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Multi-factor-controlled ReRAM devices and

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their applications
Cite this: J. Mater. Chem. C, 2022,
10, 8895
Bai Sun, †*ab Guangdong Zhou, †c Tian Yu, d
Yuanzheng Chen, a

Feng Yangb and Yong Zhao*ab

Received 16th December 2021,
Accepted 16th May 2022
DOI: 10.1039/d1tc06005h
rsc.li/materials-c
Resistive random access memory (ReRAM) based on a resistive switching (RS) effect is a new type of
non-volatile memory device that stores information based on the reversible conversion of resistance
states controlled by an electrical pulse. The RRAM has many advantages such as high read/write speed,
high storage density, and low power consumption. In particular, many recent studies have found that
the conversion of resistance states in some RRAMs can be controlled by extra factors except electrical
pulses, such as light, magnetic field, mechanical force, moisture, temperature, acid-base (pH), and so on.
The multi-factor-controlled ReRAM devices are expected to be used in the manufacture of multistate
memory for information processing, special sensors and neuromorphic applications; thus, it can be
expected to be used in multifunctional devices with wider applications. Therefore, the development
of multi-factor-controlled ReRAM devices is of great significance. In this review we discuss the
research progress, current problems, and future development trends for the multi-factor-controlled
ReRAM devices for information processing, neural sensing and neuromorphic applications in artificial
intelligence.

1. Introduction
a
School of Physical Science and Technology, Key Laboratory of Advanced
Technology of Materials (Ministry of Education of China), Southwest Jiaotong The advancement of nanodevice manufacturing technology has
University, Chengdu, Sichuan 610031, China. E-mail: bsun@swjtu.edu.cn, greatly promoted the development of information technology.
yzhao@swjtu.edu.cn Traditional memory devices are facing huge challenges because
b
Superconductivity and New Energy R&D Center, Southwest Jiaotong University,
traditional memory technologies are about to reach the physi-
Chengdu, Sichuan 610031, China
c
School of Artificial Intelligence, Southwest University, Chongqing 400715, China cal limit of their storage.1,2 In particular, the von Neumann
d
College of Physics, Sichuan University, Chengdu 610065, China bottleneck caused by the central processing unit (CPU) and
† These authors equally contributed to this work.

Dr Bai Sun received his PhD degree
in the Faculty of Materials and
Energy from Southwest University
(China) in 2015, and conducted
postdoctoral research at the Uni-
versity of Waterloo (Canada) from
2018 to 2021. Currently, he is an
associate professor at Southwest
Jiaotong University. His research
interests mainly focus on the
development of new energy
materials, the preparation of
Bai Sun memristive devices and their
applications in brain-like chips,
neural synapses, neural networks, neuromorphic computing,
information sensing, intelligent electronic skin, etc.
Dr Guangdong Zhou received his
PhD degree at the Faculty of
Materials and Energy from
Southwest University (China) in
2018. He conducted his post-
doctoral research at Southwest
University during 2018–2020. His
research focuses on the physical
mechanism of memristor and
memristor-based functions includ-
ing memory logics, displays and
synapses. His memristor related
Guangdong Zhou researches are supported by the
Postdoctoral Program for
Innovative Talent Support of Chongqing. During the past 10 years,
more than 90 peer-reviewed papers were published.

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data storage unit is an important factor for the limitation of
further increase of storage density and processing speed.3–5
Therefore, the development of new types of memory devices is
extremely important for high-tech daily life. In various new
concept memory devices, the ReRAM devices based on RS
effects, such as memristors, phase change memories (PCM)
and spin torque memories (STM), have many obvious advan-
tages among all competitors for high-performance memory,
logical function, neural networks, neuromorphic computing,
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and so on.6–10 These advanced operations are expected to
promote the vigorous development of artificial intelligence.
ReRAM devices have received extensive attention due to
their fascinating potential applications spanning informa-
tion science, materials science, physics, chemistry and
biomedicine.11 This technology can perform reversible RS
between the high resistance state (HRS) and the low resistance
Dr Yuanzheng Chen received his
PhD degree at the State Key Lab
of Superhard Materials of Jilin
University (China) in 2014. And
then he joined Southwest
Jiaotong University (China) as
an associate professor. Recently,
he moved to the Beijing
Computational Science Research
Center for postdoctoral research,
and to the National University of
Singapore as a visiting scholar.
Yuanzheng Chen His research focuses on
functional device design and the
discovery of new chemical and physical properties using density
functional theory (DFT) calculations.
Dr Feng Yang received his
Master’s degree in Physics and
Chemistry of Materials from
Yanshan University in 2005
(China). He then joined the
Department of Polymer Science
& Engineering & State Key
Laboratory of Silicon Materials
at Zhejiang University and
completed his PhD degree in
2008. Afterwards, he became a
lecturer (2008–2011) and associ-
Feng Yang ate professor (since 2011) at
Southwest Jiaotong University.
His current research interests include the surface photovoltage,
photoelectronic, memristor, and resistive switching properties of
metal oxide nanomaterials.
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state (LRS), which is usually defined as logic ‘‘0’’ and ‘‘1’’ in logic
function and data storage applications. Traditionally, these two
states can be controlled by applying a sufficiently large electrical
pulse on the two electrodes of the device with a sandwich
structure.12,13 In many previous studies, the significant RS beha-
vior has been observed in many oxide materials, such as NiO,
ZnO, TiO2, ZrO2, Al2O3, Nb2O5, Ta2O5, Fe3O4, Zn2SnO4, SrZrO3,
BiFeO3, SrTiO3, Pr0.7Ca0.3MnO3, etc.14–20 In addition, it has also
been found that many biomaterials also have a resistance con-
version effect comparable to that of oxide materials.21–25 These
studies imply that the materials used to fabricate ReRAM devices
have the advantage of wide selection. In fact, the diversity of
materials for device preparation also implies the complexity of its
physical mechanism and the wide range of applications.
In many current reports, it is considered that ReRAM devices
have potential applications in multistate memory. Thus, it can
significantly improve the storage density and read/write speed
of the memory devices.26–30 Unlike other memory devices,
except electrical pulse control, the RS effect of some special
materials can also be controlled by extra-factors, such as light-
illumination, magnetic field, mechanical force, moisture, tem-
perature, acid-base (pH), and so on.31–47 It can be seen from
Table 1 that light and moisture are currently the two most
popular control methods because light and moisture are easily
implemented. The RS behavior controlled by multiple factors
greatly enriches the physical process of the RS phenomenon.
Therefore, these multi-mode response ReRAM devices are
attracting more and more interest for advanced applications,
for performing some tasks such as in sensors and detectors, not
just as memory devices for information processing.
For information storage applications, the ReRAM devices
controlled by the multi-factors provide the basis for the pre-
paration of multistate memories, which not only open the way
towards ultra-high storage density memory devices, but also lay
a theoretical basis for a device integrating multiple physical
Dr Yong Zhao is currently a
Professor of Physics at Fujian
Normal University, and a Chair
Professor at Southwest Jiaotong
University (SWJTU). He received
his PhD degree from the
University of Science and
Technology of China in 1988.
During 1988-1990, he was a
lecturer and an associate
professor at the School of
Physics at Zhejiang University.
Yong Zhao During 1992-2003, he is a
Senior Researcher Fellow,
Research Professor at the University of New South Wales. Since
2003, he has been a Chair Professor and Director of
Superconductivity R&D center at SWJTU. He has been working in
the field of superconductivity and functional devices for the last
40 years.
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Table 1 Some extra-factor-controlled ReRAM devices and their potential applications

Functional layer Top electrode Bottom electrode Extra-factors Potential applications Ref.
Al2O3 Pd SiO2/Si Light Complex memory architectures 31
ZnO nanorod Au ITO Light Information storage devices with optical writing 32
CeO2 x ITO AlOy/Al Light Non-volatile optoelectronic memory devices 33
rr-P3HT/PCBM Ag ITO Light Non-volatile memory and image detector 34
ZnO rods Ag FTO UV light Multilevel memory device 35
BiFeO3/ZnO Ag FTO Light Multifunctional electronic devices 36
Zn0.95Co0.05O Pt Pt Magnetism Random access memories with encoded quaternary information 37
BiFeO3/g-Fe2O3 Ag FTO Magnetism and light Multistate memory controlled by light and magnetism 38
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SrTiO3 d Pt Pt Moisture High-performance anionic–electronic resistive switching 39

TiOx Ag FTO Moisture Multilevel resistive switching memory 40
MoOx Ag Ag Moisture Bifunction device with logic gate and display 41
a-Carbon Ag Ag Moisture Self-powered memory system 42
Pt nanogap Pt Pt Temperature High-temperature memory device 43
C15H11O6 Ag FTO Moisture and temperature Green multifunctional electronic device 44
GeS2 Ag W Mechanical stress Stress-aware programming device 45
NiO/ZnO GaIn ITO Bending Bending-controlled resistive switching device 46
(C7H7O4N)n Ag FTO pH pH-controlled resistive switching device 47

rr-P3HT: regio-regular poly(3-hexylthiophen-2,5-diyl); PCBM: phenyl-C61-butyric acid methylester.

realize a multistate memory pattern to improve the storage

Fig. 1 Some ReRAM devices can be controlled by multi-factors.
performances for artificial sensing applications. Therefore, the
research on ReRAM devices controlled by multi-factors is very
imperative for practical application. In this review, we will
discuss in detail the research progress on the preparation of
ReRAM devices controlled by multi-factors. Although the clas-
sification may not be accurate and strict enough, in order to
give a clearer discussion, we tried to make a classification, as
shown in Fig. 1. Then, the current problems are thrown out and
some suggestions for improvement are given. Finally, the
development trends in future research are outlined.
2. Research progress
2.1 Light-controlled ReRAM devices
Recently, light plus electric pulse-controlled RS memory beha-
viors have been reported in many works, which is expected to
capacity of ReRAM devices.31–36 The light-control mode can
also be useful for long-distance applications and enables
operation without electronic disruption interference.48–50 In
this way, the operation of involving optical signals in ReRAM
devices should have potential application prospects. In addi-
tion, the photoelectric RS property can also be beneficial for the
preparation of multifunctional electronic devices, such as
photoelectric sensors and photodetectors.51,52 If the wavelength
and frequency of light are taken into consideration, light-
controlled ReRAM devices will further present more application
perspectives.
For the study of introducing optical signals into ReRAM
devices, Mariana Ungureanu et al. firstly demonstrated a light-
controlled RS memory in a Pd/Al2O3/SiO2/Si structure.31 By
testing the RS effect under light-illumination, it was found that
the resistance states of the device can be simultaneously
controlled both by voltage pulse and light. This device can
add the light as a new control pattern which is different from
the traditional RS memory device controlled by only an elec-
trical pulse. Fig. 2a shows the as-prepared ReRAM device with
the vertical stacks of a Pd/Al2O3/SiO2/Si multilayer structure.
This ReRAM device can be made to have different exposure
areas by an etching method. During the measurement of I–V
curves for two devices with different light-exposed ring areas at
room temperature, an interesting phenomenon can be
observed in that the current increase of the device became
more significant when the device with a larger area was exposed
under light-illumination. Fig. 2b clearly shows the mechanism
dynamic process of carrier movement when the device with a
light-exposed area (AL) of 1.0 cm2 was irradiated. According to
the theory of solid physics, the carrier concentration in the
depletion region of the interface can be changed by light-
illumination. For an RS memory device, it allows a light to
control the writing process of information. It implies that this
ReRAM device is expected to be developed as a light-assisted
multistate memory. Besides, the light-controlled ReRAM device

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Fig. 2 (a) Schematic diagram of the as-prepared ReRAM device with a Pd/Al2O3/SiO2/Si structure; (b) the dynamic process of a light-controlled ReRAM
device. Panels a and b were reproduced with permission.31 Copyright 2012 Wiley-VCH. (c) Schematic diagram of the light-controlled new concept logic
devices. Panel c was reproduced with permission.32 Copyright 2013 Wiley-VCH. (d) Schematic diagram and operation mechanism of the light-controlled
ITO/CeO2 x/AlOy/Al device. Panel d was reproduced with permission.33 Copyright 2015 Wiley-VCH.
has the capability to work as a light sensor and light-electric
signal detector,53,54 a combination that opens the door to novel
multifunctional devices.
In the research of photoelectric devices, ZnO is an important
member of semiconductor materials. ZnO is usually an n-type
semiconductor with four crystal structures, namely the wurtzite
phase, sphalerite phase, NaCl structure, and CsCl structure,
respectively. ZnO has a large energy band gap and exciton
binding energy, high transparency, and excellent luminescence
performance at room temperature. Therefore, it has been
usually used in the research of many optoelectronic devices.
Here it should be mentioned that Jinjoo Park et al. designed a
new conceptual method for controlling memristors based on
ZnO nanorods.32 The schematic diagram of the light-controlled
new concept logic devices is illustrated in Fig. 2c. By adjusting
the angle of light incidence on the device, it can be found
that the obtained signal can be switched reversibly between
the memristor and the resistor. This reversible switching
device between memristor and resistor has many interesting
potential applications.55,56 The inset of Fig. 2c shows a three-
dimensional (3D) cross-sectional view of different regions of a
memristor and resistor. This novel design concept is widely
applicable in many light-controlled multifunctional devices.
When the light radiation incident at y = 601 irradiated the
device, the device showed no significant memristive effect. This
is in stark contrast to when the device exhibits bipolar RS
characteristics when the light incident on the sample at an
angle of y = 101 with respect to the normal irradiates the device
array. Thus, the structure and design methods of the as-
described device can stimulate future technological develop-
ment of nanodevices, such as the development of manufactur-
ing information memory devices that perform optical writing
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under constant sunlight and photoelectric sensors. Further-
more, Hongwei Tan et al. reported the design and construc-
tion of an optoelectronic RS memory device with integrated
demodulating and arithmetic functions for information
technology.33 The as-prepared ReRAM device is composed of
a simple ITO/CeO2 x/AlOy/Al multilayer structure (Fig. 2d). In
this work, an electrically erasable persistent photoresponse
characteristic in the as-prepared memristive device can be
observed. The first-digit information can be transmitted and
demodulated from the wavelength of the light beam. The green
light with a wavelength of 560 nm and the blue light with a
wavelength of 499 nm can be demodulated as ‘‘0’’ and ‘‘1’’,
respectively. At the same time, the second-digit binary informa-
tion can be carried and demodulated with the intensity of the
light beam, where 4 and 6 pW mm 2 for either colored light
stand for ‘‘0’’ and ‘‘1’’, respectively. Thus, the four pieces of two-
digit information of ‘‘00’’, ‘‘01’’, ‘‘10’’, and ‘‘11’’ can be demo-
dulated and stored from the wavelength and intensity of
the incident light beams, with the corresponding device resis-
tances of B1.5  1010, 9.0  109, 4.3  109, and 1.7  109 O
in response to the optical beams of green light with lower
intensity (GL), green light with higher intensity (GH), blue
light with lower intensity (BL) and blue light with higher
intensity (BH), respectively. Finally, the word ‘‘NIMTE’’ can be
demodulated from the light signals by and stored in the ITO/
CeO2 x/AlOy/Al device. This work demonstrates the possibility
of using a photoresponsive ReRAM device for future high-
performance information storage, computing and communica-
tion applications.57–59
At present, it is undeniable that the selection of suitable
functional materials is still a challenge in order to achieve high-
performance photo-electronic ReRAM devices.60–62 Sebastian
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Fig. 3 (a) Microscope photo of a 32  32 array detector. (b) A schematic cross-sectional view of a single unit of the ReRAM device, showing the materials
used in each component. (c) Optical photograph of the fabricated image detector array on the flexible substrate. (d) The I–V curve of the organic
photodiode under dark conditions and using different power illumination. (e) The I–V curve (red line) of the organic photodiode under dark conditions
and the hysteresis I–V curve (blue line) of the organic ReRAM device on top of the organic photodiode. Panels a–e reproduced with permission.34
Copyright 2015 Wiley-VCH.
Nau et al. introduced a unique imaging device concept using an
organic and flexible detector array with simple passive matrix
wiring.34 The appropriate functionality of this concept was
demonstrated in single elements and an array structure with
32  32 cells, which was integrated into an organic and flexible
passive-matrix image detector array (Fig. 3a). As illustrated in
Fig. 3b, a single pixel of the as-presented image detector, which
is comprised of a vertical stack of an organic photodiode and an
organic non-volatile multibit ReRAM device. As an organic
photodiode, a well-known system based on a photoactive layer
consisting of a blend of regio-regular poly(3-hexylthiophen-2,5-
diyl) (rr-P3HT) and phenyl-C61-butyric acid methylester (PCBM)
was used to form a p–n bulk-heterojunction in the interface
between the two electrodes. Fig. 3c shows an optical photo-
graph of a high-density array of image detectors fabricated on a
flexible substrate, indicating that the as-fabricated ReRAM
device has good flexibility and can be bent under a small
clamping force between the fingers. The detection mechanism
of a single pixel using the device is that the illumination using
the organic photodiode will cause the voltage drop across the
two devices to be redistributed. This can be used to trigger a
threshold event, which causes the non-volatile resistance
changes of the organic ReRAM device to change. A typical I–V
curve of the organic photodiode at different illumination con-
ditions is shown in Fig. 3d. The current of the device shows an
obvious gradual increase trend with the increase of the light
power density in the negative voltage region. The I–V curves of
the vertically stacked combination of both devices are shown in
Fig. 3e and can be described as follows: Initially the organic
ReRAM device is at the HRS. When the I–V sweep was started at
–6.0 V and then the bias was decreased to 0 V, it detected only
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the reverse current of the diode. In the forward direction (0 V -
6.0 V - 0 V), the photodiode is conductive and does not act as a
current-bottleneck for the organic ReRAM device. A typical
hysteretic I–V characteristic with an obvious RS effect can be
clearly observed in this organic device. When the applied
voltage was scanned back to 6.0 V again, the ReRAM device
exhibited a very obvious low reverse current. Although the
organic ReRAM device had switched to its LRS, the current still
did not increase significantly. This work proposed a unique
image detection array technology based on an organic ReRAM
device. Since organic materials usually have the advantages of
good scalability, flexibility, bendability, and light weight, com-
pared with traditional inorganic image detector technology,
this organic device technology has many applications, espe-
cially in wearable electronics.63–65
With the development of light-controlled ReRAM devices,
the wavelength of light has also become a factor worth con-
sidering. For example, the ultraviolet (UV) light-controlled RS
behavior has attracted the attention of researchers.66–69 It
should be mentioned that Paola Russo et al. reported, for the
first time, the multilevel current amplification of ReRAM
devices induced by UV light illumination based on ZnO
rods.35 In this work, in order to study the electrical perfor-
mances of the ZnO rod-based ReRAM device, Ag as the top
electrode and FTO as the bottom electrode of the ReRAM device
were fabricated. A schematic of the Ag/ZnO rods/FTO device is
displayed in the insets of Fig. 4a and b. The electrical measure-
ments were performed in the dark and under UV irradiation.
Considering that the nanorod array usually has an obvious
leakage current, a relatively small applied voltage was used for
the ZnO rod-based ReRAM device. A sweeping voltage of 4.0 V
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Fig. 4 (a) I–V curves of the ReRAM device with a Ag/ZnO rods/FTO structure under dark conditions and (b) under UV irradiation with a sweeping voltage
of 4.0 V for the first cycle (black curves) and after 40 cycles (red curves). (c and d) UV photoresponse time of the as-prepared ReRAM device in the
constant positive voltage region and negative voltage region, respectively. Panels a–d were reproduced with permission.35 Copyright 2018 Wiley-VCH.
was applied at the top electrode Ag, and the bottom electrode
FTO was kept grounded. The I–V curves are displayed in Fig. 4a
and b, respectively, in which it can be observed that the current
of the device is increased by nearly an order of magnitude when
UV irradiation was applied to the ReRAM device. The photo-
response performances of the ReRAM device under positive and
negative voltage are shown in Fig. 4c and d, in which we can see
that UV light has a very significant modulation effect on the
output current of the Ag/ZnO rods/FTO device. Therefore, a
conclusion can be drawn from this work that the UV-induced
multilevel current amplification can be employed for the opti-
mization of the devices’ performance by controlling the UV
exposure. This work provides a good valuable reference for the
preparation of UV-controlled ReRAM devices, UV-response
field-effect transistors (FET), real-time UV detectors, and so
on.70–72
In our previous work, a light-induced negative differential
resistance (NDR) effect in a ReRAM device with a Ag/BiFeO3/
ZnO/FTO structure was observed.36 The I–V characteristics
show asymmetric behavior under dark and light-illumination
conditions, respectively. We can observe that an NDR effect
occurs when the device was exposed to light-illumination
conditions. Based on conductivity analysis, the physical
mechanisms of the RS and NDR effect for the Ag/BiFeO3/ZnO/
FTO device were proposed. Based on the energy band structure
and electron–hole pair separation in the p–n heterojunction, it
is well known that the BiFeO3 film is a typical p-type semicon-
ductor due to the formation of oxygen vacancies during the
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preparation process, while the ZnO film is a stable n-type
semiconductor. Therefore, a p–n junction would be formed at
the interface of this heterojunction. At this time, the holes in
BiFeO3 can be diffused into ZnO, and the electrons in ZnO can
be diffused into BiFeO3. Thus, an internal electric field would
be formed inside the p-n junction, and the direction of the
internal electric field is directed from ZnO to BiFeO3. When the
device was exposed to light-illumination, it further strengthens
the internal electric field because a large number of photo-
generated carriers was generated inside BiFeO3 and ZnO,
resulting in an obvious NDR phenomenon being presented.
Therefore, the formation of this internal electric field leads to
the appearance of the NDR effect. Through the above analysis,
the RS memory behavior can be attributed to the formation of
oxygen vacancies assisted Ag conductive filaments, while the
NDR effect can be attributed to the inner electric field and the
efficiently separated photo-generated electrons and holes
under light-irradiation in the interface of the BiFeO3/ZnO p–n
heterojunctions. This work opens up a new way to design a new
type of electronic device which can be conversed between RS
memory and NDR effect by using light-illumination. Indeed,
many works report that the NDR effect has very important
potential applications in electronics.73–77 Therefore, it is
expected that the light-induced coexistence of the RS and
NDR effect has highly important potential applications in the
photo-electric multifunctional electronic devices.
In short, through the above discussion of the light-controlled
ReRAM devices, it can be seen that the light-controlled RS
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memory behavior shows an increasingly important duo as it
provides a reliable basis for the development of multistate mem-
ory using light as an additional control parameter. In particular,
the light-controlled RS behavior can also be applied to other
functional electronic devices, such as light sensors, light-
controlled field effect transistors (FET), light image detectors,
light-controlled synaptic devices, light-controlled neural networks,
photo-rechargeable battery, and so on.78–82 Therefore, the devel-
opment of light-controlled ReRAM devices will have broad
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Guang Chen et al. firstly fabricated a RS device with a Pt/
(Zn0.95Co0.05)O/Pt sandwich structure on the SiO2/Si substrate
with Ti as the buffer layer.37 In the RS device, a (Zn0.95Co0.05)O
film with a thickness of 60 nm acts as the functional layer of the
device, and Pt acts as the top and bottom electrodes. The inset
of Fig. 5a shows a schematic diagram of the 3D structure of the
RS device and the test circuit. To demonstrate the effect of RS
behavior on the magnetic properties of Co:ZnO, Fig. 5a shows
the magnetization hysteresis loop of the as-prepared Pt/

potential application prospects for multifunctional electronic
devices in the future.
2.2 Magnetism-controlled ReRAM devices
It is well known that magnetic phenomena and electrical
phenomena are essentially related. The electrical applications
of devices are usually significantly affected by a magnetic field
because the magnetic properties of materials are closely related
to the movement structure of electrons. Recently, magnetism
controlled electronic devices have also been a very popular
research field because the magnetic field is not blocked by
obstructing objects.83–85 In particular, the application of mag-
netic field-controlled devices is even more widely used in
biomedicine.86,87 Therefore the magnetic field as a very effec-
tive control method has also been used in ReRAM devices in
recent years of research.37,38
Co:ZnO/Pt device, in which the magnetic field (H) was applied
in-plane, and the diamagnetic signal of the substrates was
subtracted by testing a clean substrate. Fig. 5b shows I–V curves
with 30 consecutive cycles for one of the memory cells with a
stable RS characteristic along with a clear set and reset process,
indicating a bipolar RS behavior was obtained from the as-
prepared samples. The inset of Fig. 5b presents the endurance
properties of the RS device, which shows that the Pt/Co:ZnO/Pt
device can continuously switch exceeds 300 cycles with slight
attenuation. This data shows that the RS device has the
capability of being an information storage device. Reversible
control of saturation magnetization (MS) in a sequence of more
HRS/LRS cycles is presented in Fig. 5c. In addition to the MS
modification, the coercivity (HC) was also modulated reversibly
between 68  3 and 94  4 Oe with the RS behavior, which
shows a robust and stable variation of 35% accordingly, as

Fig. 5 (a) The magnetization hysteresis loop of the as-prepared RS device with a Pt/Zn0.95Co0.05O/Pt structure at room temperature when the sample
plane is parallel to the direction of the magnetic field. (b) The semilogarithmic I–V curves with 30 cycles for the RS device. (c and d) The MS and HC are
reversibly modulated by the RS effect of the device. (e) Schematic of ferromagnetic ordering based on the bound magnetic polarons (BMP) mechanism at
HRS. (f) Mechanism of the RS and magnetic modulation during the set process. All panels were reproduced with permission.37 Copyright 2012 Wiley-
VCH.

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depicted in Fig. 5d. Hence the initial ferromagnetism of the device
at HRS is naturally explained by the bound magnetic polarons
(BMPs) mechanism (Fig. 5e), in which it is discounted in this
scenario for a lack of enough oxygen vacancy (VO) in the insulating
Co:ZnO composite to achieve effective coupling. During the set
process, accumulations of VO resulting from the oxygen migration
to the anode are aligned along the film growth direction to form
conductive filaments (Fig. 5f), resulting in the RS device entering
the LRS or ‘‘ON’’ state from HRS or ‘‘OFF’’ state. Therefore, the Pt/
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the magnetic field controlled RS behavior. Obviously, the
magnetic field can effectively control the set and reset voltage
of the RS device. In addition, this device is also controlled by
light-illumination (the related data is not shown here). The
physical mechanism of the magnetic field and white-light
controlled RS behavior of the Ag/[BiFeO3/g-Fe2O3]/FTO device
is displayed in Fig. 6c. It should be noted that the ferroelectric
polarization of the BiFeO3 nanoparticle and the magnetization
of the g-Fe2O3 nanoparticle are the key roles for the magnetic

Co:ZnO/Pt device achieves a reversible conversion of resistance
between HRS and LRS in the magnetic field. Therefore, the
combination of the RS and magnetic modulation gives rise to
the integration of ferromagnetism and electrical properties into
an RS device with a Pt/Co:ZnO/Pt structure, which is promising for
broadening the applications from RS behavior to magnetism
controlled multifunctional devices.88,89
Based on the above research, a magnetic field controlled
ReRAM device with a Ag/[BiFeO3/g-Fe2O3]/FTO structure was
also designed.38 Fig. 6a shows a schematic representation of
the sandwich RS device. Fig. 6b displays typical current density-
dependent voltage (J–V) curves on linear scale in various
magnetic fields from 0 T to 2.5 T, which exhibit an asymmetric
hysteresis behavior with a significant bipolar RS effect. The
inset of Fig. 6b is a schematic diagram of the test method for
field and white-light simultaneously controlled RS effect in the
BiFeO3/g-Fe2O3 heterojunction based ReRAM device. BiFeO3 is
a typical multiferroic material, thus it has both ferroelectricity
and ferromagnetism. The ferroelectric polarization of BiFeO3
results in an extra opposite-direction electrical field (Ei) in
the BiFeO3/g-Fe2O3 composite film. Light-illumination can
enhance the ferroelectricity of BiFeO3, which leads to increas-
ing the extra opposite-direction electrical field (Ei) in the
BiFeO3/g-Fe2O3 composite film. In addition, the magnetic field
can magnetize the g-Fe2O3. The J–V curve of the RS device
shows a macroscopic change because of the micro-rotation of
the magnetic domain of g-Fe2O3 and the ferroelectric domain of
BiFeO3 in the light-illumination and magnetic field. Therefore,
such an RS memory can be controlled simultaneously by
voltage pulses, magnetic field and light-illumination, which

Fig. 6 (a) A schematic representation of the magnetism-controlled ReRAM device with a Ag/[BiFeO3/g-Fe2O3]/FTO structure. (b) The linear scale J–V
characteristic curves in various magnetic fields, and the inset is the schematic diagram of the testing circuit in a magnetic field. (c) Ferroelectric
polarization of BiFeO3 under an applied voltage. By applying a magnetic field or white light, ferroelectric polarization of BiFeO3 can be increased. All
panels were reproduced with permission.38 Copyright 2015 Royal Society of Chemistry.

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reveals the potential for next-generation nonvolatile memory
applications based on a multifunctional composite material.
Based on the above discussion, it can be seen that the
magnetic field controlled RS effect is also a research focus
because the magnetic field can’t blocked by obstacles, thus the
magnetic field controlled electronic device can be effectively
used in medical diagnosis and treatment.90–92 Therefore, the
magnetic field controlled ReRAM devices should have potential
applications in advanced multifunctional electronics.
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impact on the performance and application of electronic
devices. However, the regulation of moisture on electronic
devices has become a research focus with the development of
multifunctional devices.93–95 In particular, many studies have
reported the regulation of moisture on ReRAM devices.96–102
Next, we will discuss in detail the research on moisture-
controlled ReRAM devices.
For the first time, Felix Messerschmitt et al. prepared a
ReRAM device with a Pt/SrTiO3 d/Pt structure and demon-

strated a reversible transition from standard RS behavior at

2.3 Moisture controlled ReRAM devices
With the miniaturization of integrated circuit packaging and
the development of surface mount technology, the develop-
ment of non-gas-sensitive surface mount devices has been very
rapid. Due to moisture absorption, its attenuation rate also
remains high. Therefore, moisture has always had a negative
ambient humidity to a capacitive-coupled memristive effect in a
dry atmosphere.39 Through electrochemical reaction analysis,
the RS behavior based on oxygen anionic–electronic transfer
with the bit structures in cross-plane configuration consisting
of two Pt electrodes separated by a SrTiO3 d thin film, as shown
in Fig. 7a. Several microelectrodes were structured onto the

Fig. 7 (a) Schematic representation of a single RS device with a Pt/SrTiO3 d/Pt structure exposed to moisture and performance test circuit diagram.
(b) Results of cyclic voltammetry measurements with 200 consecutive cycles at a constant sweep rate of 0.05 V s 1. (c) Schematic diagram of the
electrochemical reaction dynamics of moisture in the memristor. Panels a–c reproduced with permission.39 Copyright 2015 Wiley-VCH. (d) Schematic
diagram of the reaction of water molecules (H2O) with oxygen vacancies at the surface and interface of an RS device with a Ag/TiOx/FTO structure. (e and
f) The I–V curves of the RS device under RH of 0% and 95%. Panels d–f reproduced with permission.40 Copyright 2018 Wiley-VCH.

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sample to characterize the memristive behavior and assure
reproducibility of the RS measurements including a close-to-
application multibit cross-bar array with the thickness of the
SrTiO3 d film of about 720 nm. The RS characteristics of the
Pt/SrTiO3 d/Pt devices using cyclic voltammetry under ambi-
ent conditions are shown in Fig. 7b. We can see that this
logarithmic form I–V curve is obvious non-zero crossing, and
it can be repeated for 200 consecutive cycles, suggesting the
RS device has a good stability with information storage
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capacity. Fig. 7c shows that moisture influences the overall
electronic structure at the space-charge region of the metal/
oxide interface. The results were discussed in relation to
the changed Schottky barrier by adsorbed surface water
molecules (H2O) and its interplay with the charge transfer
in the SrTiO3 d thin film. From a fundamental perspective,
these results show that moisture cannot be neglected in
the development of an anionic–electronic RS device as hydro-
xyl interactions seem to be crucial to the basic property
of memristive devices. These new insights on moisture con-
trolling the I–V profile transition from a standard memristive
behavior to a fully capacitive-coupled memristive effect
allow us to formulate future device design guidelines to
tweak the resistance ratios and their addressable states and
to engineer high-performance anionic–electronic ReRAM
devices.
Inspired by the above research, we also designed a ReRAM
device using moisture controlling based on an Ag/TiOx/F-
doped-SnO2 (FTO) structure, and observed a coexistence of
negative differential resistance (NDR) and RS memory at room
temperature.40 It was found that the coexistence starts to
appear when the RS device was exposed to a humidity environ-
ment, and the phenomenon gradually became obvious when it
was exposed to a relatively high humidity with a relative
humidity of 35%, and then becomes dramatically enhanced
as the relative humidity becomes higher. Fig. 7d shows a
schematic diagram of a water molecule (H2O) reaction with
oxygen vacancy (Vo) at the surface of the RS device and the
interfaces of Ag/TiOx and TiOx/FTO. The I–V hysteresis can be
found in Fig. 7e and f under the bias voltage scan rate of
1.0 V s 1 with the bias voltage sweep sequence between 6.0 V
and 6.0 V. A typical RS phenomenon can be observed in the RS
device under relative humidity (RH) of 0% from Fig. 7e. How-
ever, a strong NDR appeared when the relative humidity was
improved to 95% in Fig. 7f. A strong NDR behavior was
observed in the RS memory cell under RH of 95% demonstrat-
ing a coexistence of NDR and RS. The coexistence can be
realized at room temperature using the RS device with an Ag/
TiOx/FTO structure by operating at different relative humidity
(RH) levels. This research reveals that the coexistence of NDR
and RS was greatly enhanced when RH was changed from 35%
to 95%. In contrast, there exist almost two orders smaller
saturation current and no NDR in high vacuum. Therefore,
this work demonstrates that moisture-modulated coexistence
of NDR and RS gives an insight into the influence of water
molecules (H2O) on transition-metal-oxide-based ReRAM
systems.
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In addition, our group developed an RS device with the
lateral Ag/MnOx/Ag structure based on a single MnOx nanorod
on a Si substrate with an insulating layer of SiO2.41 An inter-
esting phenomenon was observed in that the RS device showed
a typical resistor property under dry ambience, while it demon-
strated the reversion between resistor and memristor under
moisture ambience. Fig. 8a shows a schematic diagram of the
Ag/MnOx/Ag device when input electric pulses of 0.7 V were
applied under the moisture of RH = 65%, and the reading
voltage of 0.5 V was employed at the same time. It was found
that a low current of B5.0 nA was presented from the ReRAM
device even without any inputs. The current versus input signal
plot demonstrated that the output value can be well maintained
for 50 seconds when applying different inputs to the device.
Furthermore, the display logic was defined to be ‘‘1’’ when the
output current exceeds 200 nA. Thus, a pre-stored single letter
‘‘G’’ can be further presented by the codes ‘‘01000111’’ accord-
ing to the American Standard Code for Information Inter-
change (ASCII), as shown in Fig. 8b. The other letters of the
alphabet (‘‘I’’ and ‘‘T’’) can be displayed by the same pattern.
Therefore, the memory logic functions, namely, the memory
logic gates and logic displays are feasible after applying the
moisture and electric pulses to the single MnOx nanorod-based
ReRAM device.
In the past few years, Z. L. Wang and C. G. Hu have stressed
that the self-powered system, which shows the brightest pro-
spect applications in smart sense and portable microelectronic
devices.103–107 In previous reports, the moisture-powered sys-
tem has also been developed.108–110 In particular, Prof. Dai’s
group developed a moisture-powered information storage
device for the first time.111 Based on the inspiration of the
above research, flame synthesis carbon-based nanogenerators
(Carbon-NGs) were developed, which can be triggered by water
evaporation at room temperature.42 These devices show a
favorable open-circuit voltage of B1.0 V and short-circuit
current of B100 nA. The typical I–V measurements illustrate
that the device has obvious bipolar RS behavior. A resistance
ratio (RHRS/RLRS) of B8 can be obtained and well maintained
for 104 s without almost attenuation at a reading voltage of
0.5 V, indicating the ReRAM device has potential applications
in information storage. Fig. 8c shows a schematic of the self-
powered memory system including the Carbon-NGs and carbon
memristor. The output current of the carbon memristor versus
the time was tested when the Carbon-NGs cells periodically
reverse the Ag electrodes inserted into deionized water (Fig. 8d),
showing a periodic output of current and open circuit voltage
signals. Fig. 8e displays the schematic of the CS-AFM measure-
ment using the carbon materials and a constant bias voltage of
0.1 V applied to the carbon layers. These results show the
carbon-NGs system possibly has potential for application in
moisture-controlled memristive sensors. Therefore, the a-
carbon-based self-powered memory system has provided a
voltage source as well as sensing to the testing environment.
From the above analysis, it is not difficult to see that the
moisture controlled RS effect has many meaningful applica-
tions in a humid environment and under water-rich conditions.
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Fig. 8 (a) Operating schematic diagram of the memristive device under an electric pulse of 0.7 V and moisture. (b) The logic display of the word ‘‘GIT’’
according to the ACSII. Panels a and b were reproduced with permission.41 Copyright 2019 Royal Society of Chemistry. (c) Self-powered memristive
system. (d) The output current versus the time for the Carbon memristor after integrating with three Carbon-NGs cells with expected voltage outputs.
(e) Schematic of the CS-AFM measurement using the a-carbon materials. Panels c–e were reproduced with permission.42 Copyright 2019 Elsevier.
(f) Schematic diagram of the potential applications of moisture-controlled memristors.

This is mainly due to the decomposition reaction of water
molecules (H2O) inside the functional material under an exter-
nal applied voltage, and then will give rise to a chemical
reaction with oxygen vacancies or other ions in the active
material, which further caused the change of the RS effect. In
addition to ReRAM devices, the moisture controlled electronic
devices, such as moisture-powered nanogenerators, moisture-
powered detectors and moisture-powered sensors have also
been widely reported.112–116 Therefore, moisture-controlled
ReRAM devices have opened a path for the development of a
new type of electronic devices. Finally, it should be mentioned
that the memristive effect controlled by the extra-factor
has potential application value for preparing multistate
memory.44,45 In such devices, because the addition of water
(H2O) can modify the memristive properties of the device,
multiple logic states can be obtained, as shown in Fig. 8f. Thus,
it is undeniable that this moisture-controlled memristive effect
can also be used in sensors. Therefore, the proposed moisture-
regulated memristive behavior can not only be applied to
multistate storage, but also can be applied to humidity sensing,
which has potential multifunctional characteristics.
2.4 Effect of temperature on ReRAM devices
In current research, temperature has also been involved in the
research of ReRAM devices as a control parameter.43,44,117,118 In
general, temperature-controlled devices have the following
advantages: (i) since an intelligent temperature controller has
the technology of temperature control by programming in
different periods, it can realize automatic controlling of the
devices in different periods through intelligent and humanized
programming settings. (ii) The temperature of the device can be
sensed by using a highly accurate thermal element, so that the
device can be accurately controlled to operate at a certain
temperature. (iii) It can be implanted into the human body as
a medical device to detect the human body’s condition in real
time, and reflect the health or other conditions through tem-
perature. Therefore, temperature-controlled ReRAM devices
should have many potential applications in wearable products,

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Fig. 9 (a) Schematic diagram of a nanogap-based RS device and SEM images of a Pt nanowire fabricated on a SiO2/Si substrate. (b) Nanogap formation
sequence. (c) SEM image of a Pt polycrystalline nanowire with nanogaps. (d) Stability of the HRS and LRS of the sharp-edged Pt nanogap at 873 K. Panels
a–d were reproduced with permission.43 Copyright 2016 NPG publisher group.
medical diagnostic devices and temperature-controlled mem-
ristive sensors.
Hiroshi Suga et al. prepared a highly stable, nonvolatile,
high-temperature memory based on the RS effect of a poly-
crystalline platinum (Pt) nanogap by high-resolution electron
beam lithography and lift-off techniques.43 In this work, the
researchers prepared the simultaneously pattern multiple Pt
nanowires with a width of 500 nm and a length of 5 mm.
Thereby they obtained a non-volatile nanogap memory on the
Si substrate with 300 nm thick SiO2, as shown in Fig. 9a. Then,
a shaping current was applied to open the gap in the nanowire
using a probe station equipped with a source meter (Keithley
2636) (Fig. 9b), which can confirm whether the gap was
successfully formed. The SEM image of a Pt polycrystalline
nanowire with nanogaps is shown in Fig. 9c, which exhibits a
nanogap of approximately 10 nm between the Pt electrodes.
Finally, a long-term retention measurement was performed, in
which we can see that the resistances of HRS and LRS are
basically unchanged within 8 hours at 873 K (Fig. 9d). These
results indicate that the nanogap-based ReRAM device has a
stable resistance memory window, and it is suitable for the
preparation of ReRAM devices as information storage devices.
This work indicates that the nanogap-based RS device can work
at high temperature, which expands the temperature range of
the RS device works.
In order to further expand the choice of materials for the
preparation of memristors, exploring the use of natural bioma-
terials as functional layers to prepare memristive devices
has attracted the attention of many researchers. In our
previous work, a memristor device with a Ag/C15H11O6/FTO
structure was prepared using natural biomaterial anthocyanin
(C15H11O6) as the functional layer.44 The preparation process of
the device using a spin coating method is shown in Fig. 10a.
The I–V curve of the Ag/C15H11O6/FTO device from 2.0 to 2.0 V
was first measured, and an obvious nonpinched (non-zero-
crossing) I–V hysteresis characteristic at ambient conditions
(Fig. 10b1) was observed. When applying a larger voltage and
moisture, the I–V hysteresis curve changes from nonpinched
(non-zero-crossing) to pinched (zero-crossing) characteristic, as
shown in Fig. 10b2 and b3. Moreover, with increasing the
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temperature from room temperature (25 1C) to 250 1C, the
nonpinched I–V at low temperature changes into a pinched I–V
loop at high temperature (Fig. 10b4). This may be because the
ionic activity in the active material is increased due to
reinforcing thermal shock with increasing the temperature,
which makes it easier to ionize atoms and then it can be
transported more rapidly. As a result, it is easy to form ionic
conduction paths, resulting in an I–V curve with pinched
behavior. Therefore, the experimental data were obtained in
C15H11O6-based devices when the ReRAM device was subjected
to an external stimulus (e.g., voltage, moisture, or temperature),
which explains a reversible transition from a nonpinched I–V
hysteresis loop to an ideal pinched I–V hysteresis loop. This
work indicates that the natural biomaterials can also be used to
prepare temperature-controlled ReRAM devices, and it can be
expected to be applied to the production of sustainable, green
and pollution-free electronic devices.
Based on the discussion about the preparation of
temperature-controlled ReRAM devices, it can be found that
temperature-controlled ReRAM devices have a wide range of
application prospects because the temperature is an easily
controlled parameter. Especially, the temperature-controlled
ReRAM device can be applied to programmable temperature
controlled electronic devices, such as temperature-controlled
sensors, temperature-controlled detectors, temperature-
controlled medical treatment, and so on.119–125
2.5 Effect of mechanical stress on ReRAM devices
The influence of mechanical stress on device performance is
also an important aspect. For example, the strain of a ferroe-
lastic material is a nonlinear function of the mechanical stress
that it is subjected to a device. Ferroelastic materials have a
wide range of applications in materials science.126–130 Similarly,
current research indicates that the RS effect of some materials
is also regulated by mechanical stress. Next, we will discuss the
control and application of mechanical stress to the RS effect.
Stefano Ambrogio et al. showed that the asymmetry of the
migration barrier can be explained by the mechanical stress
gradient opposite to the growth of conductive filaments based
on the GeS2 functional layer, and helps to retract it during the
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Fig. 10 (a) The preparation process of a biomemristor by using natural biomaterial (C15H11O6) as the functional layer. (b) The transition between the
capacitive-coupled memristive and pure memristive effect. (b1) The initial I–V curve. (b2) Applying larger voltage. (b3) Adding moisture. (b4) Increasing
temperature. Panels a and b were reproduced with permission.44 Copyright 2019 American Chemical Society.
negative erasing process.45 Fig. 11a shows the measured I–V
curve for an RS memory device, in which the Ag works as the
top electrode, the GeS2 electrolyte as the functional layer and W
metal as the bottom electrode. The set transition from the high
resistance state (HRS) to the low resistance state (LRS) takes
place at Vset of B0.3 V, while the reset transition from LRS to
HRS occurs at Vreset of B 0.2 V. In the set process, the
conductive filament was first formed by nucleation followed
by conductive filament growth, which was activated by positive
ion migration as shown in Fig. 11b. To illustrate the impact of
stress gradient on the impurity migration in the ReRAM device,
Fig. 11c–e shows the energy potential profile for ion migration
at V = Vset (point P1 in Fig. 11f), V = VC (bias point P2) and V =
Vreset (bias point P3), respectively. After the nucleation of the
conductive filament and during its growth under an applied
voltage, the mechanical stress (hence U) can be released
through plastic relaxation, as described in Fig. 11g. This
process allows the growth of the conductive filament by plastic
relaxation of the surrounding electrolyte to be accommodated.
The results provide a new direction for improving reliability
and switching of RS memory through control of the stress
around the accommodating either through electrolyte engi-
neering or stress-aware programming schemes.
Furthermore, the effect of bending on RS behavior was
investigated by Hai-Lin Yuan and Jian-Chang Li.46 The NiO/ZnO
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nanocomposite thin films were used as the functional layer in
the ReRAM device. Fig. 12a shows the RS device was continu-
ously deformed by sinusoidal bending under the force of the
external force. Fig. 12b shows that the ON/OFF resistance ratio
of the RS device drops more than 10 times after 100 consecutive
cycles, and the distribution of threshold voltage increases
linearly with the increase of bending time, which can be
attributed to the internal conduction filament of the functional
layer being broken. In addition, it can be found that the
threshold voltage was increased with the decrease of the bend-
ing radius, and after 100 consecutive cycles, the switching
characteristics remained reduced at a bending radius of
15.2 mm, as shown Fig. 12c. Fig. 12d shows an atomic force
microscopy (AFM) image of the NiO/ZnO film fabricated on the
poly (ether sulfone) (PET) substrate. It can be observed that
the surface of the NiO film is relatively smooth compared with
the ZnO film, so this sample can be regarded as the ZnO
nanoparticles embedded into the NiO film. In addition, the
schematic illustration of the O2 transfer in the NiO/ZnO layer
(sectional view) is also shown in Fig. 12d. It is known that the
breaking position in the oxygen vacancy path is an important
feature of the RS mechanism. For this device, the cathode
interface may be localized due to the filament with a smaller
diameter on the cathode side, as shown in Fig. 12e. This
mechanical stress can effectively affect the formation and
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Fig. 11 (a) The I–V characteristic of the ReRAM device with set and reset
transitions under a positive and negative voltage region. (b) Schematic
illustration of the potential energy profile of ion migration for zero or
positive applied voltage. (c–e) Profiles of the potential energy for ion
migration within the stress field at the three bias points. (f) Schematic
illustration of the asymmetric I–V curve indicating the three bias points.
(g) Schematic representation of the change in stress gradient (hence U)
over time in response to cation migration and subsequent plastic relaxa-
tion of stress due to viscous flow. Panels a–g were reproduced with
permission.45 Copyright 2014 Wiley-VCH.
disconnection of oxygen vacancy conductive filaments. There-
fore, this study shows that the oxygen in the air can easily enter
the device functional layer through the film crack, thereby
reducing the oxygen vacancy density and weakening the con-
ductive filament in the functional layer. In short, this work may
provide some useful information for further understanding the
working mechanism of flexible ReRAM devices under bending
conditions.
Through the above analysis, we can see that the stability of
the flexible ReRAM devices under repeated bending conditions
is the key factor to achieve a practical application. Currently, in
order to improve the working stability and long-term retention
of flexible ReRAM devices, organic materials with good flexible
properties have also been involved in the research of ReRAM
devices.130–140 It is expected that this flexible ReRAM device can
be used in the field of future wearable electronics.
2.6 Effect of pH on ReRAM devices
In many previous works, the regulation of pH on the perfor-
mance of devices, such as a sensor and detector, has been
reported,141–145 but the regulation of pH on ReRAM devices has
rarely reported. In recent work, we have studied the regulation
of pH on the performance of natural biomaterial-based mem-
ristors, and obtained some meaningful research results.47 In
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fact, the human body is a typical environment in which pH is
maintained in a dynamic balance. Therefore, pH-controlled
memristors have the potential to be applied as implantable
electronic devices. Next, we will discuss in detail the regulation
of pH on the RS performance in recent research works.
For the first time, we prepared a RS memory device with the
structure of Ag/(C7H7O4N)n/F-doped SnO2 (FTO) using natural
biomaterial (C7H7O4N)n extracted from a lichen plant,47 and
pH-controlled RS behavior was observed during the self-colored
switching layer of (C7H7O4N)n. An external voltage was applied
to measure the I–V curves of the Ag/(C7H7O4N)n/FTO cells under
a compliance current of 1.0 mA. The first cycle I–V curves on a
linear scale at different pH conditions are shown in Fig. 13a–c.
The measured electrical I–V curve of the RS device shows an
obvious non-zero-crossing behavior, which strongly suggests a
capacitive effect existed in this RS device, and can explain the
appearance of a reverse non-zero current with a decrease in the
positive voltage. As shown in Fig. 13d, the interface based on
the Ag/(C7H7O4N)n/FTO cell can be equivalent to a parallel plate
capacitor. When a positive external voltage was applied to the
RS cell, the positive charges migrated toward the FTO electrode
and accumulated at the interface of (C7H7O4N)n/FTO, while the
negative charges moved to the Ag electrode and accumulated at
the interface of Ag/(C7H7O4N)n, as shown in Fig. 13e, leading to
a capacitive effect being formed in the testing process. The
reversible switching between HRS and LRS of the memristive
effect is equivalent to the charge and discharge of the capacitive
effect. The internal electric field, which was generated after the
capacitive effect is formed, is the physical mechanism that
causes the I–V curve to non-crossing zero. In a word, this
ReRAM device provides a promising application in the pH-
controlled neuromorphic artificial synapse as well as a selec-
tion of memory states. As mentioned above, the human body is
an environment in which the pH is dynamically balanced, thus
the pH-controlled ReRAM devices have the function of real-time
detection of human pH.
In fact, pH-controlled sensors and batteries are currently
attracting extensive research because of their attractive applica-
tion prospects.146–150 The pH-controlled ReRAM devices also
have rich physical connotations and excellent potential appli-
cation value. The pH controlled RS effect can be used in many
multifunctional devices because organisms usually have a
relatively stable pH environment, so that the performance of
ReRAM devices can indirectly understand the pH of the organ-
ism, so as to achieve the purpose of real-time detection for
organisms. Therefore, pH-controlled ReRAM devices should
have potential applications in the fields of biomedicine and
medical diagnosis.
3. Applications
It can be seen from the above discussion that the RS effect
controlled by multi-factors has the function of preparing a
memristive sensor, which has a very advanced potential appli-
cation in many multifunctional devices. Furthermore, by
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Fig. 12 (a) Schematic illustration of the bending test for the NiO/ZnO naocomposite film-based ReRAM device. (b) The dependence of Vset, Vreset and
ON/OFF ratio on the bending times, respectively. (c) Effect of bending radius on the ON/OFF ratio, Vset and Vreset, respectively. (d) AFM image of the NiO/
ZnO film fabricated on a PET substrate and schematic illustration of the O2 transfer in the NiO/ZnO layer. (e) Schematic of the switching mechanism and
corresponding energy band diagrams for NiO/ZnO devices at zero bias, forward bias, and reverse bias, respectively. Panels a–e were reproduced with
permission.46 Copyright 2019 Elsevier.

introducing flexible substrates, such devices can be applied as
skin-connected or skin-like electronic sensors.151–155 For example,
Changhyun Pang et al. presented a simple architecture for a
flexible and highly sensitive strain sensor that enables the detec-
tion of pressure, shear and torsion.156 Fig. 14a–d show schematic
illustrations of the assembly and operation of a flexible, sand-
wiched device in which two layers with high-density (B1 : 85 
109 cm 2) nanohairs replicated from a silicon master were
reversibly bonded between two flexible polydimethylsiloxane
(PDMS) supports (B500 mm thickness each). Fig. 14b presents a
photograph of the real device with good softness, and the
corresponding SEM image is shown in Fig. 14c. Its working
mechanism is shown in Fig. 14d. When uniformly paired, a small
displacement of hair-to-hair interlocking in response to external
loading can be precisely converted into a change in the electrical
resistance signal with compressive deformations, as illustrated in
Fig. 14e. Therefore, the assembled device was used to detect the
dynamic motion of a small bouncing water droplet and the
physical force of a heartbeat, indicating its potential for applica-
tions in real-time monitoring, skin-like wearable electronics or
implantable medical devices.
It is well-known that the skin transmits sensory information
to the brain through neurons to form a tactile memory when
perceiving external stimuli, so that people can recognize the
stimuli applied to the skin,157–160 as shown in Fig. 15a. Bowen
Zhu et al. integrated the RS memory device with a resistive
pressure sensor, thereby successfully achieving the transmis-
sion and recognition of mimicking human tactile perception
and tactile memory, and can reconfigure the resistance state in
the memory unit by applying pressure on the pressure
sensor.161 As shown in Fig. 15b, the device realized the integra-
tion of the RS memory device and the pressure sensor by
replacing the bottom electrode of the pressure sensor with
the top electrode of the ReRAM device. Fig. 15c schematically
illustrates the operation process: letter molds made of SU-8 on
the PET film were put on the top of the device. Fig. 15d shows a
digital photo of a letter mold ‘‘T’’ on the top of device arrays. As
illustrated in Fig. 15e, the device only beneath the letter molds
can be programmed to LRS by a positive voltage sweep from 0
to Vprogram, providing discernible current mapping of the device
subjected to external pressure. This device has potential appli-
cation characteristics in the manufacture of electronic skins,
humanoid robots, and human-machine interfaces. Therefore,
the design and integration of this haptic memory device
provide guidance for future sensing and memory devices to
imitate other human sensory memory functions. This study

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Fig. 13 (a–c) The typical I–V characteristic curve of the RS device with Ag/(C7H7O4N)n/FTO structure in the first sweeping cycle under different pH
conditions. (d) The interface of the RS device can be equivalent to a parallel plate capacitor. (e) The charge distribution under the charge state in the as-
prepared ReRAM device cell. Panels a–e were reproduced with permission.47 Copyright 2019 Royal Society of Chemistry.

opens up a new way for the development of next-generation
high-performance sensing systems.
In a recent study, researchers used memristors to achieve
human sensory memory and developed a new device that
combines a bionic electronic skin (e-skin) and non-volatile
ReRAM device to create a self-powered artificial tactile memory
system.162 Yihui Sun et al. developed a fully self-powered
flexible smart e-skin integrated with a ReRAM device and
triboelectric nanogenerator (TENG) to successfully memorize
the mechanical stimuli.163 The touching sensing–memorizing–
integrated system was composed of a ReRAM device with a Au/
Ta2O5/AZO structure and poly tetra fluoroethylene (PTFE)/Al
triboelectric nanogenerator device, and the diagram of the
device structure is illustrated in Fig. 15f. Meanwhile, a series
of measurements without external bias, containing a respon-
sive test, nonvolatile test, anti-interference test and recoverable
test, were carried out as presented in Fig. 15g. The touching
sensing–memorizing–integrated system (integrating ReRAM
and triboelectric nanogenerator) matrix with 3  3 pixels in a
size of 1 cm  1 cm was constructed. Accordingly, the measured
currents from each ReRAM cell were summarized and the
results were in good agreement with the motion trajectory.
Therefore, the preparation of this fully self-powered sensor and
memory integrated system may open up new research avenues
for the next generation of high-performance intelligent sys-
tems, which can be applied to smart sensors, electronic skin
and artificial intelligence.
In addition to the ability to perceive external stimuli, the eye
can also perceive light to provide visual information from the
surrounding environment.164,165 Based on a light-controlled RS
effect, Shuai Chen has also designed a facile architecture to
construct an artificial flexible visual sensing system by

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Fig. 14 Multiplex, flexible strain-gauge sensor based on the reversible interlocking of Pt-coated polymer nanofibres. Panels a–e were reproduced with
permission.156 Copyright 2012 Nature Publisher Group.
employing an UV-motivated ReRAM device.166 Fig. 16a shows a
schematic diagram of human visual reception and recognition
information. It is formed by receiving image information from
the retina, which enables individuals to remember the observed
image information.167,168 In this study, they used the ReRAM
device to prepare a bio-inspired flexible visual sensing system
by rationally integrating UV image sensors. In the as-prepared
bio-inspired visual storage unit, the top electrode of the ReRAM
device was replaced by one electrode of the image sensor at
both ends, thereby forming a series of integrated visual storage
devices. From the result of RS performance of the device, it can
be found that the device can adjust the dark current of the
image sensor to match the resistance state of the ReRAM
device. The resistance state of the image sensor can be excited
by external UV light from HRS to LRS. The decrease in resis-
tance in the image sensor will cause the voltage on the ReRAM
device to increase, which would cause the resistance of the
ReRAM device to change from the HRS to the LRS, and the
optical information would be stored in the ReRAM device.
Therefore, the designed bio-inspired flexible visual sensing
system provides a novel way to integrate functional sensors
This journal is © The Royal Society of Chemistry 2022
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and memory devices, thereby opening up new possibilities for
the application of flexible visual memory devices in wearable
electronic devices and electronic eyes in the future.
In addition, Feichi Zhou et al. showed a simple two-terminal
optoelectronic resistive random access memory (ORRAM)
synaptic device for an efficient neuromorphic visual sensing
system that exhibits non-volatile optical RS and light-tunable
synaptic behaviours.169 Fig. 16b illustrates the schematic struc-
ture of the designed two-terminal ORRAM with a structure of
Pd/MoOx/ITO on a SiO2/Si substrate. The inset of Fig. 16b
presents a cross-sectional SEM image of the as-fabricated RS
device. Fig. 16c illustrates the schematic structure of an 8  8
ORRAM array, in which each structural unit is equivalent to a
synapse. In the image recognition process, the researcher
transmits the preprocessed image to a three-layer artificial
neural network to complete the image training and recognition
function, which shows that perfect neuromorphic preproces-
sing can be achieved. Therefore, ORRAM synapse devices have
shown great application potential in the application of neuro-
morphic vision sensing systems by simplifying circuits and
reducing power consumption, which helps to effectively
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Fig. 15 (a) Schematic diagram of human skin responding to applied pressure. (b) Schematic diagram of the haptic memory device that comprises pressure sensing
and RS memory devices. (c) Schematic diagram of recording pressure distribution on letter molds. (d) A digital photo of the mold (letter ‘‘T’’) put on integrated device
arrays. (e) Mapping of the letters ‘‘N’’, ‘‘T’’, and ‘‘U’’. Only device cells beneath the characters can be programmed to LRS. Panels a–e were reproduced with
permission.161 Copyright 2016 Wiley-VCH. (f) Schematic diagram of the integrated TENG and ReRAM system. (g) Photograph of a cell matrix with 3  3 pixels and
relevant current mapping before, in and after press. Panels f and g were reproduced with permission.163 Copyright 2017 American Chemical Society.

Fig. 16 (a) Schematic diagrams of a human visual system when a butterfly was observed by eyes. Panel a was reproduced with permission.166 Copyright 2018
Wiley-VCH. (b) Schematic structure of the MoOx ORRAM. (c) Schematic structure of an 8  8 ORRAM array. Panels b and c were reproduced with permission.169
Copyright 2019 NPG publisher group.

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process a large amount of dynamic visual information from the
surrounding environment.170–172
Pei et al. have developed a new method, in which the
memristors were completely used to simulate the artificial
visual perception nervous system (AVPNS),173 as shown in
Fig. 17a. The system consists of two parts with quantum dot-
based photoelectric memristor and nanosheet-based threshold
switching (TS) memristor. It can use photoelectric and TS
memristors to realize synapse, leakage integral emission
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systems based on memristors can systematically simulate the
functions of the biological visual nervous system, thereby
expanding the potential applications of memristors in artificial
intelligence. In order to achieve strong perception and informa-
tion processing capabilities of biological vision, photoelectric
synaptic units were required to have excellent light response
capabilities and tunable plasticity. Xu’s group showed an
artificial synapse based on a perovskite doped with a methyl-
ammonium (MA) halide.174 The schematic diagram of an as-

(LIF), and neuron function. Applying the proposed AVPNS, it
can successfully demonstrate the biological image perception,
integration and firepower, as well as the process of biosensiti-
zation. In addition, the system can accurately simulate the self-
regulation process of the speed conference control system in an
unmanned car. Therefore, this research shows that hardware
prepared organometallic halide perovskite (OHP)-based artifi-
cial synapse is shown in Fig. 17b. The introduction of MA
halide additives into formamidine lead iodide (FAPbI3) can
effectively improve the morphology and crystallinity of the film,
thereby effectively expanding the adjustment range of synaptic
plasticity. It reveals the influence of light irradiation on shaping

Fig. 17 (a) Visual perception of a nervous memristor-based system imitating the human visual system, and fully memristor-based artificial nervous
system circuit, consisting of a synaptic device (TPI) and a neuron constructed using a TSM (MAM), a capacitor (10 nF), and a resistor (10 kO). Panel a was
reproduced with permission.173 Copyright 2021 American Chemical Society. (b) Schematic diagram of the OHP-based artificial synapse. Panel b was
reproduced with permission.174 Copyright 2021 Elsevier. (c) Schematic illustration of optoelectronic synapses stimulated by three types of light pulses.
(d) Schematic diagram of the photo-induced polarization switching in the BaTiO3 film underneath the monolayer MoS2. (e) A schematic image of
encoding the color information into the corresponding photocurrent intensity. Panels c-e were reproduced with permission.175 Copyright 2021 Elsevier.

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Review
the plasticity of synapses to realize important synaptic func-
tions. With the aid of light stimulation, the device realizes high-
order learning behaviors, including dynamic logic operations
and conditioned reflexes. In the simulation, a higher accuracy
of handwritten digital pattern recognition was achieved. In
addition, the correlation between light irradiation and hybrid
perovskite-based artificial synapses can be used to sense envir-
onmental changes and adjust information processing effi-
ciency. Therefore, this work provides a new idea for building
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advanced artificial intelligence systems.
Furthermore, the rapid development in the field of artificial
intelligence has led to an urgent need for a neuromorphic
vision sensor inspired by the retina with integrated sensing,
memory and information processing functions. Based on this,
Du et al. proposed a neuromorphic vision sensor with a photo-
transistor structure composed of a single layer of MoS2 and a
ferroelectric BaTiO3 film.175 Fig. 17c shows the schematic
illustration of optoelectronic synapses stimulated by three
types of light pulses with wavelengths of 450 nm, 532 nm,
and 650 nm. The schematic diagram of the photo-induced
polarization switching in the BaTiO3 film underneath the
monolayer MoS2 is shown in Fig. 17d. It shows that the light
pulses can change the upward polarization state in the ferro-
electric layer to a downward polarization state as the illumina-
tion time increases. In addition to the conventional electrical
tuning of ferroelectric polarization, phototransistors can also
exhibit neurosynaptic behavior with an adjustable light dose,
Fig. 18 (a) Schematic illustration of a human visual sensing system. (b) Schematic structure of an Au/LSNO/Au photoelectric memcapacitor. Panels a
and b were reproduced with permission.180 Copyright 2020 Wiley-VCH. (c) Schematic diagrams of a human vision system and neuromorphic vision using
the optoelectronic memristor. Panel c was reproduced with permission.181 Copyright 2022 Wiley-VCH.
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with a high switching ratio and good non-volatile memory
function. This was achieved by light-induced ferroelectric
polarization, which can use wavelength-dependent optical sen-
sing and multi-level optical memory characteristics to achieve
neuromorphic visual preprocessing in the sensor. A schematic
image of encoding the color information into the corres-
ponding photocurrent intensity is shown in Fig. 17e. The
simulated artificial neural network constructed by the vision
sensor with neuromorphic preprocessing function shows that
the image recognition rate of the revised National Institute of
Standards and Technology (NIST) handwritten data set can be
significantly improved by reducing redundant data. This work
shows that 2D semiconductor/ferroelectric phototransistors
can provide promising hardware implementations in artificial
intelligence applications for building high-performance neuro-
morphic vision systems.
Through the above discussion, we can clearly understand
that traditional photodetectors can detect images like the
retina, but they lack the memory function of the visual cortex,
as shown in Fig. 18a. Thus, the integration of light sensors and
memory devices has become an urgent research bottleneck for
artificial intelligence applications. Among them, the integra-
tion of light sensor and RS memory is one of the favorable
solutions. In fact, memcapacitors and meminductors also pre-
sent many potential application advantages similar to
memristors.176–179 The constraint relationship between the
voltage and current of the capacitive element and the inductive
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Fig. 19 (a) Schematic diagram of the moisture-powered ReRAM device with a W/WOx/OAC/Pt structure and its moisture-powered reading operation.
(b) Typical I–V curves of the ReRAM device for 100 continuous cycles. (c) Power-free reading of the HRS/LRS through human breath after reversible RS
operations. (d) Demodulated display results of the word ‘‘NENU’’ according to ASCII eight-bit code obtained in moisture-powered reading operations.
Panels a–d were reproduced with permission.182 Copyright 2020 Elsevier.
element is expressed by the derivative or integral, so it is called
a dynamic element. That is to say, the voltage of the device is
related to the history of the current, and it has the function of
memorizing current and is a memory element. Lei Zhao et al.
recently reported a new design by a planar Au/La1.875Sr0.125NiO4
(LSNO)/Au structure, as shown in Fig. 18b, which uses a photo-
electric memcapacitor for artificial optoelectronic synapse
applications.180 This research represents a new paradigm for
artificial optoelectronic synapse sensing systems and opens up
an opportunity for developing low-power humanoid optoelec-
tronic devices for artificial intelligence applications in the
future. In addition, X. Shan et al. developed a plasmonic
photomemristive device using Ag–TiO2 nanocomposite thin
films as the functional layer of the device,181 demonstrating a
multifunctional integrating visual sensing device with low-level
image preprocessing (Fig. 18c). Moreover, the photomemristive
device can also perform high-performance image processing
functions with a high recognition rate and accuracy for
advanced image recognition application in artificial intelli-
gence. Therefore, this work developed a novel plasmonic
optoelectronic ReRAM device with full light modulation cap-
ability, which will facilitate the further development of efficient
neuromorphic vision.
With the diversification of electronic device applications,
the research of self-powered sensor devices is more and more
favored by scientific researchers. In order to design some new
devices with self-powdered capabilities, Ye Tao et al. reported a
moisture-powered memristor in a multi-layer structure of a
W/WOx/oxygen-plasma-treated amorphous-carbon (OAC)/Pt
structure.182 The reversible oxygen migration across the WOx/
OAC interface formed between the memristor layer and the
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nanogenerator layer occurs in this integrated device, which
allows simultaneous modulation of the resistance state and
open circuit voltage (Voc) of a memristive device. Fig. 19a
depicts the memristor with a multi-layer stack of W/WOx/
OAC/Pt and the motivation of the moisture-powered memristor,
which can be used to realize the power-free reading operation
of RS memory. Subsequently, this memristor device presented a
typical bipolar RS behavior as shown in Fig. 19b, in which it can
be seen that the device has a good RS performance with long-
term stability. The low/high-level Voc rather than the HRS/LRS
will be regarded as the readout signal, as illustrated in Fig. 19c.
As shown in Fig. 19d, Voc signals of the HRS and LRS were
respectively represented by the binary values 1 and 0. The pre-
programmed single letters ‘‘NENU’’ can be simultaneously
displayed by the standard eight-bit code of the American
Standard Code for Information Interchange (ASCII) under the
circumstance of human-breathing operation. Therefore, this
research proposed a new concept of the moisture-powered
memristor, which may open the pathway to the development
of self-powered memristive sensors. The self-powered memris-
tive sensor can be used in some implantable bioelectronics in
the future.183–186
4. Conclusion and outlook
As shown in Fig. 20, the multi-factor controlled ReRAM devices
based on RS behavior can be applied to memristive
sensors,187–190 which is expected to be applied to more
advanced artificial intelligence devices, bio-sensing, medical
diagnosis, etc. Thus, more advanced multifunctional devices
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Fig. 20 The multi-factor controlled RS behavior can be applied to mem-
ristive sensors, which is expected to be applied to advanced artificial
intelligence devices.
should be developed by the multi-factor controlled RS effect. In
particular, in order to achieve a fully practical multifunctional
biomedical device based on the RS effect for long-term contin-
uous operation in the human body, the development of bio-
safe materials is very important.191–194 It is undeniable that
devices fabricated using organic materials have many signifi-
cant advantages.195 Therefore, in the development of current
multi-factor controlled ReRAM devices, the choice of functional
materials is also a factor that needs to be considered. Recently,
the choice of functional materials can be transitioned from
semiconductor materials to organic materials, biomaterials
and polymer, thereby preparing the ReRAM devices with
flexible properties, laying the foundation for wearable
electronics.196–205
In addition, the preparation of implantable electronic
devices is an indispensable key technology in biomedicine,
which is also an important support for the development of
biomedicine. In many previous studies, it has been found that
biomemristors have huge potential applications as implantable
devices. The biocompatibility of biomemristors is feasible for
absorbable medical systems, such as biomedical monitoring,
biotherapy, biosensing, bioinformation storage, and neuro-
morphic computing.206 In particular, memristors can mimic
the function of neural synapses,207 which can match the
synaptic behavior of the brain and can be used to monitor
and control bioinformation in real time. The biomemristor
outputs the corresponding current under the applied voltage,
and can complete the multiplication function in parallel.
Similarly, the output currents from multiple biomemristors
can also be used for additive computing functions. By combin-
ing multiplication and addition, biomemristors can be used for
neuromorphic computing.208 In particular, the resistance value
of the memristor can be rapidly and reversibly switched under
the applied voltage, which makes the neuromorphic computing
chip or brain-like chip integrated by the memristor not only
perform energy-saving computing, but can also be reprogram-
mable, which brings unparalleled advantages to neuromorphic
computing.209–212
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In summary, such ReRAM devices add extra-factors as extra
control parameters besides the traditional electrical pulse to
manipulate resistive memories, and it can realize more func-
tions so as to be better used in artificial intelligence, such as
integrating the photodetectors with the nonvolatile memory
devices, which can simulate visual sensing and visual memory
functions. Therefore, the multi-factor controlled ReRAM
devices reveal the potential of functional integration for next-
generation nonvolatile memory and other applications in
electronics, physical devices, bio-sensing, medical diagnosis,
and so on.
Author contributions
B. Sun drafted the review manuscript. G. Zhou made revisions.
T. Yu and Y. Chen made some discussions. F. Yang and Y. Zhao
gave some useful suggestions. All authors gave their approval to
the final version of the manuscript.
Conflicts of interest
The authors declare no conflict of interest.
Acknowledgements
The authors gratefully acknowledge financial support from the
Sichuan Science and Technology Program (Grant No.
2020YJ0086), the Fundamental Research Funds for the Central
Universities (Grant No. 2682021CX076), and the National Key
R&D Program of China (No. 2017YFE0301401), and Y. Zhao is
grateful to the Fujian Normal University for the financial
support of the talent project.
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