Current Applied Physics 31 (2021) 22–28

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Current Applied Physics

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

Coexistence of nonvolatile unipolar and volatile threshold resistive

switching in the Pt/LaMnO3/Pt heterostructures
Yanfeng Yin a, b, Chaoyang Kang a, Caihong Jia a, *, Weifeng Zhang a, **
a
Henan Key Laboratory of Photovoltaic Materials, Henan University, Kaifeng, 475004, PR China
b
School of Physics & Electronics, Henan University, Kaifeng, 475004, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: Coexistence of nonvolatile unipolar and volatile threshold resistive switching is observed in the Pt/LaMnO3
Unipolar resistance switching (LMO)/Pt heterostructures. The nonvolatile unipolar memory is achieved by applying a negative bias, while the
Threshold resistance switching volatile threshold resistive switching is obtained under a positive bias. Additionally, the pristine low resistance
Oxygen vacancy
state (LRS) could be switched to high resistance state (HRS) by the positive voltage sweeping, which is attributed
Insulator-to-metal transition
Oxide heterostructure
to the conduction mechanism of Schottky emission. Subsequently, the insulator-to-metal transition in the LMO
film due to formation of ferromagnetic metallic phase domain contributes to the volatile threshold resistive
switching. However, the nonvolatile unipolar switching under the negative bias is ascribed to the formation/
rupture of oxygen-vacancy conducting filaments. The simultaneously controllable transition between nonvolatile
and volatile resistance switching by the polarity of the applied voltage exhibits great significance in the appli­
cations of in-memory computing technology.

1. Introduction number of unwanted sneak-path currents [12,13], which could be

The resistive switching (RS) is a phenomenon that the resistance of a
device can be changed by an external electrical stimulation [1–4], which
is the core of burgeoning technologies such as neuromorphic computing
and resistive memories [4–6]. Generally, the resistive switching is
categorized into two types of nonvolatile memory RS and volatile
threshold RS [2]. For the nonvolatile memory RS, resistive variable
memory realizes data storage by using the mutual conversion between
the high-resistance and low-resistance states under the condition of
electric excitation, which has the advantages of small unit size [3], fast
reading and writing speed [7], low power consumption [8], simple
fabrication process [9]. In contrast, the volatile threshold RS could only
be stabilized at HRS under zero bias, which hinders its application in
nonvolatile memory [2]. However, because of its volatility (the LRS can
only be obtained under a high enough external voltage or current),
threshold RS exhibits potential applications in frontier regions including
neuromorphic devices [4,10], novel true random number generators [9]
and voltage selectors in resistive random access memories [6,11].
Especially, in perspective of in-memory computing, the cross-point array
memories are preferred for the size reduction of bit units, leading to a
avoided by using a device with the coexistence of unipolar memory and
threshold RS.
As proposed in previous studies, the mutual transitions between the
nonvolatile unipolar memory switching and volatile threshold switching
could be achieved on NiO by oxygen content [14], temperature [15],
compliance current [16], and electrical pulse polarity [17]. In NiOx
films, unipolar and threshold switching were found at low and high
oxygen content [14], at a measurement temperature below and above
156 K [15], at a compliance current of 1 and 10 mA [16], after applying
a negative and positive pulse of 2 V in width between 10− 2 and 10− 4 s,
respectively [17].
However, due to inconvenient conversion mode between memory
and threshold switching and poor endurance, the above NiO devices
have been compromised for practical applications. As a Mott insulator
and an A-type antiferromagnetic insulating material (with ferromag­
netic spin correlations on a (001) crystal plane and antiferromagnetism
between these crystal planes) [18], LaMnO3 (LMO) compound has been
widely studied due to its RS characteristics by controlling oxygen con­
tent or electronic reconstruction [19,20]. Recently, Liu et al. reported
that the Ag/Sr-doped LMO heterostructure can exhibit a nonvolatile

* Corresponding author.
** Corresponding author.
E-mail addresses: chjia@henu.edu.cn (C. Jia), wfzhang@henu.edu.cn (W. Zhang).

https://doi.org/10.1016/j.cap.2021.07.009
Received 17 January 2021; Received in revised form 18 June 2021; Accepted 6 July 2021
Available online 18 July 2021
1567-1739/© 2021 Korean Physical Society. Published by Elsevier B.V. All rights reserved.
 Y. Yin et al.
bipolar RS behavior, which could be attributed to the formation/rupture
of Ag nanofilaments [21]. Meunier et al. observed that the Au/LMO/­
Si3Nx/SiO2/Si heterostructure LMO exhibits an asymmetric bipolar
counter-eight wise-type switching without requiring an electroforming
step [22]. However, the unipolar RS was observed in the Au/Pr0.7
Ca0.3MnO3 heterojunctions [23]. According to the aforementioned
studies, the switching modes (unipolar and bipolar ones) in a nonvola­
tile or volatile manner may be drastically different in the
manganite-based junctions. As a consequence, exploring the new
switching modes and involved mechanism in such a memristor is
extremely important for designing the data storage and miniaturized
electronic devices.
In the present work, we report on the coexistence of the nonvolatile
unipolar memory and volatile threshold RS in the LMO thin film at room
temperature by switching the polarity of the bias voltage. The nonvol­
atile unipolar switching and volatile threshold switching are observed,
which could relate with the different migration direction of oxygen
vacancies under different voltage polarity. In particular, both stable
threshold and unipolar memory switching on the one device coexist in
the LMO heterostructures, which can be realized by versatilely con­
trolling the voltage polarity. This work sheds light on the future appli­
cations in the ReRAM and in-memory computing technology.
2. Experimental section
Polycrystalline LMO thin films were deposited on the Pt/Ti/SiO2/Si
substrate by pulsed laser deposition (PLD) using a KrF excimer laser
(248 nm, 25 ns pulse duration, COMPexPro201, Coherent) with an en­
ergy of 300 mJ and frequency of 5 Hz. The base pressure was pumped to
~2 × 10− 4 Pa. During the film growth, the substrate temperature was
maintained at 750 ◦ C, and the target-substrate distance was set to 6.5
cm. The oxygen partial pressure was 5 × 10− 4 Pa, and the growth time
was set to 20 min. Afterwards, the sample was annealed in situ for 20
min, followed by cooling process at a rate of 10 ◦ C/min in a vacuum
environment. In order to measure the electrical transport properties, the
top electrodes Pt (0.04 mm2) were sputtered on the LMO thin films
through a shadow mask by DC sputtering at room temperature. Then the
Fig. 1. (a) XRD pattern of the LMO thin film. (b) The atomic force microscope image of the LMO film. (c) Cross-sectional SEM image of the LMO film deposited on the
Pt/Ti/SiO2/Si substrate. (d) Schematic of the LMO/Pt/Ti/SiO2/Si device for the resistive switching measurement.
23
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Current Applied Physics 31 (2021) 22–28
obtained sample was finally post-annealed at 500 ◦ C for 30 min under 5
× 10− 4 Pa oxygen pressure in the same PLD chamber. Electrical trans­
port properties were measured by using Keithley 2400 source meter. The
X-ray diffraction (XRD, DX-2700) was utilized to measure the crystalline
structure of the LMO thin film. The atomic force microscope (AFM) and
scanning electron microscope (SEM) were employed to characterize the
surface morphology and interfacial cross section by Bruker Multimode 8
and JSM-7001F instrument, respectively. The chemical environments
were investigated by X-ray photoelectron spectroscopy (XPS, Kratos
AXIS ULTRA).
3. Results and discussion
According to the XRD patterns in Fig. 1(a), the LMO thin film is of
polycrystalline nature on the Pt/Ti/SiO2/Si substrate. In addition, all the
peaks were correctly indexed, indicating the LMO thin film in a pure
phase. From the AFM image in Fig. 1(b), the LMO thin film is granular
and uniform. Fig. 1(c) shows the cross sectional SEM image, indicating
the film thickness of approximately 140 nm. The device architecture is
delivered in Fig. 1(d) and the resistive switching behaviors were
measured by the two-probe technique.
Fig. 2(a) presents that the initial positive reset I–V curve of the Pt/
LMO/Pt devices. The voltage sweeping in sequences is shown by the
arrows. First, the pristine state of the Pt/LMO/Pt heterostructure is a low
resistance state (LRS), which is in an Ohmic characteristic through the
I–V fitting as labelled by “1”. Second, when the positive voltage sweeps
back, the resistance starts to increase as shown by “2”. Third, as further
decreasing the voltage (close to 2.00 V), a sharp current drop occurs,
indicating an occurrence of the HRS. In addition, the resistance state is
unstable during the voltage sweeping back to zero as marked by “3”.
Fig. 2(b) shows that a linear fitting relationship between the natural
logarithm of I [ln(I)] and the square root of the applied voltage (V1/2) for
the HRS. According to this result, we can determine that the appearance
of the HRS should be ascribed to the Schottky emission conduction
mechanism (See more details in the following discussion).
Fig. 3(a) shows that the volatile threshold switching occurs, when
again performing a positive voltage cycling. As increasing the bias
Y. Yin et al. Current Applied Physics 31 (2021) 22–28

Fig. 2. (a) The log-log scale I–V curves of Pt/LaMnO3/Pt device for the initial positive reset process. The fitting curve (red) shows the Ohmic conduction mechanism
for the LRS of the device. (b) The fitting result of the I–V curves of “3” for the HRS marked in (a). (For interpretation of the references to colour in this figure legend,
the reader is referred to the Web version of this article.)

Fig. 3. (a) 1000 consecutive positive bias volatile threshold switching cycles. (b) The statistical distribution of the Vth and Vhold with the number of cycles. The
orange solid line corresponds to a Lorentz fitting curve for the Vth. (c) The cumulative distribution of the Vth and Vhold. (d) The Vth and Vhold are as a function of the
number of cycles.

voltage, the HRS is switched to the LRS at a threshold voltage (Vth) of
around 3.40 V (on-switching) a compliance current of 0.002 A. Then the
LRS is resumed to the HRS at a low voltage (Vhold) of about 2.35 V (self-
off-switching) as decreasing the voltage. These results suggest that the
resistance states can be switched in a volatile manner with the feature of
the volatile threshold switching. To further confirm this behavior, the
threshold switching was performed with 1000 cycles. The LMO film
indeed exhibits a repeatable threshold switching behavior. The statis­
tical distribution of the Vth and Vhold with the number of cycles are
shown in Fig. 3(b). The Vhold distributes in a sharp manner. However,
the Vth distributes more diffusely, which is fitted by the Lorentz fitting as
shown in Fig. 3(b). Subsequently, the fitted threshold voltage is derived
as approximately 3.40 ± 0.40 V. The corresponding electric field is
about (2.43 ± 0.29) × 105 V cm− 1, which is comparable with the pre­
vious reports [6,9]. Fig. 3(c) shows the cumulative distributions of Vth
and Vhold. The on-switching voltages (Vth) vary within the 0.50 V range,
well consistent with the above result. However, the self-off-switching
voltages (Vhold) are almost stable at 2.35 V. The trend of Vth and Vhold
with the threshold switching cycles are shown in Fig. 3(d). The Vth de­
creases along with the cycling times, but this case is absent in the
self-off-switching voltages of Vhold. That is, the Vhold is much more stable
than the Vth in the threshold switching probably owing to the formation
of oxygen vacancies. The above results have also been observed in some
other Mott two-terminal devices with the similar variations of the Vth
and Vhold, such as the VO2-based heterostructures [6].
Since the resistive switching behaviors strongly depend on the
voltage polarity, the I–V characteristic curves of the device under the
reverse voltage were measured as shown in Fig. 4(a). It is interesting that
the nonvolatile unipolar switching is observed by changing the voltage
polarity and magnitude. Initially, the HRS (OFF state) maintains under
the reverse voltage. Subsequently, the current increases sharply
accompanied with the device turning back to the LRS (ON state) at a
certain voltage (defined as the set voltage, Vset) and quickly reaches the
compliance level. Herein the compliance current was used to avoid the

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Y. Yin et al.
dielectric breakdown of the LMO film layer. Then the bias voltage re­
duces to the origin and the LRS nearly maintains, implying a nonvolatile
switching under the reverse voltage switching. As decreasing the nega­
tive maximum voltage [See the definition in inset of Fig. 4(a)], the LRS is
initially achieved and then switched to the HRS (OFF state) at a certain
voltage (defined as the reset voltage Vreset), which is much lower than
Vset. The statistical distribution and the corresponding Lorentz fitting
results of the Vset and Vreset are demonstrated in Fig. 4(b). The Vset and
Vreset are determined to be − 7.46 ± 3.26 V and − 2.65 ± 1.85 V,
respectively. The corresponding electric field in the order of magnitude
~105 V cm− 1 is prominently lower than that of the Ni/NiO core-shell
heterostructure (106 V cm− 1) [2]. Hence the device in this work seems
more applicable in reducing the energy consumption in memory de­
vices. Due to numerous kinds of defects including impurities, vacancies,
dislocations, and grain boundaries, large fluctuations in the switching
parameters become inevitable in all resistive switching phenomena.
Thus, the broad distributions of Vset and Vreset in the present work can be
attributed to irregular and random formation and clustering processes of
oxygen vacancies [24]. Indeed, the major technical obstacle of the
actual commercialization of unipolar RRAM is the large shifts of
switching voltages. When the distributions were too large, there will be
an overlap between Vreset and Vset, leading to a switching failure for
memory devices. In the present work, there is a small operation window
between Vreset and Vset.
Fig. 4(c) presents the cumulative distributions of the Vset and Vreset,
in which a slightly wider distribution could be observed compared with
that in the Ni/NiO core-shell heterostructure [2]. The discrepancy could
be attributed to the more measurement cycles (over 500) in this test,
while there is only about 25 cycles in that work [2]. The resistance
values of the HRS and LRS are obtained as ~104 Ω and 60 Ω, respectively
as shown in Fig. 4(d). Consequently, the ROFF/RON is close to ~103. A
large distribution of Vset and Vreset and a relative uniform of resistance
have also been found in NiO films, which has been attributed to the
lowering of interface barrier [25]. It is mentionable that, by applying the
forward voltage again, the device recovers to reproducible volatile
threshold switching. Remarkably, it exhibits a stable threshold switch­
ing over ~1000 cycles and unipolar memory switching over ~500 cycles
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Current Applied Physics 31 (2021) 22–28
Fig. 4. (a) 500 cycles of the nonvolatile unipolar
switching under the reverse voltage bias. The
inset of (a) shows the definition of the negative
maximum voltage and the arrows indicating the
direction of the transitions. (b) Statistical distri­
bution of the Vset and Vreset with the number of
cycles. The red and black solid lines correspond to
the Lorentz fitting curves. (c) The cumulative
distribution of the Vset and Vreset. (d) Endurance
test of the LRS and HRS obtained with a reading
voltage of − 0.3 V. (For interpretation of the ref­
erences to colour in this figure legend, the reader
is referred to the Web version of this article.)
on the one device, implying a better endurance than that in the VO2- and
TaOx-based resistive devices under the coexistence of the nonvolatile
and volatile switching [26,27].
In order to investigate the mechanism of the above switching be­
haviors, the chemical environment of elements in the LMO film were
detected by XPS. The XPS spectra of La 3d, O 1s, Mn 2p and Mn 3s are
demonstrated in Fig. 5(a)-(d), respectively, wherein the energies are
calibrated with C 1s peak (284.80 eV). According to Fig. 5(a), the peaks
of La 3d5/2 and La 3d3/2 are fitted at 834.96 eV and 851.76 eV, with
corresponding satellite features locating at 838.44 eV and 855.21 eV,
respectively. From the above analysis, the spin-orbital splitting energy of
La 3d is 16.80 eV, implying the presence of La3+ ions [28]. In Fig. 5(b), a
doublet characteristic of O 1s are observed at 529.60 eV and 531.70 eV,
respectively. The former could be attributed to the lattice oxygen in
LMO film, while the latter is related to the oxygen vacancies. In Fig. 5(c),
the Mn 2p doublet and the corresponding shake-up satellite indicate the
coexistence of Mn3+ and Mn2+ oxidation states [28]. Furthermore, Fig. 5
(d) shows the fitting data of the Mn 3s doublet, with the level splitting
(△E3s) of 5.58 eV. Hence the Mn valence is calculated to be 2.58 by
utilizing the linear equation vMn = 9.67–1.27△E3s/eV, which solidly
confirms the mixed Mn2+/3+ state in LMO film [28].
As mentioned in the previous context, the LMO thin film was fabri­
cated and annealed under a low oxygen pressure (5 × 10− 4 Pa), which
inevitably inducing a large amount of oxygen vacancies, as confirmed by
the aforementioned XPS result of the O 1s signal. The presence of oxygen
vacancies well explains the initial low resistance state in our device.
Since the oxygen-deficient LMO is generally considered as an n-type
semiconductor, the oxygen vacancies act as donors in oxides and
become positively charged after releasing electrons to the conduction
band [19,29]. Meanwhile, the rectification characteristics of positive
HRS suggests that the top Pt/LMO interface is responsible for the
resistance switching. Furthermore, the interface of the bottom electrode
and LMO thin film could be regarded as an Ohmic-like contact owing to
the inevitable leakage in a larger area. And the top electrode interface
could be treated as a Schottky-like contact due to the very small contact
area through shadow mask.
Fig. 6(a) shows the schematic band structure of the HRS of Pt/LMO/
Y. Yin et al. Current Applied Physics 31 (2021) 22–28

Fig. 5. The XPS spectra of (a) La 3d, (b) O 1s, (c) Mn 2p and (d) Mn 3s for the LMO/Pt/Ti/SiO2/Si thin film, respectively.

Fig. 6. The schematic energy band structure

for the initial HRS under a forward bias (a)
and LRS under a reverse bias (d), respec­
tively. The “circled plus” symbols represent
the ionized oxygen vacancies and the dark
arrows show the drifting direction of the
ionized oxygen vacancies. (b) and (c) show
the schematic mechanism of the volatile
threshold switching. The irregularly shaped
black pieces show the metallic domains and
the light blue area represents the insulating
domains. (e) and (f) show the schematic
mechanism of the nonvolatile unipolar
switching. The “hollow circle” symbols
represent the oxygen vacancies. The thick
orange and black lines represent the top and
bottom Pt electrode, respectively. The “plus”
and “minus” symbols represent the positive
and negative polarity of the bias voltage,
respectively. (For interpretation of the ref­
erences to colour in this figure legend, the
reader is referred to the Web version of this
article.)

Pt after applying a forward bias. Under a positive bias, the oxygen va­ formation of Schottky contact [19]. This scenario could be confirmed by
cancies drift away from the top electrode interface, which results in a the fitting curve (red) of the HRS as shown in Fig. 2(b), which indicates
wider and higher barrier at the top Pt/LMO interface, leading to the Schottky emission conduction mechanism [30]. Meanwhile, the oxygen

26
Y. Yin et al.
vacancies drift from the top Pt/LMO interface to the bulk LMO thin film.
Consequently, the charge disproportionation effect of the Mn3+→Mn2+
in the oxygen-deficient LMO thin film must be enhanced, resulting in an
increase of Mn2+ concentration [31,32]. Then the double exchange (DE)
effect occurs in Mn2+-O-Mn3+ in the electron-doped LMO thin films, as
similar as in the case of Mn3+-O-Mn4+ in the hole-doped manganites
[31,33]. Thus the ferromagnetic metal phase domains randomly
distribute in the charge ordered antiferromagnetic insulator phase do­
mains in the LMO thin film as shown in Fig. 6(b) and (c). Accordingly,
the observed HRS in the positive voltage cycle might have relationship
with the strong antiferromagnetic insulating background in the
electron-doped LMO thin films to the device [34]. As further increasing
the magnitude of the positive voltage, a percolation-type transition be­
tween the antiferromagnetic insulating phase and ferromagnetic
metallic phase domains should happen [35], leading to the formation
conducting filament as schematically shown in Fig. 6(c). Therefore, the
insulator-to-metal transition occurs, and the device exhibits the char­
acteristics of the volatile threshold switching as also reported in the
VO2-based memristor [6].
When changing the polarity of the bias voltage, the schematic band
structure of the device is shown in Fig. 6(d). Under a negative bias, the
oxygen vacancies drift toward the top electrode interface, leading to a
decrease in the height and width of the Schottky barrier. Simulta­
neously, the concentration of oxygen vacancies in bulk LMO film re­
duces and finally results in the disappearance of the ferromagnetic
metallic phase domains. The oxygen vacancies may migrate in the bulk
LMO thin film under the negative voltage bias. As a consequence, the
oxygen vacancies conducting filaments should be emergent and
responsible for the nonvolatile unipolar switching [36], which is further
verified by the linear fitting relationship with log-log scale I–V curve for
the LRS (not shown here). The conducting filaments of oxygen vacancies
between the top and bottom electrodes are shown in Fig. 6(e) and (f) for
the ON and OFF states, respectively. As further increasing the magnitude
of the negative voltage bias, the conductive filaments induced by the
oxygen vacancies are fused down with the help of Joule heating, and
thus the device switches from the low resistance state to the high
resistance state.
4. Conclusions
In summary, the coexistence of the nonvolatile unipolar memory and
volatile threshold resistance switching was observed in the Pt/LMO/Pt/
Ti/SiO2/Si heterostructures, which depends on the bias polarity. The
voltage polarity affects the migration direction/distribution of oxygen
vacancies and the width/height of the top interface barrier, resulting in
a transition between nonvolatile unipolar switching and volatile
threshold switching. The simultaneously nonvolatile and volatile oper­
ation modes may integrate the storage and computing functionalities in
one memristor. In addition, owing to the excellent endurance behavior,
the Pt/LMO/Pt device proposed in this work is expected to be applied in
in-memory computing technology and accelerate the development of
post-Moore industry.
Author contribution
Yanfeng Yin: Conceptualization, Investigation, Writing - Original
Draft. Chaoyang Kang: Formal analysis. Caihong Jia: Methodology,
Writing - Review & Editing, Funding acquisition. Weifeng Zhang:
Writing - Review & Editing, Supervision, Funding acquisition.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
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Current Applied Physics 31 (2021) 22–28
Acknowledgements
This work was supported by the National Science Foundation of
China (11974099), Intelligence Introduction Plan of Henan Province in
2021 (CXJD2021008), Plan for Leading Talent of Fundamental Research
of the Central China in 2020, Natural Science Foundation of Henan
Province (202300410090) and Key Scientific Research Projects of
Henan Province (21A140005).
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