Acta Materialia 206 (2021) 116607

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Acta Materialia
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Strain engineering of ferroelectric negative capacitance in

PbZr(1-x) Tix O3 thin films
Chang Liu a, Jie Wang a,b,∗
a
Department of Engineering Mechanics, Zhejiang University, Zheda Road 38, Hangzhou, Zhejiang 310027, China
b
Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province, Zheda Road 38, Hangzhou, Zhejiang 310027, China

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

Article history: Negative capacitance (NC) in ferroelectric materials has been proposed to overcome the fundamental lim-
Received 25 August 2020 itation on the energy efficiency of electronics. Understanding the impact of mechanical strain on the NC
Revised 4 December 2020
of ferroelectrics is of scientific significance and technological importance because the strain-polarization
Accepted 23 December 2020
coupling could substantially influence the multifunctional properties of epitaxial ferroelectric thin films.
Available online 3 January 2021
Based on time-dependent Ginzburg-Landau equation and Kirchhoff’s law, we reveal that a tensile strain
Keywords: decreases the magnitude and duration time of the transient NC of PbZr(1-x) Tix O3 (PZT) thin films while a
Negative capacitance compressive strain increases it in a resistor-ferroelectric capacitor circuit. In particular, the tensile strain
Ferroelectric materials makes the transient NC completely disappear near the morphotropic phase boundary (MPB), whereas the
Phase-field simulation compressive strain can maintain it up to a temperature higher than Curie temperature. The detailed en-
Strain engineering ergy analysis reveals that the change of transient NC with strain and composition is attributed to the
change of the negative curvature of energy landscape, which is the origin of NC in ferroelectric materials.
The work gives considerable new insight into the mechanical control of ferroelectric transient NC, and
offers guidance in searching for large transient NC in the widely used PZT thin films through strain and
composition engineering.
© 2020 Published by Elsevier Ltd on behalf of Acta Materialia Inc.

1. Introduction terials, extensive numerical investigations [8–11] and experimental

The size of microprocessors has been significantly decreased
while the computation capability has been improved during past
decades in keeping with the Moore’s law [1,2]. In recent years,
however, the decrease of size of integrated circuit is facing chal-
lenges from reducing the power dissipation and heat generation,
which is limited by Boltzmann Tyranny [3]. To overcome this phys-
ical limitation, the negative capacitance (NC) in ferroelectric ma-
terials has been proposed as a promising solution [4]. The nega-
tive capacitance refers to the response of a ferroelectric capacitor
where voltage decreases whilecharges increase [4–6]. In a transis-
tor circuit, a ferroelectric NC can serve as an amplifier that boosts
the input voltage and effectively decreases the voltage required to
operate the transistor [7]. Therefore, the energy dissipation of the
integrated circuit can be reduced dramatically if the NC is em-
ployed.
From the theoretical point of view, the origin of NC is the neg-
ative curvature in a double-well energy landscape of ferroelectric
materials. To understand and realize the NC of ferroelectric ma-
∗
Corresponding author.
E-mail address: jw@zju.edu.cn (J. Wang).
studies [5,12–18] have been carried out in recent years. The NC of
ferroelectric materials are generally classified as two types. One is
the steady-state NC resulting from stabilizing the ferroelectric po-
larization in the region of negative curvature of energy landscape,
which is typically achieved in a ferroelectric-dielectric capacitor
[17,19]. Another is the transient NC [6], which refers to a transient
response of a ferroelectric capacitor in a resistance-ferroelectric
capacitor (R-FEC) circuit, as shown in Fig. 1(a). The transient NC
originates from the mismatch in switching rate between the free
charge on the metal and the bound charge in a ferroelectric ca-
pacitor during the polarization switching, which is also related to
the negative curvature of energy landscape of ferroelectric materi-
als [6].
The ferroelectric capacitors in the R-FEC circuit are usually de-
posited on different substrates, where the epitaxial strain exhibits
because of the lattice mismatch between the ferroelectric thin film
and substrate, as shown in Fig. 1(b). The epitaxial strain has great
influence on the phase transition [20,21], piezoelectric and elec-
trocaloric properties [22,23] of ferroelectric thin films, which may
also influence the transient NC of ferroelectric capacitors due to
the coupling between polarization and strain [19,24]. However, the
influence of epitaxial strain on the transient NC of ferroelectric thin

https://doi.org/10.1016/j.actamat.2020.116607
1359-6454/© 2020 Published by Elsevier Ltd on behalf of Acta Materialia Inc.
C. Liu and J. Wang Acta Materialia 206 (2021) 116607

Fig. 1. (a). The schematic diagram of a ferroelectric thin film in a resistance-ferroelectric capacitor circuit, in which VS , VF and R represents the input source voltage, the
voltage across the capacitance, and the resistor, respectively. The coordinate of thickness direction of the ferroelectric capacitor is denoted by x3 . (b) The epitaxial PZT
ferroelectric thin film grown on a perovskite substrate with electrode, the biaxial strain of ε11 = ε22 = ε exhibits in the PZT thin film due to the lattice mismatch of the thin
film and substrate/electrode.

2
Fig. 2. Transient responses of VF and ∂ 2U /∂ P 3 of PZT capacitance when an initially negative input voltage (VS = −10V ) becomes a positive one (VS = −10V ). (a) with the
composition x = 1 and the misfit strain ε = −1%, 0, 1%, respectively. (b) with the strain of ε = 0 and the composition x = 0.1, 0.5 and 1, respectively. The areas between
two dash lines with same color denote the durations with negative capacitance. A negative input voltage is initially applied on the capacitor to set the polarization in the
negative direction.

films has not been studied yet. In particular, the effect of strain on
the transient NC of the widely used PbZr(1-x) Tix O3 (PZT) thin films
near the morphotropic phase boundary (MPB) where the anoma-
lous behaviors often exhibit is still unknown.
In this paper, based on the time-dependent Ginzburg-Landau
equation and Kirchhoff’s law, a phase-field model with constant-
strain assumption is developed to describe the evolution of free
charge and polarization in a R-FEC circuit. The phase-field model is
employed to investigate the transient response of free charge and
polarization in ferroelectric phase PZT (0.1 ≤ x ≤ 1 ) [25] thin films
with different strains. The effect of strain and composition on the
magnitude and duration time of transient NC is obtained for the R-
FEC circuit under different temperatures. The temperature versus
composition phase diagrams of transient NC are constructed and
an anomalous transient NC are found near the MPB. The underly-
ing physics on the anomalous transient NC with different strains
and compositions is discussed in terms of the negative curvatures
of energy landscape.
2. Method
For the R-FEC circuit of Fig. 1(a), the current flowing through
the resistor R can be determined by i=∂ QF /∂ t, where QF denotes
the free charge density per area and t is time. The current in this

2
C. Liu and J. Wang Acta Materialia 206 (2021) 116607

Fig. 3. The ferroelectric hysteresis loops of P 3 − VF in (a) and (c), and the free energy profiles of U − P 3 in (b) and (d) in the ferroelectric capacitor when the input voltage
Vs switches back and forth from -10 V to 10 V in the R-FEC circuit. (a) and (b) With the composition x = 1 and the misfit strains of −1%, 0 and 1%. AB and CD in (a) denote
the segments where the negative capacitance appears for ε = 1%. (c) and (d) With the strain ε = 0 and the compositions of x = 0.1, 0.5 and 1. A B and C D in (c) represent
the segments where the negative capacitance exists for x = 1.

circuit is governed by Kirchhoff’s law as total free energy density includes the Helmholtz free energy den-
sity fLD , the polarization gradient energy density fG , and the elec-
∂ QF
RA =VS −VF (1) tric energy density fE . The Helmholtz free energy density takes the
∂t form as
in which R and A represent the resistance and area of the ferro-    
fLD = α1∗ P12 + P22 + α3∗ P32 + α11
∗
P14 + P24 + α33
∗ 4
P3 + α12
∗ 2 2
P1 P2
electric capacitor, respectively. Vs and VF are the input voltage and    
the voltage across the ferroelectric capacitor, respectively. + α13
∗ 2
P3 P12 + P22 + α111 P16 + P26 + P36
Following pervious work on ferroelectric thin films [26], the       
+ α112 P14 P22 + P32 + P24 P12 + P32 + P34 P14 + P24
polarization components Pi (x3 )(i = 1, 2, 3 ) are assumed dependent
only on the coordinate of thickness direction of the ferroelectric ε2
+ α123 P12 P22 P32 + , (3)
capacitor, as shown in Fig. 1(a). The epitaxial strain of ε11 = ε22 = ε s11 + s22
is employed in ferroelectric capacitor and other strain components
in which α1∗ , α ∗3 , α ∗11 , α ∗33 , α ∗12 and α13
∗ are the renormalized
are assumed zero. In previous studies, the Landau-Khalatnikov
Landau coefficients [26]. For simplicity, the epitaxial strain is as-
model (L-K model) is commonly adopted to predict the tempo-
sumed uniform and is included in the renormalized Landau coeffi-
ral evolution of polarization in ferroelectric capacitor [27,28], in
cients as [26,29]
which only the polarization component P3 is concerned. Thus, the
rotation of polarization during the polarization switching process 2(Q11 + Q12 )ε
α1∗ = α1 − , (4a)
cannot be determined in the L-K model. To precisely describe the s11 + s12
polarization evolution, the time-dependent Ginzburg-Landau equa-
tion (TDGL equation) is used to predict the temporal evolution of 2Q12 ε
α3∗ = α1 − , (4b)
polarization in ferroelectric capacitor in the present work: s11 + s12
 
1 ∂ Pi ∂U ∂U  2  
− = − , (2) 1
L ∂t ∂ Pi ∂ Pi,3 α11
∗
= α11 +   Q11 2
+ Q12 s11 − 2Q11 Q12 s12 , (4c)
2 s211 − s212
in which L is the dynamics coefficient andU = fLD + fG + fE is
the total free energy density. The comma after the variable rep- 2
Q12
resents the derivative with respect to the spatial coordinate. The α33
∗
= α11 + , (4d)
s11 + s12

3
C. Liu and J. Wang Acta Materialia 206 (2021) 116607

in which EF = VF /tF is the external electric field across the ferro-

electric capacitor and tF denotes the thickness of ferroelectric ca-
pacitor. On the right side of Eq. (6), the first term is the energy
density introduced by an external electric field. The last term de-
notes the depolarization energy density due to the inhomogeneous
polarization distribution in the thickness direction, where 0 is the
t
vacuum permittivity and P 3 = t1 0F P3 (x3 )dx3 represents the av-
F
erage polarization along the x3 direction [31]. The middle term
represents the depolarization energy induced by the unscreened
charge at interface with td representing the effective depolariza-
tion thickness [6,31].
The free charge density on the ferroelectric capacitor can be ex-
pressed as

QF = 0 EF + P 3 (7)
Based on Eqs. (1)–(7), the free charge on the capacitor and
the polarization in ferroelectric capacitor are coupled via the elec-
tric field EF = VF /tF in the ferroelectric capacitor. The response of
the polarization Pi in the ferroelectric capacitor and the voltage VF
across it can be obtained by solving the Eqs. (1) and (2) numeri-
cally when an input voltage Vs is applied in the R-FEC circuit. To
solve the Eqs (1) and (2), the finite difference method and Runge-
Kutta method are employed for spatial discretization and time in-
tegration, respectively. In the present work, 20nm-thick PZT capac-
itor with different Ti compositions x are selected as examples to
demonstrate the strain effect on the ferroelectric negative capaci-
tance. The material coefficients used in the simulations are listed
in Supplementary Materials. In all the present simulations, a neg-
ative input voltage is initially applied on the capacitor to set the
polarization in the negative direction.

3. Results and discussion

2
Fig. 4. (a). The strain-composition phase diagram of minimum of ∂ U /∂ 2
P3
dur-
ing polarization switching under different strains and compositions at 300 K. The Due to the coupling of strain and polarization, it is expected
dashed line denotes the phase boundary between then negative and positive value that the epitaxial strain ε has a significant influence on the tran-
2
of ∂ 2U /∂ P 3 . The red area in the diagram represents the existence of negative sient NC in ferroelectric capacitor. Fig. 2(a) shows the transition
capacitance while the negative capacitance vanishes in the blue area. (b) The response of voltage VF and the curvature of free energy landscape
strain-composition phase diagram of duration time of τ with the negative capac-
in the PbTiO3 (x = 1 ) capacitor at 300 K when the initially input
itance. The area with red color on the up-left sides represents positive capacitance
2 voltage Vs changes from the negative to positive under differ-
(∂ 2U /∂ P3 > 0 ) with zero duration. The duration time of negative capacitance in-
creases as the color changes from yellow to blue. (For interpretation of the refer- ent strains. The curvatures of free energy density landscape are
2
ences to color in this figure legend, the reader is referred to the web version of this calculated from ∂ 2U /∂ P 3 in which U and P 3 denote the average
article.). free energy density and average polarization component P3 along
the x3 direction. These curvatures are inverse proportional to the
capacitances of ferroelectric layer CF [6]. It is found that there
2
1  2   Q2 is a duration where ∂ VF /∂ t < 0 and ∂ 2U /∂ P 3 < 0 with ε = 0 in
α12
∗
= α12 − 2
Q11 + Q12 s12 − 2Q11 Q12 s11 + 44 , (4e) Fig. 2(a), which indicates the existence of transient NC. The tran-
s11 − s12
2 2 2s44
sient NC duration at ε = 0 for x = 1 is 2.8 μs, which is close to the
time consistent of 2.65 μs in the RC circuit. When a compressive
Q12 (Q11 + Q12 )
α13
∗
= α12 + , (4f) epitaxial strain (ε = −1% ) is applied, the duration with transient
s11 + s12
NC is extended and its magnitude becomes more pronounced. On
where Qij and sij denote the electrostriction and stiffness coef- the contrary, a tensile strain decreases the magnitude and duration
ficients, respectively. The Landau coefficient α1 = (T − T0 )/2κ0C0 . of NC in ferroelectric layer. When the tensile strain is large enough
Here, T and T0 denote the temperature and Curie–Weiss temper- 2
(ε = 1%), the NC can be even eliminated with ∂ 2U /∂ P 3 > 0 during
ature, respectively, C0 is the Curie constant and κ0 is the dielectric
the whole time. It is well known that the multifunctional proper-
constant of vacuum.
ties of PZT films are also highly dependent on the Ti composition
According to the phase-field theory, the gradient energy density
x. In order to understand the composition effect on the transient
of polarization is given by [30] 2
NC, Fig. 2(b) shows the transient response of VF and ∂ 2U /∂ P 3
1 1 ’  
for x = 0.1, 0.5 and 1, respectively, in the absence of strain. It
fG = G11 P32,3 + G44 + G44 P12,3 + P22,3 , (5)
2 2 is found that both the duration and magnitude of NC become
in which polarization Pi is a function of x3 . The electric energy larger with the increase of Ti composition x. The PZT capacitor
of ferroelectric capacitor includes the energies introduced by the with the composition x = 1 has the longest NC duration compared
external electric field and depolarization field, which is expressed with other compositions, which implies that the PbTiO3 capacitor
by has the best transient NC among different compositions at 300
td 2 1   K. In the present R-FEC circuit, the transient NC originates from
fE = −EF P3 + P3 + P3 − P 3 P3 (6) the mismatch in switching rate between the free charge on the
0tF 20

4
C. Liu and J. Wang
2 2
Fig. 5. (a). The temperature-strain phase diagram of ∂ 2U /∂ P 3 for the PbTiO3 thin films with x =1; (b)–(d) the temperature-composition phase diagrams of ∂ 2U /∂ P 3 for the
PZT thin films with the misfit strains of ε = −1%, 0 and 1%, respectively. The solid black lines in (c) denotes the Curie temperature and MPB, respectively. The tensile strain
or zero strain makes the transient NC completely disappear near the MPB at all range of temperature, whereas the compressive strain maintains it up to a temperature
higher than the Curie temperature of PZT bulk.
metal and the bound charge in a ferroelectric capacitor during the
polarization switching. Therefore, the polarization switching be-
havior in the present work is different from those of the previous
ferroelectric thin films without the R-FEC circuit [32,33.34].
When the input voltage Vs switches back and forth from -
10 V to 10 V, the average polarization P 3 and voltage VF in the
ferroelectric capacitor form hysteresis loops with different strains
and compositions as shown in Fig. 3(a) and (c), respectively. The
transient NC of ferroelectric capacitor can be confirmed by the
negative slope of the hysteresis loops as shown by the segments
AB and CD in Fig. 3(a) and by the segments A B and C D in
Fig. 3(c). The voltage range with negative slope in the P 3 − VF
hysteresis loops is reduced as the epitaxial strain changes from
compressive to tensile in Fig. 3(a), which is consistent with the
results of Fig. 2(a). It is interesting that all P 3 − VF loops with
different strains have the identical coercive field. The coercive
fields are also the same for the P 3 − VF loops with different com-
positions in Fig. 3(c). This phenomenon can be explained from
Eqs. (2) and (7). When the polarization is zero in the ferroelec-
tric capacitor, the right side of Eq. (2) equals −EF = VF /tF , hence
−∂ P3 /(L · ∂ t ) = VF /tF . Considering 0 EF is much smaller than P 3 ,
QF ≈ P 3 is hold in Eq. (7). Substitute QF ≈ P 3 into Eq. (1), one
can obtain
−1
tF tF
VF |P=0 = RA + VS
L L
The Eq. (8) shows that, for a certain R-FEC circuit, the mag-
nitude of VF at P = 0 is independent of strain and composition,
which is proportional to the input voltage and thus makes the
coercive field identical. To understand the origin of transient NC
in ferroelectric capacitor, the energy curves with double-well are
plotted for different strains and compositions in Fig. 3(b) and
Acta Materialia 206 (2021) 116607
(d), respectively. It is found that the compressive and tensile
in-plane misfit strains increase and decrease, respectively, the
energy barrier and the negative curvature in the energy profile, as
shown in Fig. 3(b). The results suggest that the negative curvature
of the energy profile is the origin of transient NC in ferroelectric
materials, which is consistent with previous work [6,15]. The
material composition x has the same impact as strain on the
energy density profile when the composition x increases, as is
shown in Fig. 3(d). With the increase of x, the both the energy
barrier and the negative curvature in the energy profile becomes
more significant, which is consistent with Fig. 2(b).
To obtain a whole picture on the transient NC with different
strains and compositions, the strain-composition phase diagram of
2
∂ 2U /∂ P3 at 300 K is constructed in Fig. 4(a). For the PZT capac-
itor with 0.1 ≤ x < 0.2, the transient NC does not exist with the
epitaxial strain ranging from −1% to −1%. A larger compressive
epitaxial strain is required near the MPB with x ∈ (0.4, 0.5 ) to
2
maintain the NC. Notice that the magnitude of ∂ 2U /∂ P 3 changes
abruptly around MPB when the tensile strain ε > 0.4%, which is
due to the strain induced phase transition from monoclinic phase
to orthorhombic phase. As a result, the double well energy profile
of U − P 3 in Fig. 3(b) becomes a single well energy profile, which
makes the negative curvature of the double well energy profile
disappears. Thus, there is an abrupt change in the magnitude of
(8) 2
∂ 2U/∂ P3 where the phase transition occurred. For PTO capacitor
(x = 1 ), the negative capacitance maintains until the tensile strain
is larger than 0.4%. The PTO capacitor exhibits the best transient
NC among different compositions for all the investigated strains.
In addition to the magnitude of transient NC, the duration of tran-
sient NC is also important in practice since the NC often works at
high frequency in an integrated circuit. Given that the switching
5
C. Liu and J. Wang
of polarization state in ferroelectrics takes a finite time, if the fre-
quency of applied voltage is too fast for ferroelectrics to respond,
the polarization will remain trapped in one stable polarization,
which cannot exhibit negative capacitance [35]. Fig. 4(b) gives the
contour plot of the duration of transient NC with different strains
and compositions at 300 K. It is found that the compressive stress
increases the duration while the tensile stress can decrease it. Like
the magnitude in Fig. 4(a), the PTO capacitor with the misfit strain
of −1% has the longest duration time of negative capacitance as
shown in Fig. 4(b).
The phase-field simulation not only give the phase diagrams
in Fig. 4, but also provides the detailed temporal and spatial po-
larization evolution during the transient NC. Video S1 and Fig.
S2(a)–(e) show the snapshots of the polarization evolution pro-
cess of PZT film, which are corresponding to the time step at point
A, B, C, D, andE in Fig. 2(a), respectively. For the PZT thin film in
monoclinic phase or tetragonal phase, the polarization at initial
state is along the direction of applied electric field E3 . When the
direction of electric field is reversed, the magnitude of polarization
decreases to zero gradually and polarization keeps along the thick-
ness direction, then the magnitude of polarization increases to the
magnitude of saturation along the reverse direction, and the po-
larization switching process is finished. On the other hand, for or-
thorhombic phase (ε > 0.4%, near MPB), |P1 | = |P2 | > 0 and |P3 | = 0
without electric field. When the electric field is applied at the ini-
tial state, the polarization component |P3 | > 0. With the reversing
of the direction of electric field, the polarization rotates from the
initial state to the final stable state gradually. During the rotation
of polarization, the direction of polarization components P1 and P2
remain unchanged while the direction of P3 is reversed, as shown
in Fig. S2(f)–(j) and Video S2.
The temperature is another important parameter to influence
the transient NC of ferroelectric materials. Fig. 5(a) presents the
temperature versus strain phase diagram of transient NC for the
thin film with the composition x = 1. The similar phase diagrams
for the compositions x = 0.1 and x = 0.5 are given in the Fig. S1(a)
and (b), respectively, in the Supplementary Materials. The phase
diagrams are divided as two regions. One is the region with tran-
sient NC, whereas the other region is the positive capacitance.
The phase boundary between negative and positive capacitances
is a straight line, which is related to the linear relationship of α3∗
with the strain and temperature. The temperature versus compo-
sition phase diagram with different epitaxial strains of ε = −1%,
ε = 0 and ε = 1% are also constructed in Fig. 5(b)–(d), respectively.
Although strain can result in significant inflection of the phase
boundary near MPB, a higher temperature always decreases the
magnitude of negative capacitance as shown in Fig. 5(b)–(d). It
should be noted that the compressive epitaxial strain strength-
ens the transient NC and even maintains it up to the temperature
higher than the Curie temperature of PZT bulk near MPB as shown
in Fig. 5(b), whereas the tensile strain weakens the transient NC
and makes it disappear completely at MPB as shown in Fig. 5(d).
When the strain is tensile or zero, there is no transient NC in the
ferroelectric capacitor near MPB for all temperature as shown in
Fig. 5(c) and (d). However, under a compressive strain of ε = −1%,
the transient NC near MPB is even larger than that of PTO when
temperature is higher than 600 K, which implies that the transient
NC of PZT near MPB can exist at high temperature with a compres-
sive epitaxial strain. The anomalous transient NC near the MPB at
high temperature is due to the presence of tetragonal phase in the
ferroelectric thin films subjected to the compressive strain. As a
result, the free energy profile of U − P 3 is still in double well state
at high temperature, where the negative curvature of the energy
profile can be found. Thus, the anomalous transient NC near the
MPB at high temperature is realized with the compressive misfit
strain.
6
Acta Materialia 206 (2021) 116607
4. Conclusion
In this paper, we have theoretically studied the influence of me-
chanical strain on the transient NC in ferroelectric materials based
on time-dependent Ginzburg-Landau theory and Kirchhoff’s law.
The results show that the epitaxial strain can considerably influ-
ence the transient NC of PZT thin films in an R-FEC circuit. A com-
pressive strain increases both the magnitude and the duration of
transient NC while a tensile strain reduces these properties. In par-
ticular, the tensile strain or zero strain makes the transient NC
completely disappear near the MPB at all range of temperature,
whereas the compressive strain maintains it up to a temperature
higher than the Curie temperature of PZT bulk. The anomalous
transient NC near the MPB at high temperature is due to the pres-
ence of tetragonal phase in the ferroelectric thin films subjected to
the compressive strain. This work reveals a new way to tune the
transient NC in the widely used PZT thin films by strain and com-
position engineering.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgment
The authors acknowledge the financial support from the
National Natural Science Foundation of China (Grant No. 11972320)
and Zhejiang Provincial Natural Science Foundation (Grant No.
LZ17A020 0 01).
Supplementary materials
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.actamat.2020.116607.
References
[1] A.D. Franklin, Nanomaterials in transistors: from high-performance to thin-film
applications, Science 349 (2015) aab2750 aab2750–aab2750.
[2] S.E. Thompson, S. Parthasarathy, Moore’s law: the future of Si microelectronics,
Mater. Today 9 (2006) 20–25.
[3] J.D. Meindl, Limits on silicon nanoelectronics for terascale integration, Science
293 (2001) 2044–2049.
[4] S. Salahuddin, S. Datta, Use of negative capacitance to provide voltage amplifi-
cation for low power nanoscale devices, Nano Lett. 8 (2008) 405–410.
[5] M. Hoffmann, F.P.G. Fengler, M. Herzig, T. Mittmann, B. Max, U. Schroeder,
R. Negrea, P. Lucian, S. Slesazeck, T. Mikolajick, Unveiling the double-well en-
ergy landscape in a ferroelectric layer, Nature 565 (2019) 464–467.
[6] S.-C. Chang, U.E. Avci, D.E. Nikonov, S. Manipatruni, I.A. Young, Physical origin
of transient negative capacitance in a ferroelectric capacitor, Phys. Rev. Appl. 9
(2018) 014010.
[7] V.V. Zhirnov, R.K. Cavin, Negative capacitance to the rescue? Nat. Nanotechnol.
3 (2008) 77–78.
[8] S. Smith, K. Chatterjee, S. Salahuddin, Multidomain phase-field modeling of
negative capacitance switching transients, IEEE Trans. Electron Devices 65
(2018) 295–298.
[9] H.W. Park, J. Roh, Y. Bin Lee, C.S. Hwang, Modeling of negative capacitance in
ferroelectric thin films, Adv. Mater. 1805266 (2019) 1–23.
[10] K. Majumdar, S. Datta, S.P. Rao, Revisiting the theory of ferroelectric negative
capacitance, IEEE Trans. Electron Devices 63 (2016) 2043–2049.
[11] M. Hoffmann, A.I. Khan, C. Serrao, Z. Lu, S. Salahuddin, M. Pešić, S. Slesazeck,
U. Schroeder, T. Mikolajick, Ferroelectric negative capacitance domain dynam-
ics, J. Appl. Phys. 123 (2018) 184101.
[12] S. Salahuddin, R. Ramesh, X. Pan, P. Yu, A. Islam Khan, D. Bhowmik, S. Joo
Kim, Experimental evidence of ferroelectric negative capacitance in nanoscale
heterostructures, Appl. Phys. Lett. 99 (2011) 113501.
[13] W. Gao, A. Khan, X. Marti, C. Nelson, C. Serrao, J. Ravichandran, R. Ramesh,
S. Salahuddin, Room-temperature negative capacitance in a ferroelectric–di-
electric superlattice heterostructure, Nano Lett. 14 (2014) 5814–5819.
[14] D.J.R.R. Appleby, N.K. Ponon, K.S.K.K. Kwa, B. Zou, P.K. Petrov, T. Wang, N.M. Al-
ford, A. O’Neill, A. O’Neill, Experimental observation of negative capacitance in
ferroelectrics at room temperature, Nano Lett. 14 (2014) 3864–3868.
C. Liu and J. Wang
[15] A.I. Khan, K. Chatterjee, B. Wang, S. Drapcho, L. You, C. Serrao, S.R. Bakaul,
R. Ramesh, S. Salahuddin, Negative capacitance in a ferroelectric capacitor, Nat.
Mater. 14 (2015) 182–186.
[16] S.J. Song, Y.J. Kim, M.H. Park, Y.H. Lee, H.J. Kim, T. Moon, K. Do Kim, J.-H. Choi,
Z. Chen, A. Jiang, C.S. Hwang, Alternative interpretations for decreasing voltage
with increasing charge in ferroelectric capacitors, Sci. Rep. 6 (2016) 20825.
[17] P. Zubko, J.C. Wojdeł, M. Hadjimichael, S. Fernandez-Pena, A. Sené,
I. Luk’yanchuk, J.-M. Triscone, J. Íñiguez, Negative capacitance in multidomain
ferroelectric superlattices, Nature 534 (2016) 524–528.
[18] X. Liu, R. Liang, G. Gao, C. Pan, C. Jiang, Q. Xu, J. Luo, X. Zou, Z. Yang, L. Liao,
Z.L. Wang, MoS2 negative-capacitance field-effect transistors with subthreshold
swing below the physics limit, Adv. Mater. 30 (2018) 1–8.
[19] A.K. Yadav, K.X. Nguyen, Z. Hong, P. García-Fernández, P. Aguado-Puente,
C.T. Nelson, S. Das, B. Prasad, D. Kwon, S. Cheema, A.I. Khan, C. Hu, J. Íñiguez,
J. Junquera, L.Q. Chen, D.A. Muller, R. Ramesh, S. Salahuddin, Spatially resolved
steady-state negative capacitance, Nature 565 (2019) 468–471.
[20] J.J. Wang, X.Q. Ma, Q. Li, J. Britson, L.Q. Chen, Phase transitions and do-
main structures of ferroelectric nanoparticles: phase field model incorporating
strong elastic and dielectric inhomogeneity, Acta Mater. 61 (2013) 7591–7603.
[21] N.A. Pertsev, A.G. Zembilgotov, A.K. Tagantsev, Effect of mechanical boundary
conditions on phase diagrams of epitaxial ferroelectric thin films, Phys. Rev.
Lett. 80 (1998) 1988–1991.
[22] F. Sun, H. Khassaf, S.P. Alpay, Strain engineering of piezoelectric properties of
strontium titanate thin films, J. Mater. Sci. 49 (2014) 5978–5985.
[23] X. Hou, H. Wu, H. Li, H. Chen, J. Wang, Giant negative electrocaloric effect in-
duced by domain transition in the strained ferroelectric thin film, 30 (2018)
465401.
[24] M. Hoffmann, M. Pešić, K. Chatterjee, A.I. Khan, S. Salahuddin, S. Slesazeck,
U. Schroeder, T. Mikolajick, Direct Observation of Negative Capacitance in Poly-
crystalline Ferroelectric HfO2 , Adv. Funct. Mater. 26 (2016) 8643–8649.
[25] N. Zhang, H. Yokota, A.M. Glazer, Z. Ren, D.A. Keen, D.S. Keeble, P.A. Thomas,
Z.-G. Ye, The missing boundary in the phase diagram of PbZr1−x Tix O3 , Nat.
Commun. 5 (2014) 5231.
Acta Materialia 206 (2021) 116607
[26] J. Wang, T.-Y. Zhang, Influence of depolarization field on polarization states in
epitaxial ferroelectric thin films with nonequally biaxial misfit strains, Phys.
Rev. B. 77 (2008) 014104.
[27] A.K. Saha, S. Datta, S.K. Gupta, “Negative capacitance” in resistor-ferroelectric
and ferroelectric-dielectric networks: apparent or intrinsic? J. Appl. Phys. 123
(2018) 105102.
[28] Y.J. Kim, H.W. Park, S.D. Hyun, H.J. Kim, K. Do Kim, Y.H. Lee, T. Moon, Y. Bin Lee,
M.H. Park, C.S. Hwang, Voltage drop in a ferroelectric single layer capacitor by
retarded domain nucleation, Nano Lett. 17 (2017) 7796–7802.
[29] J. Wang, T.Y. Zhang, Effects of nonequally biaxial misfit strains on the phase di-
agram and dielectric properties of epitaxial ferroelectric thin films, Appl. Phys.
Lett. 86 (2005) 192905.
[30] J. Wang, Y. Li, L. Chen, T. Zhang, The effect of mechanical strains on the ferro-
electric and dielectric properties of a model single crystal–phase field simula-
tion, Acta Mater. 53 (2005) 2495–2507.
[31] S.-C.C. Chang, A. Naeemi, D.E. Nikonov, A. Gruverman, Theoretical approach
to electroresistance in ferroelectric tunnel junctions, Phys. Rev. Appl. 7 (2017)
1–12.
[32] D.J. Kim, J.Y. Jo, T.H. Kim, S.M. Yang, B. Chen, Y.S. Kim, T.W. Noh, Observation
of inhomogeneous domain nucleation in epitaxial Pb(Zr,Ti)O3 capacitors, Appl.
Phys. Lett. 91 (2007) 132903.
[33] Y.W. So, D.J. Kim, T.W. Noh, J.G. Yoon, T.K. Song, Polarization switching kinetics
of epitaxial Pb(Zr0.4Ti 0.6)O3 thin films, Appl. Phys. Lett. 86 (2005) 1–3.
[34] Y. Kim, H. Han, W. Lee, S. Baik, D. Hesse, M. Alexe,
Non-Kolmogorov−Avrami−Ishibashi Switching dynamics in nanoscale fer-
roelectric capacitors, Nano Lett. 10 (2010) 1266–1270.
[35] Z.C. Yuan, S. Rizwan, M. Wong, K. Holland, S. Anderson, T.B. Hook, D. Kienle,
S. Gadelrab, P.S. Gudem, M. Vaidyanathan, Switching-speed limitations of fer-
roelectric negative-capacitance FETs, IEEE Trans. Electron Devices 63 (2016)
4046–4052.