Thin Solid Films 583 (2015) 1318

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Thin Solid Films

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Mechanism of ferroelectric resistive switching in Bi0.9La0.1FeO3 thin lms

R.L. Gao a,b,, C.L. Fu a, W. Cai a, G. Chen a, X.L. Deng a, H.W. Yang b, J.R. Sun b, Y.G. Zhao c, B.G. Shen b
a
b
c

School of Metallurgy and Materials Engineering, Chongqing University of Science and Technology, Chongqing 401331, China
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Science, Beijing 100190, China
Department of Physics, State Key Laboratory of Low-Dimensional Quantum Physics, Tsinghua University, Beijing 100084, China

a r t i c l e

i n f o

Article history:
Received 24 April 2014
Received in revised form 17 March 2015
Accepted 18 March 2015
Available online 27 March 2015
Keywords:
Switching mechanism
Resistive switching
Bismuth lanthanum ferrite
Thin lms
Pulsed laser deposition

a b s t r a c t
Resistive switching devices are considered as one of the most promising candidates for the next generation memories and nonvolatile logic applications. In this paper, we report an anomalous resistive switching effect in BiFeO3
based hetero-structures. Different from conventional resistive switching devices made of metal oxides, no
forming process is needed to obtain a stable resistive switching effect in the ferroelectric resistive switching devices. Both positive and negative current peaks are observed under forward bias and reverse bias, respectively,
suggesting that exible Schottky-like barriers and conductive channels form at the top and bottom interfaces,
which play important roles in the resistive switching of Ag/Bi0.9La0.1FeO3/La0.3Sr0.7MnO3 sandwiched structures.
These exible Schottky-like barriers may come from the migration of charged oxygen vacancies/ions under the
electric eld of sweeping bias and the redistribution of carriers with ferroelectric switching, while the conductive
channel resulted from charged oxygen vacancies/ions. These results demonstrate promising prospects for application of the ferroelectric resistive switching effect at interfaces to nonvolatile memory.
2015 Elsevier B.V. All rights reserved.

1. Introduction
Resistive switching phenomena in metal oxides have attracted
considerable attention not only due to its advantages in high-speed
switching but also because of the potential high-density memory applications. The resistive switching phenomena have been observed in
capacitor-like structures consisting of various metal oxides, such as
multielemental perovskite-type oxides [14] and binary oxides [59],
and the observed resistive switching behaviors differ depending on
the material.
Ferroelectric resistive switching effects can be categorized into two
types depending on the mechanism involved. The tunnel electroresistance effect [1012] relies on a change in tunneling barrier height
induced by polarization reversal. For the resistive switching of a ferroelectric Schottky diode [79,13], a Schottky-like barrier forms at the interface between a metal electrode and conductive ferroelectric oxide,
and the potential prole of the Schottky-like barrier is reversibly modied by the polarization ipping. Resistive switching has been reported
recently in BiFeO3(BFO) thin lms [1416], which have been intensively
investigated concerning their multiferroic properties [1719]. Ferroelectric resistive switching effects have usually been studied in terms
of hysteretic currentvoltage (IV) characteristics [15,17,18,20], but investigation of the switching characteristics in the pulse-voltage mode is
needed for memory applications.
Corresponding author.
E-mail address: gaorongli2008@163.com (R.L. Gao).

http://dx.doi.org/10.1016/j.tsf.2015.03.038
0040-6090/ 2015 Elsevier B.V. All rights reserved.

This work mainly focuses on the analysis of the transport characteristics of the resistive switching. IV measurements with a higher voltagesweep frequency (f) reveal that ferroelectric displacement charges owed
prior to set and reset switching processes, suggesting that the exible
Schottky-like barrier forms at the top interface, and the exible
Schottky-like barrier plays an important role in the resistive switching
of Ag/BLFO/LSMO sandwiched structures.
2. Experimental process
Bi0.9La0.1FeO3 (BLFO) thin lms with 350 nm thickness were grown
epitaxially on the La0.7Sr0.3MnO3 (LSMO) coated (001) SrTiO3 (STO)
substrates using pulsed laser deposition (PLD). The doping of 10% La
was used to decrease the leakage current. The target was prepared by
mixing Bi2O3, La2O3 and Fe2O3 in a 1.1:0.1:1 stoichiometric ratio and
sintering at 800 C in air. The extra amount of Bi2O3 was used to compensate for the easy volatilization of Bi. For the study of electrical properties, the conductive metallic oxide LSMO layer with the thickness of
30 nm serves as the bottom electrode. LSMO was chosen as bottom electrode because its lattice parameter (LSMO ~ 0.388 nm) is very close to
STO (~ 0.391 nm), BFO (~ 0.396 nm), and therefore, with small lattice
parameter mismatch and stress, one expects the epitaxial growth.
First, a sintered stoichiometric LSMO target was employed for deposition of LSMO thin lms on STO substrates under a deposition temperature of 700 C, and an oxygen pressure ~50 Pa. Then, the BLFO thin lms
were grown at 650 C under a low oxygen pressure of 15 Pa. The other
laser parameters during depositions were (i) laser source: KrF excimer

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R.L. Gao et al. / Thin Solid Films 583 (2015) 1318

laser with = 248 nm, (ii) repetition frequency: 5 Hz, and (iii) energy
density was about 1.5 J/cm2. Typical lm growth rate was around 9 nm
per minute. In order to ensure oxygen equilibrium, the lms were slowly cooled to room temperature (2 C/min) in the oxygen atmosphere of
100 Pa. For measuring the electrical properties of the lms, a 200 nm
thick Ag layer patterned with 0.2 mm diameter was deposited on
BLFO as the top electrodes by PLD through a shadow mask. Structural characterization of the BLFO lms was performed using X-ray diffraction (XRD, Bruker D8-Discover system), with a Cu K radiation,
with a characteristic wavelength of 1.5418 . The X-ray diffractometer was set up in the BraggBrentano geometry. The X-rays were
generated from a Cu anode supplied with 40 kV and a current of
40 mA. Leakage current and polarization hysteresis loop measurements were carried out using two probes connected with Radiant
test system Premier-II. The IV measurements were performed by

Fig. 1. (a) XRD patterns of BLFO/LSMO/STO lms with 2 in the range of 1080, inset
shows the rocking curve of (002) BLFO peak. (b) Polarization hysteresis loops of BLFO
lms at room temperature. (c) Rectifying and hysteretic IV curves of Ag/BLFO/LSMO;
Ag is positively biased and LSMO is grounded. The arrows indicate the sweep direction
of the bias.

computer controlled Keithley 2611 source meter and oscilloscope

monitored pulse generator.
3. Results and discussion
Fig. 1(a) shows the 2 XRD patterns of the 350 nm BLFO thin lms.
One can clearly see that only the (00 l) (l = 1, 2, 3) peaks of BLFO and
STO are visible, indicating pure single-oriented perovskite BLFO phase.
The inset of Fig. 1(a) shows the rocking curve of the BLFO (002) peak;
the full width at half maximum is about 0.40.5, which is slightly
narrower than the value reported by Dho et al. [21]. The ferroelectric
properties of the BLFO lms have been investigated at room temperature.
Fig. 1(b) shows polarization hysteresis loops (PE) measured at a frequency of 10 kHz. The corresponding current response is also shown to
better understand the ferroelectric switching behavior. This obtained
value for Pr is slightly larger than the value obtained for other BFO lms
(~60 C/cm2) [2224].
Owing to the high polarization of the BLFO thin lms and its possible
application in data storage, it is very important to understand the resistive switching characteristics. Fig. 1(c) shows IV curves of our samples,
the voltage step is 0.2 V with the step time of 0.1 s. The numbers 14 and
the arrows indicate the scanning direction of the applied voltages. The
sample shows typical bipolar resistive switching behavior without an
electroforming step is necessary before the observation of the hysteretic
IV curves. It can be easily concluded that the positive-voltage sweep induces set (exhibits low resistance state (LRS)) followed by reset (be
switched to high resistance state (HRS)). The initial reset state with
high resistance is recovered by a similar sweep under negative polarity.
The slightly asymmetric of IV curves is thought to be due to the formation of a Schottky-like barrier at the Ag/BLFO and BLFO/LSMO interfaces,
as well as the different barrier between this two interfaces. In addition
to the bipolar resistive switching behavior, two current peaks can be
observed at about +6 V and 3.5 V in the sweeping process 1 and 3,
respectively. This abrupt current change often appears in ferroelectric
lms and this large values of current peaks is generally regarded as
the charges owing through the circuit when the sample polarization
reverses [2527]. However, the occurrence of the peak can also be easily
explained by the phenomenon of complementary switching or complementary resistive switching in some non-ferroelectric lms such as
HfOx based devices, with the formation and rupture of laments resulted by ion-migration [2830]. Therefore, it is of great importance and urgency to nd out whether this current peak is induced by polarization
switching or ion-migration or both of them.
In order to analyze how the current peak occurs, the negative part of
the IV curves was measured at different sweeping voltages varying
from 3.5 V to 8 V, as shown in Fig. 2(a)(d). It can be seen that
when the maximum sweeping voltage is 3.5 V, no current peak is
observed, only a rather gradually changing current is observed during
resistive switching, i.e., in the sweeping process, the resistive state
switches from HRS to LRS, which indicates the interface-mediated resistive switching. As the sweeping voltage increases to 4 V and 5 V,
cross curves can be observed at about 3.7 V and 3.2 V, respectively,
shown in Fig. 2(b) and (c). The cross curve voltage (Vcc) is dened as
the voltage which the current of forward and backward sweeping is
the same, it can be seen from Fig. 2(b)(c) that the Vcc decreases
from 3.7 V to 2.7 V while the sweeping voltage increases from
3.7 V to 2.7 V, and the cross curve will become less obvious if the
voltage further increases. As the sweeping voltage increases to 8 V,
besides the observed current peak, the cross curve disappears entirely
and the resistive state is exactly high (or low) in the backward (or forward) sweeping, as shown in Fig. 2(d). Besides, when a current peak appears, then the current decreases with increasing voltage, and a cross
curve can also be observed, as shown in Fig, 2(c) and (d). One can nd
that once the sweeping voltage exceeds Vcc, the HRS and LRS will be exchanged, which indicates that there may be another physical resistive
switching that existed and this mechanism is primary when V N Vcc.

R.L. Gao et al. / Thin Solid Films 583 (2015) 1318

15

Fig. 2. IV curves after BLFO lm polarized by +30 V in different sweeping negative bias of 3.5 V (a), 4 V (b), 5 V (c) and 8 V (d), respectively. (e) 1st and 2nd cycles of IV curves
after BLFO lm polarized by +30 V and 30 V, respectively (f) IV curves after BLFO lm polarized by different negative pulse voltages, before each negative voltage, +30 V pulse voltage
was applied. Inset is the schematic of the pulse sequence.

These results suggest that the device is switching at both interfaces. As

shown in Fig. 2(a), one interface switches to LRS. If the voltage is increased the second interface switches to the OFF state (Fig. 2bc).
Sweeping with opposite polarity rst switches the second interface
into ON state and then the rst interface into ON state. As the current
peak appears in high sweeping voltage, it may be that the electric polarization state of BLFO lms may be changed under higher electric eld.
Therefore, it can be deduced that Schottky-like barrier forms at the interface and the Schottky-like barrier may come from the migration of
charged oxygen vacancies/ions under the electric eld of writing bias
[29] and the redistribution of carriers with ferroelectric switching [31].
To elucidate the mechanism of the abnormal resistive switching and
current peak observed in the IV curves, pulse voltages of + 30 V
and 30 V (with the pulse lengths of 20 s) were applied to the
sample before IV sweeping, as shown in Fig. 2(e). It can be seen

from Fig. 2(e) that after applying + 30 V pulse voltage, the current
shows a peak in the sweeping process from 0 to 6 V, however, in
the 2nd sweeping process, the peak disappeared but a small loop can be
observed. There was no current peak observed both in the 1st and 2nd cycles after a 30 V pulse voltage was applied. Moreover, anomalous HRS
and LRS are also exhibited after being polarized by 30 V and +30 V, respectively. These results seem to indicate that the current peak originated
from the transient current of the polarization orientation switching. Nevertheless, it can be seen from the PE curves [Fig. 2(b)] that the coercive
electric eld is ~17 V, which is far larger than the voltage of the corresponding current peak (~4 V) that happens in the negative orientation.
As another example, before each sweeping process, the sample was polarized to different polarization states by choosing proper negative pulse
voltages, as seen in Fig. 2(f). It can be seen from Fig. 2(f) that current
peak exhibits only when the pulse voltage doesn't exceed 18 V,

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R.L. Gao et al. / Thin Solid Films 583 (2015) 1318

which is roughly equal to the coercive electric eld (~17 V). When the
negative pulse voltage is larger than the coercive electric eld, no current
peak can be observed at all. This result once again indicates that the current peak is indeed associated with the polarization variation.
To further analyze the polarization switching in the IV sweeping
process, triangle wave voltage with the amplitude of 30 V with different
periods was applied to measure the polarization variation. Fig. 3(a) displays the repeated measurement of IV characteristics of the Ag/BLFO/
LSMO device with the triangle wave period of 144 s. The initial IV
curve (i.e., the 1st cycle) is almost identical to that obtained from the
second measurements. These results mentioned above suggest that
no forming process is needed to obtain stable resistive switching in
our device. This lack of need for a forming process suggests that the
observed resistive switching does not rely on the formation of conductive laments observed in other oxides. Besides, the peak current distinctly increases with the sweep-period from 144 s to 4.5 s, as can
be seen in Fig. 3(b), further conrming the domination of the ferroelectric switching. Under a faster voltage sweep, a larger transient current
would be expected due to the polarization switching in a shorter time.
It notes that the ferroelectric switching (in microsecond time scale
[32]) is much faster than our voltage sweeping (in second time scale).
Fig. 3(c) shows the switched polarization as a function of the period of
the triangle wave. It can be seen that the switched polarization increases
with the period, and then tends to saturate while the period exceeds
18 s. The maximum P value was estimated to be ~ 50 C/cm2, which
is slightly smaller than that obtained from Fig. 1b (~80 C/cm2). Considering the fact that the polarization estimated by current integration
from IV curves involves the leakage current part induced by ionic migration such as oxygen vacancies. This result suggests that the ferroelectric displacement current is not the predominant cause of the observed
current peaks, and that polarization ipping is only involved in the resistive switching of the device.

To further prove that the peak current is not entirely induced by

polarization switching, the whole and the segmented IV curves were
measured, the sample was pre-polarized by + 30 V pulse voltage in
order to ensure that the polarization state is basically the same before
each measuring curve. The results are shown in Fig. 3(d). The whole
sweeping process is 0 8 V 0, and the current peak occurs at
~ 3.7 V. When the voltage swept from 0 to 3 V, 3 to 5.25 V and
5.25 V to 8 V, in the 1st, 2nd and 3rd segments, respectively, it
can be seen from the overlying of each segment curves that the overlying is roughly identical to that of the whole process. This result indicates
that the peak current is not entirely transient, but a relatively stable one.
Otherwise, the current at the voltage of 5.25 V must be larger than
that at 3.75 V (corresponding to the current peak), because larger
voltage should be corresponding to greater transient current that resulted from polarization switching. Considering the fact that the current
peak occurs only when the sweeping voltage is big enough and the sample is pre-sweeping or pre-polarized by opposite sign of the voltage (see
Figs. 1(c) and 2), and the peak current is not entirely transient (see
Fig. 2(f)). Moreover, even considering the contribution of leakage current, the maximum P (~50 C/cm2) estimated from Fig. 3(b) is always
smaller than that obtained from Fig. 1(b) (~80 C/cm2). Therefore, we
argue that the current peak should consists of two parts, the transient
current (caused by polarization switching) and the quasi-steady-state
current (ionic current and oxygen vacancy current). The migration
time for the uniform oxygen vacancies decreases with the temperature, and can vary from ~109 s (at ~300 K) to ~10 s (at ~500 K) [33]. The
relaxation time for the carrier trapping/detrapping is also above 100 s
time [34,35]. Such long migration/relaxation times are consistent with
the observations in Fig. 3(d).
To elucidate how the current peak occurs, it is necessary to investigate the conduction mechanism for both the HRS and LRS. Based on
the discussion mentioned above that the device is switching at both

Fig. 3. (a) Repetition behavior of the hysteretic IV characteristics of the Ag/BLFO/LSMO device. The arrows indicate the sweep direction of the bias. Inset is the schematic of the pulse.
(b) Hysteretic IV characteristics under different pulses. The lines indicate different sweeping rate varying from 4.5 s to 144 s. The numbers 1 to 4 mean the sweeping sequence, and
the green arrow shows the varying trend of the corresponding voltages at the current peak. (c) Obtained polarization from Fig. 3(b) as a function of periods. (d) The whole and segment
of IV curves in the sweeping process. (For interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)

R.L. Gao et al. / Thin Solid Films 583 (2015) 1318

interfaces, when the sweeping voltage smaller than Vcc, one interface
switches to LRS. If the voltage is larger than Vcc, the second interface
switches to the OFF state. Sweeping or pulse voltage with opposite polarity rst switches the second interface into ON state and then the
rst interface into ON state. As oxygen vacancies (OV) with positive
charge can attract electron, therefore, they act as electron trapping centers [3639]. Therefore, it can be deduced that Schottky-like barrier
forms at the interface and the Schottky-like barrier may come from
the migration of charged oxygen vacancies/ions under the electric
eld of writing bias [29] and the redistribution of carriers with ferroelectric switching [31]. In order to get further insight into the interface and
polarization switching effect on the resistive switching, the corresponding bandstructure at different states is also presented in Fig. 4. Considering the different work functions of Ag, BLFO and LSMO that, the barrier
height of the BLFO/LSMO junction is always higher than that of the
Ag/BLFO junction both in LRS and HRS [40,41], therefore, the current
in the negative bias part is mainly limited by the Ag/BLFO interface and
the current in the negative bias part is always smaller than that in the positive part, as shown in Fig. 1(c).
In the polarization switching process, the domains move, nucleate
and grow, which is in favor of the trapped electrons inside the BLFO
thin lm easy to be released and emitted into LSMO bottom electrode,
and iron ions are reduced from Fe2 + to Fe3 +, which destroys the
electron hopping paths. Therefore, after applying a positive voltage,
Schottky-like contact forms at both the top and bottom interfaces, as
shown in Fig. 4(a), and the current is controlled by t (here t is the
top barrier height between Ag top electrode and BLFO lm) by applying
a negative reading bias, if the negative sweeping voltage is less than Vcc,
it is too small to switch the polarization, only the oxygen vacancies can
move accompanying sweeping, and a small current ow (HRS). After
applying negative voltage sweeping, for one hand, t decreases while
b (here b is the bottom barrier height between bottom LSMO electrode and BLFO lm) increases as oxygen vacancies move toward the
top interface as the negative sweeping voltage, and thus the resistance
can be switched from HRS to LRS, as shown in Fig. 2(a). As the negative
sweeping voltage increases, t further decreases and some conductive
channels may be formed as a result of ionic migration, as shown in

17

Fig. 4(b) and (c), therefore, the device can be switched to a lower resistive state, as shown in Fig. 2(b). While the voltage increases, although t
further decreases, the conductive channels may be switched off as a
result of joule heating (Fig. 4(d)), thus the current decreases suddenly
as can be seen from Fig. 2(c). When the sweeping voltage increases to
8 V, the current increases again after a low, t further decreases
resulting from the migration of charged oxygen vacancies/ions under
the electric eld of writing bias and the redistribution of carriers with
some of the ferroelectric switching, as shown in Fig. 4(e). A Schottkylike contact forms at the bottom interface, and the current is controlled
by b, by applying a negative reading bias, b is forward biased and a
large current ow (LRS), which is consistent with that in Fig. 2(d).
These results suggest that exible Schottky-like barrier forms at the
top interface, and the exible Schottky-like barrier plays an important
role in the resistive switching of Ag/BLFO/LSMO sandwiched structures.
The exible Schottky-like barrier may come from the migration of
charged oxygen vacancies/ions under the electric eld of sweeping
bias and the redistribution of carriers with ferroelectric switching. As
the structures do not show ferroelectric switching under the sweeping
bias, so the exible Schottky-like barrier is supposed to result from the
migration of charged oxygen vacancies/ions. The accumulation of
charged oxygen vacancies/ions in the interface effectively reduces the
corresponding Schottky-like barrier as BFO can be regarded as n-type
semiconductor due to the naturally produced oxygen vacancies, while
the Schottky-like barrier is recovered when the charged oxygen vacancies/ions drift away from the interface, which has been used to explain
the resistive switching behavior in other samples [11,12]. The corresponding bandstructure presented in Fig. 4 can explain the pulse voltage results in Fig. 2(e) and (f) well. The role of positive pulse voltage
is just like that of positive sweeping, resulting oxygen vacancies accumulated at the bottom interface, thus induces exible Schottky-like
barriers.
4. Conclusions
In summary, an abnormal resistive switching effect has been
observed at rectifying Ag/BLFO interfaces and the impact of oxygen

Fig. 4. The schematic diagram of the barrier of Ag, BLFO and LSMO, Schottky-like contact forms at both the top and bottom interfaces. (a) after applied positive pulses or positive voltage
sweeping, (b) after negative voltage (less than Vcc) sweeping. (c) after negative voltage (larger than Vcc) sweeping. (d) after the negative sweeping voltage further increased. (e) the
negative sweeping voltage further increase and much larger than Vcc. t and b indicate top barrier between Ag/BLFO and bottom barrier of BLFO/LSMO, respectively. The cycle dots denote
oxygen vacancies and the arbitrary curves express conductive channels.

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R.L. Gao et al. / Thin Solid Films 583 (2015) 1318

deciencies on its characteristics was presented and discussed. Unlike

conventional resistive switching devices made of metal oxides, no
forming process is needed to obtain a stable resistive switching effect
in the ferroelectric resistive switching devices. In IV characteristics
measured at a voltage-sweep model, positive and negative current
peaks were observed under forward bias and reverse bias, respectively,
suggesting that exible Schottky-like barriers and conductive channels
may form at the top and bottom interfaces, and these exible Schottkylike barriers and conductive channels play important roles in the resistive
switching of Ag/BLFO/LSMO sandwiched structures. These conductive channels may come from the migration of charged oxygen
vacancies/ions under the electric eld of sweeping bias, while the
exible Schottky-like barriers come induced by oxygen vacancies/
ions and the redistribution of carriers with ferroelectric switching.
Acknowledgments
The present work has been supported by the Knowledge Innovation Project of the Chinese Academy of Sciences (KZCX3-SW-127),
the Beijing Municipal Natural Science Foundation (1132004),
the National Natural Science Foundation of China (Grant Nos.
51372283, 51402031, 61404018), the Natural Science Foundation
Project of CQ(CSTC2012jjA50017) and the cooperative project of academician workstation of Chongqing University of Science & Technology (CKYS2014Z01, CKYS2014Y04).
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