaxial growth and
multiferroic properties of the (001)-oriented BiFeO3/YMnO3 bilayer
films [12]. Much progress has been made in the series of the multi-
ferroic bilayers such as BiFeO3/YMnO3 [13–15], Pb(Zr,Ti)O3/CoFe2O4
[16,17], BaTiO3/CoFe2O4 [18,19], BiFeO3/NiFe [20,21], BiFeO3/
CoFe2O4 [22], BiFeO3/Bi4Ti3O12 [23].
On the other hand, theoretical interpretation can lay the foundation
for experimental evidences. Up to now, a great number of theoretical
models and numerical methods have been devoted to exploring the
external electric field [24–28]. With a simple model of superlattices,
ONG et al. have studied the intermixing and magnetoelectric coupling
in ferroelectric/multiferroic bilayer [29]. The effects of the intermixing
and magnetoelectric coupling on multiferroic phase transitions in the
ferroelectric/multiferroic superlattices have been discussed. By the
mean-field approximation (MFA), Li et al. have researched the im-
portance of the magnetoelectric coupling in a three-sublattice multi-
ferroics bilayers [30]. The temperature dependence of magnetization,
magnetic susceptibility and magnetoelectric susceptibility under dif-
ferent coupling strengths are calculated. By a two-dimensional model,
Zhang et al. have studied The static and frequency-dependant magne-
toelectric effects in the functionally graded multiferroic bilayers [31].
By the effective field theory (EFT), Ainane et al. have studied the effects
of the interfacial coupling and the transverse field on the hysteresis
behaviors and susceptibility of the ferroelectric/antiferroelectric bi-
layer [32]. By the use of the EFT, Benhouria et al. have researched
pyroelectric, dielectric properties and hysteresis loops of a ferroelectric
bilayer system described by the transverse Ising model with long-range
interactions [33]. It is discovered that the critical temperature increases
with the antiferroelectric interfacial coupling increasing. Based on first-
principles calculations, Duan et al. have studied the predicted magne-
toelectric effect and ferroelectric controlling of magnetism in Fe/
BaTiO3 multilayers. Its origin is a change in bonding at the ferroelectric-
ferromagnet interface that alters the interface magnetization when the
electric polarization reverses [34]. These above theoretical studies have
demonstrated the significance of the exchange coupling, the crystal-

∗
Corresponding author.
E-mail address: weiwang@sut.edu.cn (W. Wang).

https://doi.org/10.1016/j.physe.2019.02.022
Received 28 November 2018; Received in revised form 24 January 2019; Accepted 18 February 2019
Available online 18 February 2019
1386-9477/ © 2019 Elsevier B.V. All rights reserved.
Z.-y. Wang, et al.
field, and the electric field in dominating the dielectric and magnetic
properties of the multiferroic bilayers.
In recent years, the mixed-spin (2, 5/2) Ising system is one of the
most widely studied mixed-spin Ising systems. On the one hand, this
model can provide the proper theoretical models for the molecular-
based magnetic materials [35–39]. On the other hand, it has been used
to understand the magnetic and thermodynamic properties of some
low-dimensional magnetic materials such as nanoislands [40,41], Ke-
kulene structure [42]. By dynamic mean-field calculations, Mehmet
Ertas have studied the dynamic hysteresis behaviors of the two-di-
mensional mixed-spin (2, 5/2) ferrimagnetic Ising model in an oscil-
lating magnetic field [43]. It is worth noting that this structure is the-
oretically constructed into a double-layer honeycomb lattice. By using
the Monte Carlo simulation, Yasuyuki et al. have studied a mixed spin-2
and spin-5/2 Ising system on a honeycomb lattice [44,45]. Recently,
much attention has been also paid to the graphene systems with hon-
eycomb structure [46–50].
Electrical phenomena are closely related to magnetic phenomena in
solid physics. One can understand the electrical behavior from the
concept of magnetism. There are many relationships between electrical
and magnetic quantities such as polarizability and magnetization, si-
milar hysteresis behaviors and definition of the susceptibility both in
the electric and magnetic field. But the only difference between them is
different external field, one is the electric field E and the other is the
magnetic field h. Theoretically, the magnetic properties of the core-
shell systems have been studied, which also inspire the researchers to
explore the dielectric properties of these nano-systems, such as nanor-
ibbon [51], nanowire [52,53], nanoparticle [54]. Monte Carlo simula-
tion has been applied to investigate the dielectric and polarization in
two-dimensional ferroelectric or ferro-antiferroelectric materials
[55–57]. It is worth mentioning that a recent Monte Carlo study has
concentrated on the ferroelectric/antiferroelectric BiFeO3/YMnO3 bi-
layer [58]. In the BiFeO3/YMnO3 bilayer, the spin values of Fe and Mn
atoms are 5/2 and 2, respectively. And studies have shown that, there is
the antiferroelectric exchange couping between two Fe atoms in the
BiFeO3 layer, while the ferroelectric exchange coupling exist between
the Mn atoms in another YMnO3 layer. Therefore, a mixed-spin (2, 5/2)
Ising model can be used to describe the ferroelectric/antiferroelectric
BiFeO3/YMnO3 bilayer system. The results revealed that the crystal-
field, the exchange coupling, the external electric field, longitudinal
field and the temperature have a profound impact on the electrical and
magnetic properties of the multiferroic bilayer system.
In our previous work, we have also used successfully the MC method
to study the magnetic and thermodynamic properties of the low-di-
mensional magnetic materials, such as graphene bilayer [59], gra-
phene-nanoribbon [60], nanoparticle [61], nanowire [62] and nanois-
land [63,64]. As far as we know, little research has been conducted on
the ferroelectric/antiferroelectric BiFeO3/YMnO3 bilayer with the co-
existence of the crystal-field and the external electric field. In parti-
cular, the internal energy and specific heat have been scarcely reported,
which inspires us to study the following research. The main work of this
paper is to study the effects of exchange coupling, external electric
field, temperature and crystal-field on the polarization, dielectric sus-
ceptibility and thermodynamic properties of the antiferroelectric/fer-
roelectric bilayer structure. In Sec. 2, we describe the Hamiltonian of
the system and the calculation procedure of Monte Carlo simulation. In
Sec. 3, we shall show typical simulation results for the polarization,
dielectric susceptibility, blocking temperature, internal energy and
specific heat. The third part is the analysis result and discussion. The
summary is given in Sec. 4.
2. Model and Monte Carlo simulation
We consider a three-dimensional antiferroelectric/ferroelectric bi-
layer on the honeycomb structure in Fig. 1, which can represent the
multiferroic BiFeO3/YMnO3 bilayer in experiment. The ferroelectric
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Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133
Fig. 1. Antiferroelectric/ferroelectric Ising bilayer structure with the honey-
comb structure has been defined here. J1 and J2 represent the intralayer anti-
ferroelectric and ferroelectric exchange couplings of different spins in the top
layer (↑↓, σ = 5/2) and bottom layer (↑↑, S = 2), respectively. J3 denotes the
interlayer exchange coupling between layers.
atoms of the top layer (BiFeO3) are Fe atoms with spin-5/2, and those in
the bottom layer (YMnO3) are Mn atoms with spin-2. As is well-known,
the Ising model can express the only component of the Z-axis direction
of the spin so that it is simpler to be implemented than the three-di-
mensional Heisenberg model, in which the spins are along the direc-
tions of x-, y-, z-axes. On the other hand, More importantly, Heisenberg
model presents generally the information of the thermodynamic
quantities at low temperature. As a result, it is difficult for Heisenberg
model to provide the phase transition temperature in the magnetization
vs. temperature curve. On the contrary, the Ising model can give the
information of the whole temperature region including the phase
transition point. In this work, because we consider the effects of the
longitudinal crystal-fields and external electric field, the extended
mixed-spin Ising model can be used properly to describe such anti-
ferroelectric/ferroelectric Ising bilayer. It is worth mentioning that the
Ising model has been wildly used to describe the various bilayer systems
and explain the electric and magnetic properties of the bilayers in re-
cent Monte Carlo studies [47,48,58,59]. The Hamiltonian of the bilayer
system is expressed as:
H = −J1 ∑ σiAz σ jB
z
− J2 ∑ z
SmC z
SnD − J3 ∑ σiAz (jB) SmC
z
(nD)
< i, j > < m, n > < i (j ), m (n) >
− D1 ∑ (σiAz (jB) )2 − D2 ∑ z
(SmC (nD) )
2
i (j ) m (n)
− 2μE ( ∑ σiAz (jB) + ∑ z
SmC (nD) )
i (j ) m (n) (1)
where, < i,j > , < m,n > , < i(j),m(n) > represent the summation over
all of spin pairs of the nearest sublattices within the top layer, bottom
layer, and between the top and bottom layers, respectively.
σiAz, σ jB
z z
, SmC z
, SnD represent the spin components of different sublattices
in each layer along the z-axis direction.σiz(j) = ± 5/2,± 3/2,± 1/2 re-
presents the spin operator of sublattices A and B in the top layer, and
Smz (n) = ± 2, ± 1,0 represents those of sublattices C and D in the bottom
layer. J1 and J2 are the intralayer exchange couplings between sub-
lattices A(C) and B(D) in the top and bottom layers, and J3 is the in-
terlayer exchange coupling between sublattices A(B) and C(D). D1 and
D2 are the crystal-fields for sublattices A(B) and C(D), respectively.
Finally, E is the external electric field, and μ is the dipole moment. For
simplicity, μ = 1.0 for our simulation.
In this work, the Monte Carlo simulation we used is the standard
single-spin-flip importance method based on the Metropolis algorithm
[65]. As shown in Fig. 1, the bilayer system contains N × L spins of the
Z.-y. Wang, et al. Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133

sublattices, where N and L are defined as the number of spins in each

layer and the thickness of the bilayer (L = 2), respectively. Additional
simulations have also been done for the choice of N from 50 to 100. But,
we can not find significant difference. Accordingly, we choose N = 50
for the simulation. We apply the periodic boundary condition in xy
plane, while the free boundary condition is used along z direction. As a
guarantee, not less than 104 Monte Carlo steps (MCS) per site were cut
off to maintain the equilibrium of the system before averaging thermal
quantities over the next 2 × 104 MCS. The error bars were calculated
with a Jackknife method [66,67] by taking all the measurement and
grouping them into 10 blocks.
The internal energy of the system per site is:
1
U= < H>
N (2)

The polarizations P1, P2, P3 and P4 of sublattices A, B, C and D in the

top and bottom layers:
2 Z
P1 = N
〈 ∑i σiA 〉
2 Z
P2 = N
〈 ∑j σ jB 〉 Fig. 2. The temperature dependences of the total polarization P, the sublattice
2 z
polarizations P1, P2, P3, P4 and the total dielectric susceptibility χ for the anti-
P3 = N
〈 ∑m SmC 〉 ferroelectric/ferroelectric Ising bilayer structure with D2 = −0.5, J1 = −1.0,
2 Z |J3| = 0.5 and E = 1.0. The numbers on the curves are the values of the crystal-
P4 = N
〈 ∑n SnD 〉 (3)
field parameter D1.
Therefore, the total polarization P is:
1 cases. It is considered to be the reason of multiple saturation values in
P= (P1 + P2 + P3 + P4 ) the P curves in Fig. 2(a). It is worth mentioning that the P1 shows the
4 (4)
saturation value P1 = 1.0 for D1 = −2.25. This is because the spins of
The total dielectric susceptibility x is: sublattice A stay the σiAz = 3/2 and σiAz = 1/2 states with the same prob-
x = NLβ ( < P 2 > − < P >2 ) (5) ability. It is found that for the same D1, the P3 and P4 always have the
same saturation value P3 = P4=2.0, and their changes are very similar
The specific heat per site: with each other, only the P3 is larger than the P4 at certain temperature.
C β2 In Fig. 2(d), one can notice that all χ curves display a peak in high
= ( < H 2 > − < H >2 ) temperature region, which should correspond to the blocking tem-
kB N (6)
perature (TB) [68,69]. The TB gives the information of the second-order
with β = 1/kBT, where T represents temperature and kB represents phase transition from the ferrielectric phase to the paraelectric phase.
boltzmann constant. As this Fig. 2(d) shows, we can get the values of TB = 8.7, 7.3, 6.3, 5.9,
6.4, 7.1, 7.6 for D1 = 0, −1.0, −1.5, −1.75, −2.0, −3.0, −5.0 re-
3. Numerical results and discussion spectively. It is clear that TB increases first and then decrease with in-
creasing |D1|. It is worth mentioning that the P and χ curves obtained in
3.1. Polarization and dielectric susceptibility this work are in good agreement with the experimental observations of
the ferroelectric Ba(Ti1-xZrx)O3 ceramics [70]. Besides, some double-
Firstly, typical results are presented to show the effects of the peak χ curves are also observed for D1 = −1.75, −2.0, −3.0 -5.0.
crystal-field, the exchange coupling and the electric field on the po- Among these χ curves, the peak in low temperature region should result
larization and the dielectric susceptibility of the antiferroelectric/fer- from the abrupt change in the P curves in Fig. 2(a). These behaviors of
roelectric bilayer system. the χ curves are similar to the recent study of a mixed spin-3/2 and
Fig. 2(a)–(d) shows the temperature dependences of the total po- spin-5/2 Ising ferrielectric nanowires [52].
larization P, the sublattice polarizations in the top and bottom layers P1, Fig. 3(a)-(d) shows the temperature dependences of P, P1, P2, P3, P4,
P2 and P3, P4, the total dielectric susceptibility χ for the different values χ for the different values of D2 when D1 = −0.5, J1 = −1.0, |J3| = 0.5
of D1 when D2 = −0.5, J1 = −1.0, |J3| = 0.5 and E = 1.0. In Fig. 2(a), and E = 1.0. Compared with Fig. 2(a), we can observe that the system
all P curves start from their saturation values and express different displays richer types P curves under the effect of D2 in Fig. 3(a), which
change behaviors for different values of D1. When D1 = 0, −0.5, suggests that the effect of D2 on the P seems stronger than that of D1.
−2.25, the P decreases gently with temperature increasing, while the P These abundant P curves also originate from the competition between
increases first and then decreases continuously from its saturation value the crystal-field D2 and temperature. Furthermore, there are still three
to the small constant polarization as T increases for D1 = −1.5, −3.0 saturation values P = 1.0, 0.75, 0.5 for different values of D2 at T = 0,
and −5.0. In addition, the P drops abruptly at low temperature and which mainly comes from the contribution of the saturation values of
then decreases slowly as T increases when D1 = −1.75. The existence the P3 and P4 as shown in Fig. 3(b) and (c). This is because the sa-
of the interesting P curves is attributed to the competition between the turation values of the P1 and P2 are unchangeable for varying the values
crystal-field D1 and temperature. It is clearly seen that there are three of D2, but the P3 and P4 have three saturation values P3(P4) = 2.0, 1.5,
saturation values P = 1.0, 1.125, 1.25, which reflects the variation of 1.0, which are responsible for three saturation values of the P curves in
spin states in sublattices under the influence of D1. This is can be easily Fig. 3(a). In Fig. 2(d), it is found that the TB decreases with the increase
get the answer for these saturation values of four sublattice in Fig. 2(b) of |D2|, which is different from the change of TB with D1.
and (c). For example, when D1 = 0, −0.5, −1.5, the saturation values The effect of J1 on the polarization and the susceptibility when
of P is P = (5/2–5/2 + 2+2)/4 = 1.0 according to Eq. (4). As |D1 | D1 = −1.0, D2 = −0.5, |J3| = 0.8 and E = 1.0 is shown in Fig. 4(a)-
increases, the spins of sublattices A and B in the top layer change from (d). From Fig. 4(a), we can find that the P has a similar behavior as that
high spin states to low states, such P curves for |D1| > 1.5 are these

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Fig. 3. The temperature dependences of the total polarization P, the sublattice
polarizations P1, P2, P3, P4 and the total dielectric susceptibility χ for the anti-
ferroelectric/ferroelectric Ising bilayer structure when D1 = −0.5, J1 = −1.0,
|J3| = 0.5 and E = 1.0. The numbers on the curves are the values of the crystal-
field parameter D2.
Fig. 5. The temperature dependences of the total polarization P, the sublattice
polarizations P1, P2, P3, P4 and the total dielectric susceptibility χ for the anti-
ferroelectric/ferroelectric Ising bilayer structure when D1 = −1.0, D2 = −0.5,
J1 = −0.5 and E = 1.0. The numbers on the curves are the values of the in-
terlayer exchange coupling |J3|.

changes as those given in Fig. 4(a), which means the effect of J3 on the
P is similar to that of J1. These distinct P curves come from the com-
petition between the exchange coupling and temperature. Similarly,
from Fig0. 5(b) and (c), the saturation values of P1 and P2 can be also
determined by the J3, whereas those of P3 and P4 are unchanged when
|J3| changes from 0.1 to 2.0. This P behaviors are similar to those ob-
served in Ref. [71]. In Fig. 5 (d), the peak of every χ curve shifts to high
temperature with |J3| increasing, suggesting the TB can be enhanced by
strengthening interlayer exchange coupling |J3|. The results are also
consistent with those of ferroelectric bilayer composed of two different
ferroelectric slabs with antiferroelectric interfacial coupling [33].
Finally, the effect of the E on the polarization and the susceptibility
when D1 = −1.0, D2 = −0.5, J1 = −0.5 and |J3| = 0.8, as presented
in Fig. 6(a)-(d). It can be seen from Fig. 6(a) that the saturation values
and the P at certain temperature increase obviously with E increasing.

Fig. 4. The temperature dependences of the total polarization P, the sublattice

polarizations P1, P2, P3, P4 and the total dielectric susceptibility χ for the anti-
ferroelectric/ferroelectric Ising bilayer structure with fixed D1 = −1.0,
D2 = −0.5, |J3| = 0.8 and E = 1.0. The numbers on the curves are the values of
the top exchange coupling J1.

in Fig. 2(a). That means the effect of J1 on the P is similar to that of D1.
For certain parameters, the system shows two saturation values
P = 1.0, 1.25 at the T = 0, which can be analyzed from the sublattice
polarization in Fig. 4(b) and (c). Note that the saturation values of the
P1 and P2 take small values for small values of |J1|. For example, when
J1 = −0.1, P1 = 1.5 and P2 = −0.5, and when J1 = −0.5, P1 = 2.5
and P2 = −1.5, which lead to the appearance of the saturation value of
P = 1.25. This is because the weak exchange coupling J1 can reduce the
relationship between sublattices A and B as to force them to stay at the
low spin states. In Fig. 4(d), the TB increases with |J1| increasing, which
is opposite to that of D2 on TB.
Fig. 5(a)-(d) shows the temperature dependences of P, P1, P2, P3, P4, Fig. 6. The temperature dependences of the total polarization P, the sublattice
χ for the different values of |J3| when D1 = −1.0, D2 = −0.5, polarizations P1, P2, P3, P4 and the total dielectric susceptibility χ for the
BiFeO3/YMnO3 bilayer with fixed D1 = −1.0, D2 = −0.5, J1 = −0.5 and
J1 = −0.5 and E = 1.0. In Fig. 5(a), the system still shows two sa-
|J3| = 0.8. The numbers on the curves are the values of the electric field
turation values P = 1.0, 1.25, and the P curves behave the similar
parameters E.

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Z.-y. Wang, et al. Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133

Fig. 8. The blocking temperature TB for the antiferroelectric/ferroelectric Ising

bilayer structure under the effects of the crystal-field parameters D1, D2 in three
dimensional space (TB, D1, D2) for J1 = −1.0, |J3| = 0.5 and E = 1.0.

Fig. 7. Phase diagrams (a) in the (TB, D1) plane for D2 = −0.5, J1 = −1.0,
|J3| = 0.5 and E = 1.0; (b) in the (TB, D2) plane for D1 = −0.5, J1 = −1.0,
|J3| = 0.5 and E = 1.0; (c) in the (TB, J1) plane for D1 = −1.0, D2 = −0.5,
|J3| = 0.8 and E = 1.0; (d) in the (TB, |J3|) plane for D1 = −1.0, D2 = −0.5,
J1 = −0.5 and E = 1.0; (e) in the (TB, E) plane for D1 = −1.0, D2 = −0.5,
J1 = −0.5 and |J3| = 0.8.

Three saturation values P = 1.0, 1.25 and 1.5 come from mainly the
change in the saturation value of the P2 (P2 = −2.5, −1.5, −0.5) in
Fig. 6(b) and (c) because the spins of sublattice B align against the di-
rection of the E. Remarkably, the experimental results of
PbZr0.51Ti0.49O3 thin films also revealed that the polarization increases
with the increase of the electric field [72]. From Fig. 6 (d), as E in-
creases, the χ curves become broader and the TB also becomes higher.

3.2. Phase diagrams of the blocking temperature
In order to clarify the change of the TB with various physical
parameters, we present the phase diagrams of the TB in different
parameter planes, as shown in Figs. 7–9.
Fig. 7(a)-(e) shows the TB versus the D1, D2, J1, |J3|, E, respectively.
From each sub-figure, we can remark that the TB of the ferroelectric
bilayer strongly depends on every physical parameter. It is found that
the TB may be improved by decreasing the crystal-field D2 or increasing
the exchange couplings J1 and |J3| as well as the external electric field
E. Interestingly, one can notice from Fig. 7(a) that the TB decreases first
and then increases with the increase of |D1|. When D1 = −1.75, the TB
takes the smallest value (TB = 5.86). These TB behaviors under the ef-
fects of various parameters are comparable with those studies of other
nano-systems such as nano-graphene bilayer [59], nanofilms [73], na-
noislands [63,64,74]. An agreement can be obtained through a com-
parison between theirs and ours.
To further under the common effect of two crystal-fields D1 and D2
on the TB, we present the three-dimensional diagram in the (D1, D2, TB)
plane with J1 = −0.5, |J3| = 0.8 and E = 1.0 in Fig. 8. It is found that
the weaker D1 and D2 are beneficial to the higher TB. Fig. 9 shows the
three-dimensional diagram in the (J1, |J3|, TB) plane with D1 = −1.0,
Fig. 9. The blocking temperature TB for the antiferroelectric/ferroelectric Ising
bilayer structure under the effects of the exchange coupling J1, |J3| in three
dimensional space (TB, J1, |J3|) for D1 = −1.0, D2 = −0.5 and E = 1.0.
D2 = −0.5 and E = 1.0. It is clear that the larger J1 and |J3| may make
the TB to be higher, which has an opposite influence to those of D1 and
D2. Our results consist with those of EuTiO3 nanowires in qualitative
[75].
3.3. Internal energy and specific heat
Firstly, we present the effects of the crystal-fields D1 and D2 on the
internal energy U and the specific heat C of the system. Fig. 10(a)-(b)
shows the temperature dependences of the U and C of the system for the
different values of D1 when D2 = −0.5, J1 = −1.0, |J3| = 0.5 and
E = 1.0. From Fig. 10(a), each U starts from its minimum constant
value at low temperature, and increases with T increasing. It is found
that the U can be enhanced by increasing |D1|. In Fig. 10(b), every C
curve express a peak near the TB, which shows the phase from ordered
to disordered in the system. The peak moves to the low temperature
with |D1| increasing. Note that besides the peak at high temperature,

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Fig. 10. The temperature dependences of the internal energy U and the specific
heat C for the antiferroelectric/ferroelectric Ising bilayer structure (a, b) for
different values of D1 with fixed D2 = −0.5, J1 = −1.0, |J3| = 0.5 and E = 1.0
(c, d) for different values of D2 with fixed D1 = −0.5, J1 = −1.0, |J3| = 0.5
and E = 1.0. The numbers on the curves are the values of the crystal-field
parameters D1 and D2.
Fig. 11. The temperature dependences of the internal energy U and the tem-
perature dependences of the specific heat C for the antiferroelectric/ferro-
electric Ising bilayer structure (a, b) for different values of J1 with fixed
D1 = −1.0, D2 = −0.5, |J3| = 0.8 and E = 1.0 (c, d) for different values of J1
with fixed D1 = −1.0, D2 = −0.5, J1 = −0.5 and E = 1.0. The numbers on the
curves are the values of the exchange coupling J1 and |J3|.
the double-peak C curves with a peak at low temperature have been
also observed when D1 = −1.5, −2.0, −5.0, which is consistent with
those in Fig. 2(d). Fig. 10(c)-(d) shows the temperature dependences of
the U and C for different values of D2 when D1 = −0.5, J1 = −1.0,
|J3| = 0.5 and E = 1.0. Comparing with those in Fig. 10(a) and (b), we
can remark that the effects of the D2 on the U and C are similar to those
of D1. These results are similar to those obtained in the nano-graphene
bilayer [76], cylindrical nanowires [77,78] and nanotubes [79].
Fig. 11(a)-(d) shows the effects of the exchange couplings J1 and J3
on the internal energy U and the specific heat C of the system. In
Fig. 11(a)-(b), we set D1 = −1.0, D2 = −0.5, |J3| = 0.8 and E = 1.0. It
is clearly seen from Fig. 11(a) that the U decreases with |J1| increasing,
which suggests the larger |J1|, the more stable the system. In Fig. 11(b),
132
Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133
Fig. 12. The temperature dependences of the internal energy U, and the tem-
perature dependences of the specific heat C for the antiferroelectric/ferro-
electric Ising bilayer structure with fixed D1 = −1.0, D2 = −0.5, J1 = −0.5
and |J3| = 0.8. The numbers on the curves are the values of the electric field
parameters E.
the peaks of the C curve shift to the high temperature as |J1| increases.
Fig. 11(c)-(d) shows the temperature dependences of the U and C for
different values of |J3| when D1 = −1.0, D2 = −0.5, J1 = −0.5, and
E = 1.0. Through a comparison with those in Fig. 11(a) and (b), it is
found that the effects of the |J3| on the U and C are similar to those of
J1.
Fig. 12(a)-(b) shows the temperature dependence of the U and C for
different values of E when D1 = −1.0, D2 = −0.5, J1 = −0.5 and
|J3| = 0.8. It is obvious that the U decreases as E increases, which
means the bigger E, the more stable the system. In Fig. 12(b), the peak
of the C curve moves towards the high temperature area with E in-
creasing. According above analysis, it is concluded that decreasing
crystal-fields or increasing exchange couplings and external electric
field can make the system more stable. The results are consistent with
those in ferrielectric nanowires [53], nanoparticles [54] and ternary
nanoislands [80].
4. Conclusions
In this work, using Monte Carlo simulation, we have studied di-
electric properties of a mixed-spin (5/2, 2) antiferroelectric/ferro-
electric bilayer structure in the external electric field. The results show
that the crystal-field, exchange coupling and external electric field play
an important role in controlling the polarization, dielectric suscept-
ibility, internal energy, specific heat and blocking temperature of the
system. Multiple polarization curves have been observed, originating
from the competition among the crystal-field, the exchange coupling,
the external electric field and temperature. The crystal-fields have an
opposite influence on the TB and U to those of the exchange couplings
and the external electric field. We hope that the theoretical study can
provide proper guidance for the application of multiferroic bilayers in
experiments.
Acknowledgements
This project was supported by Natural Sciences Foundation of
Liaoning province, China (Grant No. 20170540672).
References
[1] J. Wang, J.B. Neaton, H. Zheng, V. Nagarajan, S.B. Ogale, B. Liu, D. Viehland,
V. Vaithyanathan, D.G. Schlom, U.V. Waghmare, N.A. Spaldin, K.M. Rabe,
M. Wuttig, R. Ramesh, Science 299 (5613) (2003) 1719.
[2] S.M. Selbach, T. Tybell, M. Einarsrud, T. Grande, Adv. Mater. 20 (19) (2008) 3692.
[3] S.R. Das, R.N.P. Choudhary, P. Bhattacharya, R.S. Katiyar, P. Dutta, A. Manivannan,
M.S. Seehra, J. Appl. Phys. 101 (2007) 034104.
[4] Y. Zhang, Z. Li, C. Deng, J. Ma, Y. Lin, C.W. Nan, Appl. Phys. Lett. 92 (2008)
152510.
[5] R.A. Islam, H. Kim, S. Priya, H. Stephanou, Appl. Phys. Lett. 89 (2006) 152908.
[6] E. Quandt, S. Stein, M. Wuttig, Transactions on Magnetics 41 (10) (2005) 3667.
[7] M. Liu, X. Li, H. Imrane, Y. Chen, T. Goodrich, Z. Cai, K.S. Ziemer, J.Y. Huang,
Z.-y. Wang, et al. Physica E: Low-dimensional Systems and Nanostructures 110 (2019) 127–133

N.X. Sun, Appl. Phys. Lett. 90 (2007) 152501. [44] Y. Nakamura, J. Phys. Condens. Matter 12 (2000) 4067.
[8] C.I. Cheon, K.Y. Yun, J.S. Kim, J.H. Kim, J. Kor. Chem. Soc. 40 (4) (2003) 398. [45] Y. Nakamura, Phys. Rev. B 62 (2000) 11742.
[9] Z.X. Cheng, X.L. Wang, C.V. Kannan, K. Ozawa, H. Kimura, Appl. Phys. Lett. 88 [46] A. Feraoun, M. Kerouad, Computational Condensed Matter 15 (2018) 7.
(2006) 132909. [47] R. Masrour, L. Bahmad, A. Benyoussef, M. Hamedoun, E.K. Hlil, J. Supercond. Nov.
[10] R. Thomas, J.F. Scott, D.N. Bose, R.S. Katiyar, J. Phys. Condens. Matter 22 (2010) Magnetism 26 (2013) 679.
423201. [48] R. Masrour, A. Jabar, J. Comput. Electron. 16 (1) (2017) 12.
[11] J. Zapata, J. Narváez, W. Lopera, M.E. Gómez, G.A. Mendoza, P. Prieto, [49] Y. Benhouria, I. Bouziani, I. Essaoudi, A. Ainane, R. Ahuja, J. Magn. Magn Mater.
Transactions on Magnetics 44 (11) (2008) 2895. 460 (2018) 223.
[12] P.X. Nie, Y.P. Wang, Y. Yang, G.L. Yuan, W. Li, X.T. Ren, Energy harvesting, Systems [50] W. Wang, S.Q. Yang, Y. Yang, Z. Peng, B.C. Li, M. Yang, Physica E 109 (2019) 30.
2 (3–4) (2015) 157. [51] S. Zriouel, B. Taychour, F. El Yahyaoui, L.B. Drissi, Physica E 91 (2017) 113.
[13] A. Venugopalan, M. Appasamy, S. Saravanan, K. Kothandaraman, [52] Y. Benhouria, I. Essaoudi, A. Ainane, R. Ahuja, F. Dujardin, Ferroelectrics 507
J. Kothandaraman, J. Rare Earths 27 (6) (2009) 1013. (2017) 58.
[14] S.N. Tripathy, K.K. Mishra, S. Sen, B.G. Mishra, Dhiren K. Pradhan, R. Palai, [53] Y. Benhouria, I. Essaoudi, A. Ainane, R. Ahuja, F. Dujardin, Physica A 506 (2018)
D.K. Pradhan, J. Appl. Phys. 114 (2013) 144104. 499.
[15] B. Wang, Y. Yang, W.J. Qian, L. l. Liu, Y. p. Wang, Symposium on Piezoelectricity 47 [54] Y. Benhouria, I. Essaoudi, A. Ainane, R. Ahuja, F. Dujardin, J. Supercond. Nov.
(1) (2012) 298. Magnetism 27 (9) (2014) 2153.
[16] Z. Li, Y. Gao, B. Yang, Y.H. Lin, R. Yu, C.W. Nan, J. Am. Ceram. Soc. 94 (4) (2011) [55] S.H. Kim, Bull. Korean Chem. Soc. 36 (9) (2015) 2208.
1060. [56] X.S. Wang, C.L. Wang, W.L. Zhong, X.Y. Xue, Mater. Sci. Eng. 99 (2003) 576.
[17] H.C. He, J.P. Zhou, J. Wang, C.W. Nan, Appl. Phys. Lett. 89 (2006) 052904. [57] W. Jiang, V.C. Lo, Commun. Theor. Phys. 43 (2005) 362.
[18] D.X. Zhou, G. Jian, Y.X. Hu, Y.N. Zheng, S. p. Gong, H. Liu, Mater. Chem. Phys. 127 [58] A. Jabar, R. Masrour, A. Benyoussef, M. Hamedoun, J. Supercond. Nov. Magnetism
(2011) 316. 29 (3) (2016) 733.
[19] B. Yang, Z. Li, Y. Gao, Y.H. Lin, C.W. Nan, J. Alloy. Comp. 509 (2011) 4608. [59] W. Wang, R.J. Liu, D. Lv, X.H. Luo, Superlattice. Microst. 98 (2016) 458.
[20] J. Dho, M.G. Blamire, J. Appl. Phys. 106 (2009) 073914. [60] W. Wang, Q. Li, D. Lv, R.J. Liu, Z. Peng, S. Yang, Carbon 120 (2017) 313.
[21] J. Richy, T. Hauguel, J. Jay, S.P. Pogossian, B.W. Fonrose, C.J. Sheppard, [61] W. Wang, D.D. Chen, D. Lv, J.P. Liu, Q. Li, Z. Peng, J. Phys. Chem. Solid. 108
J.L. Snyman, A.M. Strydom, J.B. Youssef, A.R.E. Prinsloo, D. Spenato, (2017) 39.
D.T. Dekadjevi, J. Phys. Appl. Phys. 51 (2018) 125308. [62] W. Wang, J.L. Bi, R.J. Liu, X. Chen, J.P. Liu, Superlattice. Microst. 98 (2016) 433.
[22] M. Alam, S. Talukdar, K. Mandal, Mater. Lett. 210 (2018) 80. [63] W. Wang, Z. Peng, S.S. Lin, Q. Li, D. Lv, S. Yang, Superlattice. Microst. 113 (2018)
[23] J.Y. Chen, Z.H. Tang, Y.L. Bai, S.F. Zhao, J. Alloy. Comp. 675 (2016) 257. 178.
[24] C.L. Zhang, L.L. Zhang, X.D. Shen, W.Q. Chen, J. Appl. Phys. 119 (2016) 134102. [64] Z. Peng, W. Wang, D. Lv, R.J. Liu, Q. Li, Superlattice. Microst. 109 (2017) 675.
[25] H.T. Chen, A.K. Soh, J. Appl. Phys. 112 (2012) 074104. [65] N. Metropolis, A.W. Rosenbluth, M.N. Rosenbluth, A.H. Teller, E. Teller, J. Chem.
[26] M. Ziese, A. Bollero, I. Panagiotopoulos, N. Moutis, Appl. Phys. Lett. 88 (2006) Phys. 21 (1953) 1087.
212502. [66] J.W. Tukey, Ann. Math. Stat. 29 (1958) 614.
[27] K. Dörr, C. Thiele, Phys. Status Solidi 243 (1) (2006) 21. [67] M.E.J. Newman, G.T. Barkema, Monte Carlo Methods in Statistical Physics,
[28] C.W. Nan, M.I. Bichurin, S.X. Dong, D. Viehland, G. Srinivasan, J. Appl. Phys. 103 Clarendon Press, Oxford, 1999.
(2008) 031101. [68] X.Y. Lang, W.T. Zheng, Q. Jiang, Nanotechnology 18 (2007) 155701.
[29] L.H. ONG, A.K.H. Chew, Ferroelectrics 450 (2013) 7. [69] M. Soda, M. Matsuura, Y. Wakabayashi, K. Hirota, J. Phys. Soc. Jpn. 80 (2011)
[30] Q.C. Li, J.M. Liu, Phys. Rev. B 75 (2007) 064415. 043705.
[31] C.L. Zhang, W.Q. Chen, C. Zhang, J. Appl. Phys. 113 (2013) 084502. [70] R. Farhi, M.E. Marssi, A. Simon, J. Ravez, The European Physical Journal B 9 (1999)
[32] A. Ainane, I. Essaoudi, M. Saber, J. Magn. Magn Mater. 315 (2007) 132. 599.
[33] Y. Benhouria, I. Essaoudi, A. Ainane, A. Oubelkacem, M. Saber, F. Dujardin, Phys. [71] Y. Benhouria, I. Essaoudi, A. Ainane, R. Ahuja, F. Dujardin, Superlattice. Microst. 73
Scripta 86 (2012) 045704. (2014) 121.
[34] C.G. Duan, S.S. Jaswal, E.Y. Tsymbal, Phys. Rev. Lett. 97 (2006) 047201. [72] P.K. Larsen, G.J.M. Dormans, D.J. Taylor, P.J. van Veldhoven, J. Appl. Phys. 76
[35] W. Jiang, W. Wang, F. Zhang, W.J. Ren, J. Appl. Phys. 105 (2009) 07E321. (1994) 2405.
[36] W. Wang, D. Lv, F. Zhang, J.L. Bi, J.N. Chen, J. Magn. Magn Mater. 385 (2015) 16. [73] D. Lv, W. Wang, J.P. Liu, D.Q. Guo, S.X. Li, J. Magn. Magn Mater. 465 (2018) 348.
[37] W. Wang, W. Jiang, D. Lv, Phys. Status Solidi B 249 (1) (2012) 190. [74] D. Lv, Y. Yang, W. Jiang, F. Wang, Z.Y. Gao, M. Tian, Physica A 514 (2019) 319.
[38] T. Kaneyoshi, Y. Nakamura, S. Shin, J. Phys. Condens. Matter 10 (1998) 7025. [75] A.N. Morozovska, M.D. Glinchuk, R.K. Behera, B. Zaulychny, C.S. Deo, E.A. Eliseev,
[39] W. Wang, W. Jiang, D. Lv, F. Zhang, J. Phys. Appl. Phys. 45 (2012) 475002. Phys. Rev. B 84 (2011) 205403.
[40] W. Jiang, Y.N. Wang, J. Magn. Magn Mater. 426 (15) (2017) 785. [76] X.H. Luo, W. Wang, D.D. Chen, S. Xu, Physica B 491 (2016) 51.
[41] A. Jabar, R. Masrour, A. Benyoussef, M. Hamedoun, J. Supercond. Nov. Magnetism [77] D. Lv, F. wang, R.J. Liu, Q. Xue, S.X. Li, J. Alloy. Comp. 701 (2017) 935.
30 (7) (2017) 1807. [78] D. Lv, W. Jiang, Y. Ma, Z.Y. Gao, F. Wang, Physica E 106 (2019) 101.
[42] A. Jabar, R. Masrour, Phys. B Condens. Matter 539 (15) (2018) 21. [79] W. Wang, Y. Liu, Z.Y. Gao, X.R. Zhao, Y. Yang, S. Yang, Physica E 101 (2018) 110.
[43] M. Ertas, Superlattice. Microst. 85 (2015) 734. [80] Y. Yang, W. Wang, H. Ma, Q. Li, Z.Y. Gao, T. Huang, Physica E 108 (2019) 358.

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