Chemical Physics 516 (2019) 168–174

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Chemical Physics
journal homepage: www.elsevier.com/locate/chemphys

A nonvolatile organic resistive switching memory based on lotus leaves T

a,1 a,b,⁎,1 c b a b
Yiming Qi , Bai Sun , Guoqiang Fu , Tengteng Li , Shouhui Zhu , Liang Zheng ,
⁎
Shuangsuo Maoa, Xiang Kanb, Ming Leib, Yuanzheng Chena,
a
School of Physical Science and Technology, Key Laboratory of Advanced Technologies of Materials, Southwest Jiaotong University, Chengdu 610031, China
b
Superconductivity and New Energy R&D Center (SNERDC), Southwest Jiaotong University, Chengdu, Sichuan 610031, China
c
Department of Electromechanical Measuring and Controlling, School of Mechanical Engineering, Southwest Jiaotong University, Chengdu, Sichuan 610031, China

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

Keywords: The resistance random access memory (RRAM) based on biomaterials, which has the advantages of sustainable,
Lotus leaves green and environment-friendly, has great potential application in the sustainable electronic devices. Herein,
Organic memory lotus leaves, a very common aquatic herb serve as a dielectric layer, was used to prepare an organic resistive
Resistive switching switching memory device with Ag/Lotus leaves/ITO structure for the first time. The biodegradable electronic
Biodegradable
device demonstrates a nonvolatile resistive switching memory behavior with large resistance ratio and long
Bio-RRAM
switching endurance at room temperature. This work exhibits the application prospect of the biomaterials in
electronics with the biodegradability and biocompatibility, which provide an effective supplement to the re-
search of organic bio-RRAM.

1. Introduction environmental damage [11,12]. Therefore, the biodegradability and

With the rapid development of electronic technology, the conven-
tional memory has hit a bottleneck in recent years, which is attributed
to the miniaturization of electronic devices [1]. Some novel memory
technology, such as magnetic random access memory (MRAM) [2],
phase-change random access memory (PRAM) [3] and resistance
random access memory (RRAM) [4], have been proposed to solve these
problems. Especially RRAM, which is considered to be the most likely
next-generation memory technology, are favored by researchers be-
cause of their lower cost, faster read and write speeds and higher in-
tegration density [5,6]. Simply speaking, a memristor is a passive
electronic device with a memory function: the resistance can be re-
versibly changed under the applied current or voltage [7,8]. The
memory operation of resistive switching device is simple to understand:
If we define the high resistance state (HRS or “OFF” state) or the low
resistance state (LRS or “ON” state) respectively as logic “1” and “0”,
the memory device can implement the function as a storage unit for
information in the electronics [9].
It is well known that the increasing demand for electronic equip-
ment would bring serious environmental issues [10]. The detrimental
substances (Pb, Cd, Hg and PVC) in the electronic devices and excessive
accumulation of electronic waste play a non-negligible role in
biocompatibility of biomaterial attract more attention from researchers
and scientists [13–15]. It is well known that biomaterial is biodegrad-
able, sustainable and environmental-friendly for electronic product.
More importantly, the research of biomaterial provides new concepts
for the development and manufacturing process of the next generation
electronic devices [16]. Such a scheme has been successfully applied
and realized in some resistive switching devices, such as chicken egg
albumen and DNA have been used as active layer to prepare resistive
switching memory [16,17] because the abundance and renewability of
biological resources will bring about a reduction in the expenditure on
electronic equipment to a large extent, especially for plant materials,
many reports have addressed that the potential application of plant-
based switching devices with their good memory properties, such as
dead leaves, pectin and aloe vera based resistive switching memories
[15,18,19], as shown in Table 1.
Here, we demonstrate an eco-friendly resistive switching device
based on lotus leaf, the lotus leaf was often used for medicinal herbs,
cooking and viewing. The micron-thick level Ag/Lotus leaves/ITO de-
vice reveals the potential of lotus leaves in electronic applications due
to its large switching resistance ratio (memory window) and stable
cycle at room temperature. The natural organic material can be pre-
pared an environmentally-friendly, low cost, wearable and

⁎
Corresponding authors at: School of Physical Science and Technology, Key Laboratory of Advanced Technologies of Materials, Southwest Jiaotong University,
Chengdu 610031, China.
E-mail addresses: bsun@swjtu.edu.cn (B. Sun), cyz@calypso.org.cn (Y. Chen).
1
These authors contributed equally for this work.

https://doi.org/10.1016/j.chemphys.2018.09.008
Received 8 July 2018; Accepted 9 September 2018
Available online 11 September 2018
0301-0104/ © 2018 Elsevier B.V. All rights reserved.
Y. Qi et al. Chemical Physics 516 (2019) 168–174

Table 1 school pond. We cleaned those leaves with distilled water and dried
Some biomaterials based resistive switching memory. them in an oven at 50 °C until the water completely evaporates.
Functional Bio- Top electrode Bottom Substrate ON/OFF References Afterwards we used a crusher and a filter to develop the blade into
material electrode ratio powder. The resulting powder was kept in bags and kept in a dry en-
vironment. During the experiment, the instruments were cleaned with
Chicken egg Al ITO Glass 103 [16]
deionized water and ethanol to remove impurities.
albumen
DNA Au Au SiO2/Si 102 [17]
Dead leaves Ag Ti PET 50 [15] 2.2. Preparation of device
Pectin Ag FTO Glass 450 [18]
Aloe vera Al ITO Glass 103 [19] The structure and preparation process of the Ag/Lotus leaves/ITO
resistive switching device is shown in Fig. 1(a). Indium tin oxide (ITO)
served as the bottom electrode was fabricated on the surface of glass.
biodegradable memory device. The proposed devices feature a simpler We mixed the lotus leaf powder with N-methyl-2-pyrrolidone, and were
fabrication process besides outstanding switching properties and relia- spin-coated uniformly on the ITO. After the lotus leaf was completely
bility which demonstrates the potential of plant-based memory. deposited, we dried the sample in an oven at a temperature of 50 °C
until the weight stays constantly. Then, the Ag top electrodes with the
2. Experiment and method diameter of about 2 mm2 were deposited on the lotus leaves layer. In
this way, a device with an Ag/Lotus leaves/ITO/Glass layered structure
2.1. Preparation of materials was prepared. Since the relative content of lotus leaves is much larger
than that of Ag and ITO, the device properties are mainly manifested by
A lotus leaf with a diameter of about 30 cm was collected from the lotus leaves.

Fig. 1. (a) Preparation of the Ag/lotus leaves/ITO device and SEM image of cross section. (b) XRD spectra of lotus leaves powder. (c) EDS spectra of lotus leaves, the
inset show the FT-IR spectra of as-prepared lotus leaves powder.

169
Y. Qi et al. Chemical Physics 516 (2019) 168–174

Fig. 2. (a) The characteristic I-V curve of the Ag/Lotus leaves/ITO heterostructure. (b) I-V curve under a scanning voltage with 100 cycles. (c) The resistance-cycles
number curve under a positive bias voltage of 1.5 V. (d) Retention test of Ag/lotus leaves/ITO memory device under a read voltage of 1.5 V.

2.3. Characteristics

The microstructure of lotus leaf powder was analyzed by X-ray

diffraction (XRD). Specific components can be derived from energy-
dispersive spectroscopy (EDS). And molecular structure of lotus leaves
powder was characterized using fourier transform infrared spectro-
scopy (FTIR, Nicolet 5700). The electrical properties were measured by
adding a cyclic scanning voltage at room temperature using an elec-
trochemical workstation, where Ag and ITO act top and bottom elec-
trodes respectively.

3. Result and discussion

Fig. 1(a) show the cross section SEM image of lotus leaves layer, in
which we can see that the thickness of the lotus leaf layer spin-coated
on the bottom electrode is about 10 µm while the thickness of the ITO
film is about 200 nm, which indicates the lotus leaves film has a large
proportion in the entire device. The XRD pattern of the lotus leaves
powder is shown in Fig. 1(b), showing a broad peaks around 2θ = 22°
and a weak peak at around 2θ = 50°, which indicate that the lotus
powder contain a large amount of amorphous carbon [20]. In Fig. 1(c), Fig. 3. The I-V curve of the Ag/Lotus/ITO device at 40 °C.
the result of EDS exhibits the element components of as-prepared lout

170
Y. Qi et al.
leaves layer. It is shown that in addition to the common C, O, K ele-
ments in organic matter, other elements, such as S, Cl and Ca elements,
are also detected in the dielectric layer. The more specifically structural
properties of leaves powder can be detected by FT-IR spectra in the
inset of Fig. 1(c). The broad band at 3420 cm−1 is assigned to the
stretching vibration of hydroxyl groups (–OH). The band at 2923 cm−1
corresponds to the antisymmetric stretching vibration of CH2 in starch
molecules. The band at 1643 cm−1 is from the free carboxyl groups
(C–O–O) in carbohydrate group and the band at 1440 cm−1 is from the
deformation vibration of CH2. The other absorption bands are:
1250 cm−1 from –CH2OH related mode, 1150 cm−1 from C–C and C–O
stretching, 1056 cm−1 from C–O stretching [21].
The quality of the switching memory can be reflected by the
switching ratio and retention [22,23]. To verify the resistance
switching behavior of the Ag/Lotus/ITO structure device, we obtained a
typical current-voltage (I-V) response at room temperature by applying
a direct cycling scanning voltage window (−6.5–6.5 V) between the Ag
and ITO electrode. The characteristic I-V curve of the Ag/Lotus leaves/
ITO heterostructure in Fig. 2(a) exhibits an asymmetric hysteresis be-
havior. As these arrows indicate, the DC scanning voltage is from 0 V →
6.5 V → 0 V → -6.5 V → 0 V with the scanning speed of 0.02 V/s.
Fig. 2(b) display the I-V curve for about 100 cycles which demonstrates
a clearly relative stability. We noticed that our device exhibits an ob-
vious bipolar switching behavior with rapid conversion and great re-
producibility. In other words, such a plant-based device exhibits ex-
cellent resistance switching properties that are comparable to those of
previous work [19]. We notice the resistance switching behavior of the
Ag/Lotus leaves/ITO structure with two stable resistance states fol-
lowed by a transition of current when voltage reaches a certain value.
At about 5.0 V (Vset), the device completes the transition from HRS
(“OFF” state) to LRS (“ON” state). In memory we define it as the “Set”
procedure. Similarly, the device repeatedly exhibit a “Reset” process
when the applied voltage sweeps −3.0 V (Vreset) and returns from LRS
to HRS. Two well-resolved resistance states (memory window) provides
distinguishable logic states to manipulate data bits which is the prin-
ciple of RRAM applications [24,25].
To investigate the switching stability, we demonstrate the change of
the I-V curve in a cyclic voltage sweeping about 100 cycles are shown in
Fig. 2(c). The resistance of the two different states was calculated, re-
spectively, with the function of sweeping cycles. To prevent the possible
effects of the read voltage [26], a low bias voltage is set at 1.5 V. We can
clearly see that the resistance is approximately 1.69 GΩ at “OFF” state
while “ON” state is about 0.057 GΩ at the initial time, signifying that
Fig. 4. (a) and (b) I-V curves in log-log scale for Ag/Lotus leaves/ITO structure, the scatters are experimental data and straight lines are the fitting curves while the
numbers are slopes of them.
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Chemical Physics 516 (2019) 168–174
the resistance ratio reaches almost 40. We observed that the stability is
relatively stable, but there is a gradual degradation process before 50
cycles. As the experiment progressed, the resistance ratio stabilized at a
value of about 25 keeping 100 cycles which indicates has a relatively
satisfactory performance of the resistance switching performance of
Ag/Lotus leaves/ITO device for plant-based memory. In other words,
the lotus-based RRAM devices can maintain a low misreading rate for
extended periods of operation for data storage [27,28]. In addition, in
Fig. 2(d) we can see that the Ag/Lotus leaf/ITO device shows good
resistance conversion effect in 1000 s, confirming the non-volatile and
non-destructive readout performance of the device [29,30].
To further understand the attenuation of the device with the in-
creasing of testing cycles, we tested the resistance switching char-
acteristics of the device at 40 °C, as shown in Fig. 3. We can see that the
high and low resistance ratios are decreased. In other words, when the
device is operated in a high temperature environment, the resistance
value of the high resistance state is lowered to cause the switching ratio
to decrease. Similarly, we can assume that the resistance conversion of
the memristor during operation is attenuated due to the increasing in
device temperature. The degradation of the performance of resistance
switching is related to the large amount of heat generated locally during
the operation of the memory, which leads to complex electrochemical
reactions in the electrolyte layer [31,32]. This phenomenon will ac-
celerate the biofilm deteriorating. Based on the above results, the
memory effect of the resistance transition of the Ag-lotus leaf-ITO de-
vice demonstrates the feasibility of the biomaterial-based resistive
switching memory in future RRAM storage applications.
To further investigate the mechanisms of switching and conduction
behavior of resistive switching device, Fig. 4(a,b) shows the I-V curve
and fitted line in both positive and negative voltage regions on the log-
log scale. Clearly, the slope of the fitting curve at LRS (“ON” state)
confirms the Ohmic conduction behavior (I ∝ V) [33,34]. However, the
I-V curve is clearly divided into two parts at HRS (“OFF” state). In the
positive voltage region, the device behaves as an Ohmic behavior in a
low voltage (0–4.5 V) as well, which can be understood as that the
density of carriers generated by thermal excitation is dominant com-
pared to the injected carriers [35,36]. In a high voltage, the slope of the
fitted line rapidly increases, which can be seen as the joint action be-
tween trap-controlled space charge-limited current (SCLC) effect
e (eV ) / (4πε ε d)
(I ∝ V2) and Schottky emission (SE) (ln I ∝ kT
r 0
). Such phe-
nomenon is understood as the defects in the lotus leaf form some bands
under the conduction band where the injected carriers will be trapped
Y. Qi et al.
Fig. 5. (a) The I-V curve of the Cu/Lotus leaves/ITO structure. (b) The I-V curve of the Al/Lotus leaves/ITO structure.
[37]. When the voltage exceeds 4.5 V, all the valid defects will be filled
up, and the device will go through a “Reset” process, where the state
switches from the HRS to the LRS. The larger slope in the actual mea-
surement can attribute to the density and energy distribution of the
defects [17].
In recent years, the mechanism of resistance switching in bioma-
terial-based device has been extensively discussed in previous reports
[38–40]. It is widely recognized that the formation of metallic filament
in a dielectric layer due to the electrolytic migration of cations and
anions play a significant role in the switching effect [41–43]. In brief,
the breakage and formation of the conductive filament in the dielectric
material enable the device to complete the switch of the OFF state and
the ON state [44,45]. In this process, effect of top electrodes is very
significant. The K, Ca elements enriched in the Ag/Lotus/ITO structure
undergo a similar ionization process as Ag. Ca and K atoms present in
the electrolyte layer are ionized to form Ca2+ and K+ by electro-
chemical process under a sufficiently large electric field [46]. These
ions move in a direction under the action of an electric field to form a
conductive path, completing the conversion process of the memristive
device. In fact, this mechanism is one of the most widely accepted
Fig. 6. A schematic diagram of the conductive filament model demonstrating the resistive switching mechanism.
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Chemical Physics 516 (2019) 168–174
physical mechanisms. In order to deeply study the contribution of the
top electrode to the conductive filament model in the device resistance
transformation, we changed different active metals, such as Cu and Al
as electrodes. The I-V results are shown in Fig. 5, which show Ag
electrodes based sample have better performance than other metals
with high HRS/LRS resistance ratio and good stability. Therefore, we
can believe that the Ag electrode plays a key role in the conduction
mechanism of the device. Based on the above analysis, we propose in
the article that metal ions formed conductive filaments dominate the
resistance switching mechanism.
Based on the above discussion, for the Ag/Lotus leaf/ITO device, Ag
ions and oxygen vacancies in the lotus leaf are the mainly reasons for
the resistance switching behavior in Fig. 6(a). The schematic is shown
in Fig. 6(b–g). Under the certain electric field, a portion of the Ag atoms
are ionized to form Ag ions which can be described as Ag → Ag+ + e−.
Ag ions, oxygen vacancy and other metal ions (K+, Ca+, etc) move
directionally under the application of an electric field shown in
Fig. 6(b). During this process, the molecular chains in the leaves serve
as a mobile channel for these ions. When the electric field accelerates
cations and oxygen vacancies to a certain extent, the conductivity of the
Y. Qi et al.
dielectric layer will increase dramatically because these ions will be
reduced for forming the conductive filaments in Fig. 6(c). The above
complete process is the machanism of the “Set” process of the device.
Therefore, Ag ions, oxygen vacancies, and other metal ions (K+, Ca+,
etc) enter the lotus leaf layer and form conductive filaments under the
action of a high electric field (> Vset) which changes the device to the
LRS. After that, the device will remain LRS in Fig. 6(e), until a sufficient
voltage of opposite polarity (< VReset) dissolute the formed conductive
filaments at the weakest point shown in Fig. 6(f), which is defined as
“Reset” process. After that, Ag ions, oxygen vacancy and metal ions
(K+, Ca+, etc) drift back to the Ag electrode due to the function of
electric field prompting the switch to HRS state in Fig. 6(g). Therefore,
the device can be repeatedly switched via formation and rupture of
conductive filaments.
4. Conclusions
The lotus leaves powder serve as the dielectric layer to prepare a
resistive switching device via spin coating technique for the first time.
This Ag/lotus/ITO device exhibits an obvious switching behavior with a
HRS/LRS resistance ratio of about 40 and stable memory time of more
than 1000 s, which reflects the potential application in future bio-
RRAM. Also, the results verify the conductive filaments model in the
organic switching memory play a significant role. This work provides a
simpler fabrication mothed for biomaterial-based memory and an ef-
fective supplement to the research of inorganic memristors as well, and
it may be useful in making the hybrid complementary metal oxide
semiconductor devices, neuron/memristor-synapse approach.
Acknowledgements
This work was supported by the National Key Research and
Development Plan (No. SQ2017YFE030073), the National Natural
Science Foundation of China (No. 11604270, 11704050), the
Fundamental Research Funds for the Central Universities
(2017X02012, 2018GF08).
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