Emerging Memory Devices For Artificial Synapses

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Materials Chemistry C
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Emerging memory devices for artificial synapses

Cite this: J. Mater. Chem. C, 2020,
Youngjun Park,† Min-Kyu Kim† and Jang-Sik Lee *
8, 9163
Increasing demands for new computing systems to fulfill enormous information processing have driven
the development of brain-inspired neuromorphic systems that can perform fast and energy-efficient
computing. Neuromorphic computing requires efficient artificial synapses. Emerging memory devices to
replace complementary metal-oxide semiconductors are being evaluated. This paper reviews recent
Received 24th March 2020, developments in artificial synapses that exploit emerging memory devices for use in neuromorphic
Accepted 5th June 2020 devices and systems. The synaptic behaviors and plasticity are described to provide the analogy between
DOI: 10.1039/d0tc01500h biological and artificial synapses, then the operation mechanism and emulation of synaptic plasticity
using various materials and structures are provided. The remaining challenges and outlooks in the
rsc.li/materials-c development of artificial synapses that use emerging memory devices are outlined.
1. Introduction information, with ultralow energy consumption.5,6 A human

brain consists of B1011 neurons which are connected by B1015
Neuromorphic computing systems combine processing and synapses.7,8 These neural networks combine memory with
memory in a single unit as in a brain. This architecture is computing in the same unit.
different from the conventional ‘von Neumann’ computing For these reasons, neuromorphic computing systems that can
system, which separates processing and memory, and therefore emulate the brain have been sought. Initial attempts to emulate
requires shuttling of information between the components that neural networks have combined machine-learning software and
perform the two processes. This shuttling slows processing and neuromorphic hardware composed of complementary metal-
increases energy consumption.1–3 These problems become oxide semiconductors (CMOSs).1,9,10 These approaches have
increasingly serious when complex information is processed.4 limited application because synaptic devices that use CMOS
In contrast, a human brain can process complex information, technology require 410 transistors to emulate synaptic func-
such as pattern recognition and analysis of unstructured tions, so the resulting neural networks have large device areas,
high energy consumption, and limited operation speed.11–13
Implementation of energy-efficient neuromorphic hardware
Department of Materials Science and Engineering, Pohang University of Science and
requires devices that can emulate synaptic functions of bio-
Technology (POSTECH), Pohang 37673, Korea. E-mail: jangsik@postech.ac.kr;
Tel: +82-54-279-2153 logical synapses in a single unit. Therefore, numerous designs
† These authors contributed equally. for such devices have been investigated. Examples include
Youngjun Park received his BS Min-Kyu Kim received his BS

degree in Materials Science and degree in Materials Science and
Engineering from Inha University Engineering from the University of
in 2016. He is now pursuing his Seoul in 2016. He is now pursuing
PhD degree in the Department of his PhD degree in the Depart-
Materials Science and Engineering ment of Materials Science and
in POSTECH under the super- Engineering in POSTECH under
vision of Prof. Jang-Sik Lee. His the supervision of Prof. Jang-Sik
research interests include emerging Lee. His research interests include
memory and neuromorphic devices. emerging memory and neuro-
morphic devices using ferroelectric
materials.
Youngjun Park Min-Kyu Kim
This journal is © The Royal Society of Chemistry 2020 J. Mater. Chem. C, 2020, 8, 9163--9183 | 9163
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Review Journal of Materials Chemistry C
two-terminal devices such as resistive switching memory

(RSM),14–18 phase-change memory (PCM),19–22 and ferroelectric
tunnel junctions (FTJs);23–27 and three-terminal devices such as
ferroelectric transistors,28–35 electrochemical devices,36–43 and
floating-gate transistors.44–47 All these devices can emulate
functions of biological synapses, such as analogue memory
switching behaviors, spike-rate-dependent plasticity (SRDP),

and spike-timing-dependent plasticity (STDP). Therefore, they
have the potential to realize hardware implementation of
artificial neural networks.
This paper reviews recent advances in artificial synapses
Fig. 1 (a) Schematic illustration of neurons and a synapse in a biological
based on emerging memory devices for neuromorphic comput-
system. (b) Schematic illustration of synaptic transmission in a biological
ing systems. It begins with a presentation of synaptic behaviors synapse. The arrival of an action potential causes the release of neuro-
and plasticity such as short-term plasticity (STP), long-term transmitters, which enables synaptic transmission from pre- to post-
plasticity (LTP), SRDP, STDP, and heterosynaptic plasticity. synaptic neurons. Reproduced with permission.43 Copyright 2019, The
Then, it provides recent developments in emerging memory devices Royal Society of Chemistry.
that can emulate synaptic functions, and finally summarizes
the current status of artificial synapses and outlines remaining
cleft (Fig. 1b).49 They diffuse across the synaptic cleft and bind
challenges.
to receptors on the post-synaptic membrane. This process causes
the ion channel to open and close, and can generate a post-
synaptic action potential. Some neurotransmitters excite the post-
2. Overview of synaptic plasticity synaptic potential, and some inhibit it. The post-neuron may be
2.1. Synaptic transmission stimulated by numerous pre-neurons; its reaction depends on the
sum of generated post-synaptic potentials. In a brain, excitatory
In a biological nervous system, information transmission occurs
and inhibitory post-synaptic potentials are important in informa-
across synapses, which are connections between pre- and post-
tion processing, learning, and memory.8,49
neurons (Fig. 1a). A synapse is composed of three parts: the pre-
synaptic membrane, the synaptic cleft, and the post-synaptic
membrane. Information transmission and processing by 2.2. Short-term and long-term synaptic plasticity
synapses entail a complex process that is usually initiated by In a brain, each neuron is connected to other neurons by
depolarization of an ion gradient across the membrane of the thousands of synapses. The strength of the connection between
pre-neuron.48 This depolarization is called an action potential. pre- and post-neurons is called synaptic weight; it can be
When it reaches the pre-synaptic membrane, the action potential modulated by synaptic plasticity, which is an activity-dependent
activates voltage-gated Ca2+ channels, so the concentration of modification of synaptic weight in response to stimuli.50 This
Ca2+ increases inside the pre-synaptic membrane, then vesicles modification is a form of learning. Synaptic plasticity can be
that contain neurotransmitters release them into the synaptic divided into STP and LTP.51,52
STP is temporary change in synaptic weight, and lasts from
ms to several min.49 STP can be excitatory (potentiation) or
Jang-Sik Lee received his BS, MS, inhibitory (depression). Short-term potentiation and depres-
and PhD degrees in Materials sion are responses to short stimuli. For STP, paired-pulse
Science and Engineering from facilitation (PPF) and paired-pulse depression (PPD) are the
Seoul National University, Seoul, most common learning rules.53,54 In a biological synapse, when
South Korea, in 1997, 1999, and two consecutive action potentials arrive within a short interval,
2002, respectively. In 2002, he the synaptic weight is temporarily increased or decreased.55 In
joined the Los Alamos National PPF, the second action potential induces a larger post-synaptic
Laboratory as a director’s current than the first action potential; in PPD the opposite
postdoctoral fellow. In 2004, he response occurs. The increase or decrease in synaptic current is
joined the Memory Division of amplified as the interval between the two spikes decreases
Samsung Electronics as a senior (Fig. 2a).56 PPF and PPD are caused by an increase or a decrease
research engineer and oversaw in the pre-synaptic Ca2+ concentration.57
Jang-Sik Lee the integration and device LTP is a permanent change in synaptic weight, and is
reliability of 32 gigabit NAND generated by repeated stimulation. In a biological synapse, the
flash memory. He worked for Kookmin University from 2006 to transition from STP to LTP is caused by structural modification
2013. In 2013, he joined POSTECH, South Korea, where he is of the synapse. During repeated stimulation, the changes in Ca2+
currently a professor in the Department of Materials Science and concentration can induce changes in dendrite size.58 A model of
Engineering and Mueunjae Chair Professor. short-term memory (STM) and long-term memory (LTM) invokes
9164 | J. Mater. Chem. C, 2020, 8, 9163--9183 This journal is © The Royal Society of Chemistry 2020
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Journal of Materials Chemistry C Review

Fig. 2 Synaptic plasticity. (a) PPF characteristics of CA3 pryamidal cells in knockout (KO) and wildtype (WT) mice. (Scale bars: vertical = 100 pA, horizontal =
100 ms.) Reproduced with permission.56 Copyright 2019, Frontiers Media SA. (b) Schematic illustration of an STM-to-LTM transition memory model.
Reproduced with permission.18 Copyright 2018, American Chemical Society. (c) STDP characteristics of a biological synapse following the asymmetric
Hebbian learning rule. Reproduced with permission.64 Copyright 1998, Society for Neuroscience. (d) Four forms of STDP learning rules (symmetric and
asymmetric Hebbian; symmetric and asymmetric anti-Hebbian). Reproduced with permission.66 Copyright 2014, Springer Nature. (e) Change in synaptic
plasticity with stimulation frequency. Reproduced with permission.52 Copyright 2011, National Academy of Sciences. Schematic illustration of
(f) homosynaptic plasticity and (g) heterosynaptic plasticity. Reproduced with permission.78 Copyright 2015, John Wiley & Sons, Inc.
STP and LTP.59 In this model, the information that is stored by These characteristics show asymmetric forms of STDP. In other
STM disappears after the stimulus is removed. Transition to forms of STDP, the synaptic weight is determined only by relative
LTM enables long-term storage of information (Fig. 2b). timing difference of spikes between pre- and post-synaptic
neurons regardless of their order.66 In all cases, the change in
2.3. Spike-timing-dependent plasticity synaptic weight increases as Dt decreases.
Synapses are responsible for transmission of electrical or
chemical signals, and for memory and learning in a brain.60 2.4. Spike-rate-dependent plasticity
STDP, also known as Hebbian learning, is a fundamental In biological systems, synaptic plasticity is a basis of memory
function of synaptic plasticity in a biological synapse.61,62 Hebb and learning functions.67 The strengthening and weakening
postulated that if axons repeatedly and continuously excite of synaptic weights are regulated by the concentrations of
another, some growth processes or metabolic changes are various ions such as K+, Ca2+, and Na+.61,68 Ions flow through
induced in one or both cells.63 STDP describes the change in ion channels in synapses and neurons, and lead to signal
connection strength between neurons after repeated stimula- processing and learning in a brain. SRDP is another funda-
tion of the post-synaptic neuron by the pre-synaptic neuron.61 mental characteristic of synaptic plasticity.52 The existence of
The concept has been used to explain cellular learning in SRDP may solve the selectivity and stability problems of synaptic
computational neuroscience and in neuromorphic hardware plasticity that are encountered in Hebbian learning.69,70 The
design. The asymmetric characteristics of STDP were discovered strength of synaptic plasticity is modulated by the pre-synaptic
in cultures of hippocampal cells (Fig. 2c).64 The extent and spike rate (Fig. 2e).52 A train of synaptic spikes with high
direction of modifications in synaptic weights are determined frequency induces long-term potentiation of synaptic connec-
by the relative timing of pre- and post-synaptic spikes. When a tions, whereas a train of spikes with low frequency induces
pre-synaptic spike arrives at time tpre before the post-synaptic long-term depression of the connections.52,71 These SRDP
spike arrives at time tpost at interval Dt = tpost tpre 4 0 of tens of characteristics are consistent with the BCM learning rule,52,69
ms, then the synaptic weight is positive and long-term potentia- in which synaptic plasticity is adjusted by post-synaptic activity
tion behavior is achieved, whereas if Dt o 0, the synaptic weight determined by the firing rate of pre-synaptic spikes.52,69 Low
is negative and long-term depression is induced. Four forms of post-synaptic activity weakens the synaptic efficacy, whereas
STDP characteristics have been reported (Fig. 2d); they show high post-synaptic activity strengths it.
different functions in information processing and storage.65 The
synaptic forms change depending on the types of synapses (e.g., 2.5. Heterosynaptic plasticity
inhibitory or excitatory) and the timing of spikes. In some cases, Information processing in a synapse is achieved by synaptic plasti-
the change in synaptic weight depends on both relative timing city controlled by Hebbian learning, which mediates the formation
and the order in which pre- and post-synaptic spikes arrive.66 and refinement of neural connectivity.72 Synaptic plasticity
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consists of homosynaptic and heterosynaptic plasticity.72 Interface-type RSM is operated by the modulation of the
Homosynaptic plasticity is input-specific synaptic plasticity, distribution of oxygen vacancies or metal ions at the interface
which indicates that the strength of a synaptic connection between the insulator and the electrodes.83,88
changes only if a post-synaptic neuron is specifically stimulated RSM can show either binary or analogue (gradual) switching
by a pre-synaptic neuron (Fig. 2f).62,72 Homosynaptic plasticity behavior.14,84,89 The type of resistive switching behavior
is believed to provide a cellular mechanism for learning depends on the switching mechanism, materials, and device
and refinement of neural connectivity in biological systems.73 structures. RSM with binary switching exhibits abrupt set and
However, the synaptic plasticity that uses Hebbian learning has reset behaviors. Therefore, to achieve multi-level data storage
the inherent limitation. Hebbian learning exhibits intrinsic characteristics, compliance currents ICC during the set process
positive feedback on synaptic changes.72,74 Potentiated synapses need to be controlled.90,91 RSM with analogue switching behavior
increase the probability that the neuron will generate a spike, can show gradual set and reset processes, so the resistance can be
which enables potentiation of additional synapses, whereas gradually modulated by the applied biases. These traits can be
depressed synapses have a lower probability of generating exploited for neuromorphic applications. RSM devices that use
spikes, so synapses tend to be further depressed.75 This positive various types of materials have been evaluated as artificial
feedback loop is prone to cause the synaptic weights to increase synapses; these devices are reviewed in this section.
to the maximum value in potentiation or to decrease to zero in 3.1.1. Inorganic artificial synapses. Many inorganic materials
depression, and thus lead to the over-excitability or silencing of have been suggested for use in RSM as artificial synapses.16,17,92–100
neurons.72 Both reactions impair the computational abilities of One inorganic synapse device composed of a layered device
neural networks.72 This ‘runaway’ of synaptic weights can be structure has a co-sputtered Ag and Si active layer with a properly
solved by heterosynaptic plasticity, which occurs in synapses that designed Ag/Si mixture ratio gradient. This layered structure has
are not active during the induction of homosynaptic plasticity.73 Ag-rich and Ag-poor regions; in this device, the conductance
The activity of a modulatory interneuron between the pre- can be controlled by the movement of Ag+ between these
synaptic neuron and post-synaptic neurons can affect the synaptic regions (Fig. 3a).14 The current of the device continuously
connection (Fig. 2g).76 Heterosynaptic plasticity constrains the increased during positive voltage sweeps, and decreased during
instability by normalizing or limiting the change in the total negative voltage sweeps (Fig. 3b). Application of 100 identical
synaptic input, and thus effectively preventing the runaway of pulses incrementally changed the conductance of the device:
synaptic weights to the maximum or to zero.72,75,77 Heterosynaptic positive pulses increased it, and therefore emulated potentia-
plasticity has been observed in central and peripheral synapses. It tion; negative pulses decreased it, and therefore emulated
performs important functions of biological synapses such as long- depression (Fig. 3c). Also, inorganic synapses can implement
term memory, sensory perception, and associative learning.78 PPF, which is an important synaptic function in a brain.
Both homosynaptic plasticity and heterosynaptic plasticity have Inorganic resistive switching devices with a Pd/WOx/W struc-
important functions in a brain, so artificial synapses need to ture showed PPF characteristics.15 The conductance of these
mimic both of them. devices was modulated by redistribution of oxygen vacancies.
The conductance was high in regions that had oxygen vacan-
cies, and low elsewhere. Oxygen vacancies can be migrated by
3. Emerging devices for artificial an applied electric field; therefore, an applied pulse can
synapses increase the conductance of the device. Afterward, the conduc-
tance decayed due to the spontaneous diffusion of oxygen
3.1. Resistive switching memory for artificial synapses vacancies. These oxygen-vacancy dynamics were used to emu-
RSM has been studied as an emerging candidate for artificial late the PPF characteristics of a biological synapse. When two
synapses due to its low power consumption, fast operation speed, identical pulses were applied sequentially, the current spike
and compatibility with three-dimensional (3D) integration.79–81 during the second voltage pulse was larger than that during the
RSM is a two-terminal device that has a simple metal–insulator– first pulse; this change is similar to PPF in a biological synapse
metal (MIM) structure. The applied voltage induces resistance (Fig. 3d). As the interval between the two pulses was reduced,
changes in the devices.82,83 The ‘set’ process is a switch from a the amplification increased. The change in conductance imme-
high resistance state (HRS) to a low resistance state (LRS). The diately after the pulses also showed a similar behavior to a
‘reset’ process is a switch from an LRS to an HRS. RSM can have biological synapse (Fig. 3e). As an extension of PPF, 10 con-
either unipolar or bipolar switching behavior. In unipolar tinuous voltage pulses were applied with different frequencies
switching, the set and reset processes occur at applied voltages to determine how the frequency of stimuli affected the change
with the same polarity, whereas in bipolar switching, the reset in conductance. The current increased when the frequency of
process is achieved by applying a voltage with the opposite the applied voltage pulses increased (Fig. 3f). A second-order
polarity to that of the set process.82,84 synaptic device composed of Pd/Ta2O5 x/TaOy/Pd showed STDP
RSM can be classified into filamentary- and interface-type learning.16 In this artificial synapse, the dynamics of filament
devices.85 Filamentary-type RSM is operated by the formation formation led to LTP, whereas the dynamics of local tempera-
and rupture of localized conductive filaments that are ture led to STP (Fig. 3g). The pre- and post-synaptic spikes each
composed of chains of oxygen vacancies or metal ions.86,87 had two parts: a high voltage with a short duration was used as
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Fig. 3 Artificial synapses composed of inorganic materials. (a) Schematic illustration of a memristor device used as an artificial synapse. (b) Measured and
calculated I–V characteristics of the memristor. Inset: Extracted and calculated values of the normalized Ag front position (w) for positive voltage sweep.
(c) Potentiation and depression characteristics of the artificial synapse. Reproduced with permission.14 Copyright 2010, American Chemical Society.
(d) PPF characteristics in a WOx-based memristor with different pulse intervals. (e) Measured (square) and simulated (line) PPF ratios with different pulse
intervals. (f) Measured (square) and simulated (line) changes in current with different pulse frequencies. Reproduced with permission.15 Copyright 2015,
John Wiley & Sons, Inc. (g) Schematic illustration of second-order memristor operation. (h) Simulated (lines) and measured (symbols) STDP
characteristics in the second-order memristor. (i) Simulation results of internal temperature and device conductance evolution with a pair of spikes.
Reproduced with permission.16 Copyright 2015, American Chemical Society.
a programming element, and a low voltage with a long duration of 5 ms.66 Pre-synaptic spikes had an amplitude of 1.2 V, and
was used as a heating element. When the low voltage with a post-synaptic spikes had an amplitude of 0.8 V. The firing rate
long duration was applied, the local temperature of the device of the post-synaptic spikes was modulated from 10 kHz to
increased but the conductance was not changed. The local 83 kHz, whereas that of the pre-synaptic spikes was fixed at
temperature spontaneously decayed after the pulses ceased. 50 kHz. If the post-synaptic spike frequency exceeded f0 = 50 Hz,
Filament growth can be enhanced by elevated local temperature. the synaptic weight increased; i.e., the synaptic strength
Because of these internal short-term dynamics, STDP learning increased. By contrast, at f0 o 50 Hz, the synaptic weight
rules were implemented without using a complex programming decreased, so the synaptic strength was weakened.
voltage waveform (Fig. 3h). A pre-synaptic spike caused a Also, RSM devices were investigated to emulate hetero-
temporary increase in temperature, so when a post-synaptic synaptic plasticity.78,101,102 A nanoscale multi-terminal memristor
spike arrived Dt later, the filament growth was enhanced. As Dt device that exploited self-organization of Ag nanoclusters was
decreased, the local temperature increased (Fig. 3i). The sign of proposed to realize heterosynaptic plasticity.78 Heterosynaptic
conductance change depended on the final spike, and the plasticity was implemented in a multi-terminal device that
amount of the conductance change depended on Dt. The included another modulatory terminal to regulate the synaptic
short-term dynamics of local temperature is similar to Ca2+ plasticity between the pre- and post-synaptic neurons. The
dynamics in a biological synapse. The conductance change in number of pulses to reach a certain facilitation level (i.e.,
STDP was a result of the modulation of the conductive filament increase in synaptic weight by a factor of 100) was changed
size, which was a result of the combination of long-term and depending on the voltage amplitude of the applied modulatory
short-term dynamics. Rate-dependent synaptic characteristics input. The modulatory terminal affected the facilitation and
were achieved using an electronic synapse composed of AgInSbTe depression of the synapse between the pre- and post-synaptic
by applying triangular pulses with rising and falling times neurons. Although inorganic artificial synapses that exploited
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resistive switching behavior successfully emulated synaptic synaptic plasticity including potentiation/depression, STP, LTP,
plasticity, they could face the reliability issues due to the STDP, and SRDP. STDP was emulated by applying pulses with
randomness of filament formation. To solve this problem, a precisely-controlled timing to the top and bottom electrodes.
single-crystalline SiGe layer with threading dislocations was Another organic biomimicking memristor was composed of a
introduced as a resistive switching layer.100 In this device, polymer that included triphenylamine-containing polymer
threading dislocations in SiGe were used to confine filament (BTPA-F) and ethyl viologen diperchlorate (EV(ClO4)2).104
growth to a defined location. This confinement improved the BTPA-F composed of a closed ring and sterically-crowded
uniformity, linearity of synaptic weight updates, and retention/ triphenylamine (TPA) group was used for its rich electrochemi-
endurance characteristics of artificial synapses. In simulation, cal redox behavior. EV(ClO4)2 was used as the counter electrode
artificial neural networks based on single-crystalline SiGe resis- and source to supply ClO4 to stabilize the charged form of the
tive switching devices showed 95.1% recognition accuracy of polymer (Fig. 4a). The organic memristor with a Ta/EV(ClO4)2/
28 28 handwritten images in the Modified National Institute BTPA-F/Pt structure showed analogue switching behaviors; the
of Standards and Technology (MNIST) data set. This result is conductivity increased from 0.03 S m 1 to 0.09 S m 1 after
comparable to the recognition accuracy (97%) obtained using consecutive positive voltage sweeps, whereas the conductivity
an ideal device. decreased from 0.25 S m 1 to 0.13 S m 1 after negative voltage
3.1.2. Organic artificial synapses. In addition to inorganic sweeps. The device also emulated SRDP characteristics under
materials, organic materials have been evaluated as artificial application of voltage spikes with frequencies from 1 Hz to
synapses based on resistive switching behaviours.103–110 These 20 Hz. The current was not changed by application of pulses at
materials are considered to be alternatives to conventional 1 Hz, but was enhanced by 30 times by application of pulses at
inorganic semiconductor technology due to their advantages 20 Hz (Fig. 4b). An artificial synapse composed of EV(ClO4)2
such as good material availability, low cost, and the possibility and triphenylamine (TPA-PI) was fabricated on a flexible poly-
of simple solution processes.111–113 Also, the electronic char- ethylene terephthalate (PET) substrate and synaptic functions
acteristics of organic materials can be tuned by molecular were successfully emulated.105 It also showed synaptic poten-
design and control of synthesis strategies.114 Furthermore, these tiation and depression after being bent 100 times to radius
materials are compatible with fabrication by solution processes o10 mm (Fig. 4c). A 3D artificial synapse for use in flexible
including spin coating, dip coating, spray coating, and ink-jet applications was composed of poly-(methylsilsesquioxane)
printing, without need for vacuum-deposition processes.115–118 (pMSSQ) as an active material due to its excellent flexibility
Organic materials are mechanically flexible and ductile, so they have as well as good thermal, chemical, and physical stability.106
potential applications to flexible and wearable devices.105,107,119–122 Cu ions were doped with a concentration gradient into the
An organic material-based artificial synapse composed of a pMSSQ, with a highly-doped layer near the top electrode, and a
PEDOT:PSS sandwiched between Ag and Ta electrodes was weakly-doped layer near the bottom electrode (Fig. 4d). The
reported.103 PEDOT:PSS was chosen as an active layer because conductance change was induced by input signals that drove
its conductivity could be easily controlled. The device emulated the migration of ions. The device showed gradual current
Fig. 4 Artificial synapses composed of organic materials. (a) Schematic structure of an EV(ClO4)2/BTPA-F bilayer artificial synapse and I–V characteristics
showing analogue switching behaviors. (b) Current changes after application of 10 pulses (1 V, 10 ms) at different frequencies. Reproduced with
permission.104 Copyright 2016, John Wiley & Sons, Inc. (c) Synaptic potentiation and depression characteristics under bent conditions with different
curvature radii. Reproduced with permission.105 Copyright 2016, The Royal Society of Chemistry. (d) Schematic illustration of three-dimensional artificial
synapses. (e) Synaptic weight change with the interval between pre- and post-spikes. Reproduced with permission.106 Copyright 2017, Springer Nature.
(f) Schematic illustration of pV3D3-based polymer memristors. (g) Potentiation and depression characteristics with incremental pulse trains for
potentiation (2 to 4 V, 60 ns) and depression ( 1.2 to 1.4 V, 100 ns). Reproduced with permission.107 Copyright 2019, American Chemical Society.
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change for set and reset processes, long-term potentiation/ biocompatible, and flexible. They have been evaluated for use
depression, and PPF characteristics. STDP characteristics were in artificial synapses and have shown potential for application
achieved by application of pre- and post-spikes to the pre- and in neuromorphic systems.18,68,125–127
post-synapses, respectively. Each spike consisted of a positive Lignin is an amorphous polymer material and is a compo-
pulse (2 V, 0.1 ms), followed by a negative pulse ( 1 V, 0.3 ms). nent of wood.125 Lignin has high carbon content; heat can
STDP was emulated by controlling Dt between pre- and post- transform it to an amorphous or a graphite structure, and thus
spikes (Fig. 4e); this result proved that the 3D structure could change its electrical conductivity; this change can be exploited
be used as an artificial synapse. An analogue memristive in artificial synapses. Also, lignin can be easily formed into thin
synapse was composed of poly(1,3,5-trivinyl-1,3,5-trimethyl- films by a simple and inexpensive solution process. An artificial
cyclotrisiloxane) (pV3D3) polymer, which was used as an active synapse made of lignin showed synaptic plasticity by reversible
layer (Fig. 4f).107 The pV3D3 layer was deposited using initiated transformation from an amorphous carbon matrix to localized
chemical-vapor deposition. The structure of Cu/pV3D3/Al mem- graphitic structures in response to application of electrical
ristors achieved gradual conductance change by controlling bias.125 The synaptic device showed analogue switching
the size of conductive filaments. To form a thin filament, ICC behavior. During five consecutive voltage sweeps from 0 V to
was controlled to suppress the high overshoot current, which 0.7 V, the current increased after each sweep, whereas during
could cause the unintentional formation of a thick filament. reverse voltage sweeps from 0 V to 0.7 V, the current decreased
A gradual increase in ICC changed the reset behavior of the after each sweep (Fig. 5a). Potentiation was emulated by
polymer-based device from abrupt to gradual switching char- applying consecutive negative pulses, and depression was
acteristics. The device emulated potentiation and depression emulated by applying consecutive positive pulses. SRDP
characteristics under application of incremental pulse trains characteristics were emulated by applying pulse trains with
for potentiation (2 to 4 V, 60 ns) and depression ( 1.2 to 1.4 V, different Dt from 100 ms to 10 s. The current increased as Dt
100 ns) (Fig. 4g). Also, simulation was conducted to confirm decreased. A lignin-based artificial synapse on a flexible PET
the applicability of artificial neural networks that used the substrate showed mechanical flexibility with good bending
organic material-based artificial synapses. Memristive synapses tolerance. Another artificial synaptic device was composed of
based on pV3D3 polymers were used for face classification.107 collagen that could be extracted from fish skin and fabricated
The simulation was performed in artificial neural networks on the flexible PET substrate.68 A Mg/collagen layer/ITO struc-
designed with crossbar architecture with 32 32 input neurons, ture emulated various synaptic functions such as analogue
10 middle neurons, and 3 output neurons. In the simulations, memory under continuous voltage sweeps, and potentiation/
the faces of two persons were classified with an average recogni- depression characteristics under 200 consecutive pulses. The
tion rate of 88% after 24 epochs of training. increase in current during the set process occurred due to the
3.1.3. Biomaterial-based artificial synapses. Among the gradual increase of ion concentration, whereas the gradual
organic materials, biomaterials obtained from organisms have decrease of the current level was a result of the progressive
been evaluated as alternative organic materials.123,124 Biomaterials expansion of the Mg-depleted region by diffusion during
are abundant, simple to extract, environmentally benign, the reset process. STDP behavior was emulated by applying a
Fig. 5 Biomaterial-based artificial synapses. (a) Chemical structure of lignin extracted from wood, and analogue switching behaviours during
5 consecutive negative and positive voltage sweeps. Reproduced with permission.125 Copyright 2017, American Chemical Society. (b) STDP characteristics
of a Mg/collagen/ITO artificial synaptic device. Reproduced with permission.68 Copyright 2018, John Wiley & Sons, Inc. (c) Short-term to long-term plasticity
transition depending on the number of applied pulses. (d) Memorization of two images using artificial synapses composed of i-carrageenan. Letters ‘‘P’’ and
‘‘T’’ are memorized on 5 5 arrays by applying 10 pulses with low frequency for letter ‘‘P’’ and 30 pulses with high frequency for letter ‘‘T’’. Reproduced with
permission.18 Copyright 2018, American Chemical Society.
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positive pulse (2 V, 10 ms) then a negative pulse ( 3 V, 10 ms) grown from the Ag electrode to the FTO electrode by repeated
to both the pre- and post-synaptic parts of the artificial synapse. application of a low voltage, which led to a decrease in the
Long-term potentiation and depression were observed in effective gap between the two electrodes and allowed analogue
response to Dt between a pair of pulses; a large change in resistive switching behaviors. An artificial synapse that used HP
synaptic plasticity was observed at short Dt (Fig. 5b). The device in an Al/CH3NH3PbBr3/buffer-capped conducting polymer
also exhibited reliable synaptic characteristics during bending. (BCCP) electrode structure showed synaptic behavior as a result
An artificial synapse was also fabricated using i-carrageenan of ion migration and trapping at the interface between
(i-car), which could be extracted from seaweed.18 The device CH3NH3PbBr3 and BCCP.128 Br ions have lower activation
was constructed in a two-terminal Ag/i-car/Pt structure. When a energy (Ea E 0.2 eV) than CH3NH3+ ions (Ea E 0.8 eV), so
positive voltage was applied to the Ag top electrode, the Br ions migrate more easily than CH3NH3+ ions; therefore,
generated and injected Ag+ ions could migrate toward the synaptic behavior may depend more on the migration of Br
bottom electrode. When they reached the bottom electrode, than CH3NH3+. The perovskite synapse showed analogue
the growth of an Ag filament was initiated by the reduction of switching behavior under voltage sweeps with an increased
Ag+ ions; the device was changed from an insulating state to a range for the set process ( 2 to 7 V) and for the reset process
conductive state by filament formation. However, the Ag fila- (2, 3 V) (Fig. 6a). The artificial synapses emulated PPF char-
ment was unstable, so the device spontaneously relaxed back to acteristics under application of two identical voltage pulses
the initial state when the electrical stimulus ceased. These Ag (Fig. 6b). The artificial synapse emulated STP after application
dynamics were exploited in devices to emulate synaptic plasti- of a low-amplitude pulse, which only moved some ions for a
city in a biological synapse. Repeated stimulation yielded a short distance, so they could return to their initial state after
transition from STM to LTM. Stimuli with different strengths the pulse ended. LTP behavior in a biological synapse was also
yielded a transition from STP to LTP. Weak stimulation by emulated after application of strong or numerous pulses, which
application of 10 pulses induced the formation of only a thin Ag drove the ions far enough that they could be trapped at the
filament, which was spontaneously ruptured after the stimula- CH3NH3PbBr3/BCCP interface, and some could be injected into
tion ceased; this reaction was STP. However, strong stimulation the BCCP layer (Fig. 6c). After the pulses ceased, the ions could
by application of 30 pulses induced the formation of thick Ag drift back to their initial state, but some trapped or injected
filaments, which were maintained after the stimulation ceased; ions remained; these ions led to long-term potentiation of the
this reaction was LTP (Fig. 5c). The ability to emulate change artificial synapse. Memristive synapses were achieved using
from STM to LTM was further demonstrated using a synapse various HP structures (CH3NH3PbBr3, CH(NH2)2PbBr3, CsPbBr3)
array to memorize two images (Fig. 5d). An image of the letter as the active layers.129 The synaptic plasticity was achieved by the
‘P’ was stored using 10 pulses with low frequency, and an image coexistence of ion migration and carrier injection barriers in
of the letter ‘T’ was stored using 30 pulses with high frequency. perovskite films. Optimized pulse schemes yielded emulation of
The image of the letter ‘P’ or ‘T’ was stored at the last stimulus, but STP and LTP characteristics including PPF and STDP.
only the image of ‘T’ was memorized in the array and persisted Two-dimensional (2D) HPs have been introduced as artificial
even after 60 s. These results indicated that by responding to input synapses.137–139 The perovskites have the structure (L)2(SMX3)n+1MX4,
parameters, the i-car synapses could determine which information where L is a long-chain organic cation, S is a short-chain organic
to change from STM to LTM, i.e., how long information should cation, M is a metal cation, and X is a halide anion.137,140 2D
be retained. HPs show anisotropic charge transport (i.e., suppressed in the
3.1.4. Halide perovskite artificial synapses. Various materials out-of-plane direction), which is desirable to achieve an artificial
including inorganic, organic, and biomaterials have been synapse that has low energy consumption.137,141 An artificial
proposed to realize high-performance artificial synapses based synapse composed of a 2D single crystal of (PEA)2PbBr4 per-
on resistive switching behaviors. Recently, halide perovskites ovskite (PEA = phenethylammonium) was proposed.137 These
(HPs) have emerged as promising candidates for use in artificial crystals were synthesized using anti-solvent vapor-assisted
synapses.128–134 HPs show significant hysteresis behavior in their crystallization, then exfoliated into thin layers. The synaptic
current–voltage response due to the migration of defects in the behavior was caused by the formation of partial filaments from
perovskite layer under an electric field.135,136 These behaviors of Br vacancies that were induced by migration of Br ions in
HPs are applicable to artificial synapses. response to electrical pulses. A device that used these layers in a
An HP-based device using CH3NH3PbI3 xClx was proposed graphene/2D perovskite/Au structure showed STP (Fig. 6d) and STP
as an artificial synapse.132 A CH3NH3PbI3 xClx perovskite layer to LTP transition (Fig. 6e) characteristics with an energy consump-
was deposited by a simple solution process. A device that had a tion of 400 fJ per spike. Artificial synapses were also constructed
Ag/CH3NH3PbI3 xClx/FTO structure showed abrupt resistive using 2D and quasi-2D perovskites.139 A (PEA)2MAn 1PbnBr3n+1
switching behavior under sweeps from 0 V to 3 V, but showed perovskite film (MA = methylammonium) was deposited by
analogue resistive switching behavior after positive voltage spin-coating, and the structural dimensionality was controlled
sweeps from 0 V to 0.5 V and negative voltage sweeps from by adjusting the stoichiometric ratio of PEA and MA cations.
0 to 0.5 V. The analogue switching behavior at low voltages The post-synaptic current decreased as the proportion of PEA
occurred because a fully-connected filament between two elec- increased (i.e., as the structural dimensionality of perovskite
trodes could not be formed. The Ag filament was gradually decreased.) (Fig. 6f). EPSC, PPF, STP, and LTP were achieved
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Fig. 6 Emulated synaptic functions using halide perovskite materials. (a) I–V characteristics with consecutive voltage sweeps with increased ranges for
the set process ( 2, 3, 4, 5, 6, 7 V) and for the reset process (2, 3 V). Inset: Schematic structure of an artificial synapse with an Al/CH3NH3PbBr3/
BCCP/ITO structure. (b) PPF characteristics. (c) Long-term potentiation by application of 30 consecutive pulses. Reproduced with permission.128
Copyright 2016, John Wiley & Sons, Inc. (d) Short-term potentiation characteristics of a 2D (PEA)2PbBr4 perovskite-based device. (e) STP-to-LTP
transition. Reproduced with permission.137 Copyright 2017, American Chemical Society. (f) Post-synaptic current with the structural dimensionality of
halide perovskites, (PEA)2(MA)n 1PbnBr3n+1 (n = 1–5, N). Reproduced with permission.139 Copyright 2019, John Wiley & Sons. (g) Schematic illustration of
an Ag/CH3NH3PbI3/Ag device with light illumination. (h) Conductance change of the device under illumination (1.29 mW cm 2). (i) Emulation of long-term
potentiation and depression characteristics with illumination. Reproduced with permission.145 Copyright 2018, American Chemical Society.
with low energy consumption (E0.7 fJ per synaptic event), had these characteristics was simulated using MNIST data
which is similar to biological synapses (1–10 fJ per event).6,142 set in single-layer artificial neural networks composed of 784
HPs have good optical characteristics with small exciton input neurons and 10 output neurons. The artificial synapses
energy and long charge-carrier lifetime, and therefore have showed 81.8% accuracy of pattern recognition after 2000
potential applications to optical devices.143,144 HP-based mem- learning phases.
ristors in which the synaptic function can be adjusted with
optical signals have been demonstrated.145 CH3NH3PbI3 was 3.2. Phase-change memory synapse devices
used as an active layer due to its high optical absorption PCM is another promising candidate for emerging memory
coefficient and low energy barrier for migration of iodine vacan- devices.146,147 A typical PCM device consists of a phase-change
cies. The conductance of the CH3NH3PbI3 film was related to material sandwiched between two metal electrodes. The most-
the increase in the concentration of iodine vacancies under established PCM structure is the so-called mushroom cell
applied electrical bias, then decay in the concentration of iodine (or T-cell) that has a pillar-like heater between the phase-
vacancies after removal of the bias. Illumination increased the change material and the bottom electrode.148 PCM is operated
formation energy of iodine vacancies and delayed the growth of by reversible change between crystalline (low resistance) and
the region that included iodine vacancies. Illumination also amorphous (high resistance) states. For the set process, appli-
accelerated the recombination of iodine vacancies after the cation of a long pulse with a low amplitude induces phase
removal of bias (Fig. 6g). Change in conductance by this process transition from the amorphous to crystalline phase. For
emulated long-term potentiation and long-term depression the reset process, application of a short pulse with a high
(Fig. 6h and i). HP-based artificial synapses have also been amplitude leads to rapid cooling of the material, which leaves
evaluated for application to artificial neural networks. An artifi- a melt-quenched amorphous phase.149 PCM has fast switching
cial synapse with an Ag/CH3NH3PbI3/ITO structure showed long- speed, good endurance, and high scalability, and has therefore
term potentiation and depression characteristics.134 A device that been evaluated for application in emerging nonvolatile memory
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technology.149 PCM cells typically use chalcogenide materials, gradually increased in the contact region between the bottom
such as Ge2Sb2Te5 (GST), GeTe/Sb2Te3, and Ag5In5Sb60Te30.150,151 electrode and phase-change material (Fig. 7b); this transition
Phase-change materials have potential to show analogue yielded numerous intermediate resistance states. The artificial
switching behaviors, and have therefore been used in artificial synapses underwent gradual reset and gradual set process.
synapses.152–154 Various pulse schemes have been proposed to Gradual reset was implemented by an incremental pulse scheme
use phase-change materials for neuromorphic computing, in 2–4 V with a 20 mV step, whereas gradual set was achieved by
because device conductance can be controlled by modulating using a stair-case pulse with a 0.1 V step. 20 pulses were applied
the ratio between amorphous and crystalline states in a PCM for each step (0.5, 0.6, 0.7, 0.8, 0.9 V) (Fig. 7c). STDP character-
cell.19,155 The resistance difference between the amorphous istics were demonstrated in GST by exploiting the thermal
and crystalline states in phase-change materials has potential accumulation effect.20 To realize STDP, square pulses were
in artificial synapses. applied as pre-synaptic and post-synaptic spikes to a two-
An artificial synapse that used a phase-change material was terminal device (Fig. 7d). Dt between the spikes was adjusted
fabricated using GST and a tungsten bottom electrode with a to control the heat accumulation, so the artificial synapses
75 nm diameter.19 Continuous resistance transitions in the showed different degrees of crystallization in the GST. As a
phase-change material were exploited to emulate the analogue result, several resistance states were achieved (Fig. 7e). Also, an
characteristics of a biological synapse. The PCM cell was artificial synapse that used PCM was evaluated for application to
observed in a fully-set state, a partially-reset state, and a fully- artificial neural networks.156 Artificial synapses that used PCM
reset state (Fig. 7a). In the fully-set state (500 O), the GST layer were fabricated using GST, then integrated into a prototype chip
was polycrystalline. During the transition from the set to reset in a 90 nm CMOS technology. To apply the synaptic devices to
state, the amorphous phase expanded from the contact region artificial neural networks, classification of hand-written digits in
between the phase-change material and the bottom electrode. the MNIST database was simulated using a multi-memristive
In the partially-reset state (200 kO), which was achieved by synapse architecture in which a synaptic weight was represented
applying a low amplitude of a reset pulse, small amorphous by the combined conductance of multiple devices. The simula-
regions was formed, and in the fully-reset state (2 MO), tion results showed that classification accuracy could be
the amorphous region covered the bottom electrode. Finite improved by increasing the number of devices per synapse; the
element simulation suggested that the amorphous region accuracy reached B90% in artificial neural networks.
Fig. 7 Artificial synapse that uses phase-change memory. (a) Cross-sectional TEM images of phase transition from a fully-set state to a partially-reset state
with a small amorphous region, and a fully-reset state of the artificial synapse using GST. The inset of the fully reset state shows a diffraction pattern in the
amorphous region. (b) COMSOL simulation of transition from the set to reset states. The colors represent the temperature distribution across the cell with
reset voltages from 0.7 V to 0.9 V in increments of 0.05 V. (c) Gradual reset and set behaviors. Gradual reset is implemented by an incremental pulse scheme
in 2–4 V in increments of 20 mV, whereas gradual set is achieved by using a stair-case pulse in increments of 0.1 V. 20 pulses are applied for each step (0.5,
0.6, 0.7, 0.8, 0.9 V). Reproduced with permission.19 Copyright 2012, American Chemical Society. (d) Implementation of STDP in the artificial synapse.
(e) ANSYS simulation of the temperature development with time interval.20 Reproduced with permission. Copyright 2015, John Wiley & Sons.
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3.3. Ferroelectric synapse devices in the ferroelectric layer was modulated by applying voltage
Ferroelectric devices have been introduced as artificial synapses pulses with different amplitudes and durations. Control of the
due to their fast operation speed, low power consumption, and maximum voltage pulse amplitude yielded distinct loops of
analogue memory characteristics.23,26,27 Ferroelectric materials resistance hysteresis (Fig. 8b). Application of different voltage
have spontaneous polarization, which can be switched by applying waveforms evoked asymmetric and symmetric STDP learning
rules, depending on the voltage waveform (Fig. 8c and d).
an electric field, then maintained even without an external electric

field.157 The switching of spontaneous polarization can be pre- However, these epitaxial ferroelectric films were deposited at
cisely adjusted by controlling the condition of the applied high temperature, so their use in practical applications could
pules.158–160 By using these characteristics, ferroelectric devices be limited. Use of hafnium oxide-based ferroelectric materials
such as ferroelectric tunnel junction synapses and ferroelectric may solve this problem.24,164–166 Hf0.5Zr0.5O2 (HZO) was used as
synaptic transistors have been introduced to implement analogue a ferroelectric layer deposited by atomic layer deposition for an
memory characteristics to mimic synaptic plasticity. In this FTJ (Fig. 8e).24 This FTJ has advantages of low fabrication cost,
section, these ferroelectric synaptic devices are reviewed. good scalability, and compatibility with the present CMOS
3.3.1. Ferroelectric tunnel junctions. Ferroelectric tunnel technology. In this device, the tunneling resistance was modulated
junctions (FTJs) have been considered as promising memory by applying pulses with incremental write voltage amplitudes
devices for neuromorphic applications.23–27 An FTJ is composed (Fig. 8f). The effective polarization in the barrier increased with
of an ultrathin ferroelectric layer sandwiched between two increase in write voltage amplitude, so the conductance ratio also
electrodes.161,162 The ferroelectric layer should be thin enough increased with increase in write voltage amplitude. By exploiting
to permit the tunneling of electrons, but thick enough to these characteristics, potentiation and depression characteristics
guarantee ferroelectric polarization characteristics. In an FTJ, were demonstrated in this FTJ (Fig. 8g). In the potentiation and
the polarization switching of the ferroelectric layer induces a depression processes, the energy consumption was B1.8 pJ per
change in tunneling resistance because the potential profile in spike. STDP characteristics were emulated by applying a pre-spike
the tunnel barrier can be changed by asymmetric polarization to the top electrode, and a post-spike to the bottom electrode.
screening at the interface between the ferroelectric layer and When the pre-spike reached the device earlier than the post-spike
electrode.163 As artificial synapses, FTJ devices have been (Dt 4 0), the conductance of the FTJ increased (Fig. 8h). When the
demonstrated using epitaxial ferroelectric films.23,25–27 post-spike preceded the pre-spike (Dt o 0), the conductance
Synaptic FTJ devices were fabricated using BiFeO3/ of the FTJ decreased. As the magnitude of Dt decreased, the
Ca0.96Ce0.04MnO3 epitaxial thin films (Fig. 8a).23 The polarization magnitude of the conductance changes increased. To estimate
Fig. 8 Artificial synapse that uses a ferroelectric tunnel junction (FTJ). (a) Schematic illustration of a synaptic FTJ device based on BiFeO3 (BFO)/
Ca0.96Ce0.04MnO3 (CCMO). (b) Multiple resistance hysteresis loops as a function of maximum voltage pulse amplitudes. (c) Asymmetric and (d) symmetric
STDP learning rules demonstrated using the synaptic FJT device. Reproduced with permission.23 Copyright 2017, Springer Nature. (e) Schematic
illustration of a synaptic FTJ device with ferroelectric Hf0.5Zr0.5O (HZO). (f) Hysteretic variation of tunneling resistance in the HZO-based FTJ device.
(g) Potentiation and depression characteristics of the FTJ based on HZO. (h) Asymmetric STDP learning rules of the synaptic FTJ with HZO. Reproduced
with permission.24 Copyright 2018, The Royal Society of Chemistry.
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the ability of the artificial neural networks based on an HZO were retained for 104 s (Fig. 9c). Potentiation and depression
FTJ, a simulation of pattern classification and recognition was characteristics were implemented by exploiting these conduc-
performed. In the simulation, the recognition accuracy of 16 tance–modulation properties (Fig. 9d). The ferroelectric
16-pixel black-and-white images was 496%. transistor composed of HfZrOx and IGZO showed potentiation
3.3.2. Ferroelectric transistors. Ferroelectric transistors have and depression characteristics, and had the advantages of highly
advantages of nondestructive read-out, low-power consumption, linear response, multiple states, and small variations.35,177 To
and fast operation.167–174 A ferroelectric transistor is composed verify the utility of these synaptic characteristics, artificial neural
of a ferroelectric layer and a semiconductor. The key compo- networks based on the ferroelectric transistor were simulated.
nents of ferroelectric transistors are ferroelectric materials that In the simulations, these artificial neural networks achieved
have spontaneous polarization characteristics. The carrier 91.1% recognition accuracy of 20 20 hand-written digits
concentration of the semiconductor can be controlled by the in the MNIST database.35 Ferroelectric transistors have been
ferroelectric layer because the charge at the interface between evaluated to realize STDP learning rules, which are also
the semiconductor and ferroelectric layer can be depleted or important synaptic characteristics.29,158,159,178,179 A ferroelectric
accumulated, depending on the polarization state of the ferro- synaptic transistor was composed of oxide materials with a
electric layer.175,176 Therefore, the channel conductance can be ZnO/Pr(Zr,Ti)O3(PZT)/SrRuO3 structure (Fig. 9e).159 The channel
modulated by the polarization states of the ferroelectric layer. conductance was modulated by the polarization states of PZT,
Ferroelectric transistors based on hafnium oxide have non- which could be controlled by applying a gate voltage with an
volatile spontaneous polarization and multi-level conductance appropriate amplitude and duration. This ferroelectric transistor
characteristics that can be exploited to obtain analogue memory showed STDP learning functions in response to a non-linear gate
properties, which are essential in synaptic devices.28,29,31,33 voltage pulse, which was generated using a sampling circuit to
A ferroelectric synaptic transistor was proposed using zirconium- produce two pulses that corresponded to the spikes from the
doped hafnium oxide (HfZrOx) as the ferroelectric layer and pre- and post-neurons (Fig. 9f). However, although STDP char-
indium gallium zinc oxide (IGZO) as the semiconductor layer acteristics were realized, the need for a sampling circuit could
(Fig. 9a).35 To achieve multi-level conductance characteristics, increase the complexity of neuromorphic systems. Furthermore,
the polarization state was gradually changed by controlling the oxide-based ferroelectric materials require a high process
amplitude of the applied bias (Fig. 9b). The polarization state in temperature, so they have limited applications in flexible elec-
the ferroelectric layer was changed from downward to upward tronics. Organic ferroelectric materials can be synthesized or
polarization as the amplitudes of the bias pulse increased. As the deposited at low temperature, so they have potential applications
upward polarization increased, the conductance of the channel to flexible and wearable electronics.121,169,171–173,180 An organic
layer increased due to electron accumulation in the interface ferroelectric transistor composed of a P(VDF-TrFE) ferroelectric
region.176 Multi-level conductance characteristics were demon- layer and MoS2 semiconductor was proposed (Fig. 9g).180 This
strated by gradual change in polarization; 4 conductance levels device showed conductance–modulation characteristics with
Fig. 9 Artificial synapse that uses a ferroelectric transistor. (a) Schematic image of a ferroelectric transistor based on HfZrOx and IGZO. (b) Schematic
diagram of changes in the polarization of the ferroelectric layer in response to amplitudes of applied bias. (c) Multi-level data storage characteristics of the
ferroelectric transistor based on HfZrOx. (d) Potentiation and depression characteristics of the synaptic ferroelectric transistor. Reproduced with
permission.35 Copyright 2019, American Chemical Society. (e) Schematic illustration of a synaptic ferroelectric transistor based on ZnO/Pr(Zr,Ti)O3 (PZT)
with upward and downward polarization. (f) STDP learning function in the synaptic ferroelectric transistor based on ZnO and PZT. Reproduced with
permission.159 Copyright 2012, American Institute of Physics. (g) Schematic device structure of a ferroelectric transistor based on P(VDF-TrFE) and MoS2.
(h) Demonstrated STDP learning rules in the organic ferroelectric transistor. Reproduced with permission.180 Copyright 2019, John Wiley & Sons, Inc.
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1000 intermediate states. To demonstrate STDP learning, the dielectric materials.39,40,183 Electrochemical devices are operated
spikes from the pre- and post-synaptic neurons were emulated by by controlling the device conductance.36,41 The device conduc-
using pulses with waveforms that included rectangular voltage tance is modulated by application of a signal to the gate
pulses followed by smooth slopes of opposite polarity. When both electrode; as a consequence, the mobile ions in the electrolyte
pre- and post-synaptic spikes were applied to the device with move to the channel and are injected into the channel layer, and
time interval Dt, the conductance of the ferroelectric transistor thus change its doping level, which induces a change in
increased at Dt 4 0, but decreased at Dt o 0 (Fig. 9h). This device conductance.41,184 One advantage of electrochemical artificial
had an ultralow energy consumption o1 fJ per synaptic opera- synapse devices is that the programming and storage mechan-
tion, which is equivalent to that of a biological synapse.6 isms are decoupled, so low switching energy and good retention
can be achieved.36 Conventional memory devices show the same
3.4. Electrochemical artificial synapses barrier heights for write and read operations; this trait imposes a
In addition to using emerging memory device technologies tradeoff between low energy consumption and good retention
such as RSM and PSM for artificial synapses, researchers time (Fig. 10a).36 However, in electrochemical artificial synapse
have proposed new materials and device structures to achieve devices, the programming and retention barriers are decoupled
artificial synapses with high-performance synaptic behaviors. by using a circuit switch (Fig. 10b). During the write operation,
Electrochemical devices that are operated by controlling the the switch is closed, so ions and electrons can be exchanged at
movement of ions have been evaluated as artificial synapses small bias, whereas the switch is open for the read operation,
due to their advantages including linear/symmetric conduc- which suppresses the electrochemical reactions; thus the device
tance change and low switching energy.36,38,39,41,42,181,182 These can maintain the stored state. These processes can achieve both
artificial synapses require a three-terminal structure with low-power operation and good retention. To investigate the
source/drain/gate electrodes and electrolyte. Electrolytes with electrochemical device, various materials and structures have
mobile ions like Li+, H+, and O2 have been used as gate been evaluated.36,38,39,43,185
Fig. 10 Electrochemical artificial synapses. (a) Schematic illustrations of energy barriers for conventional memory devices (FRAM, MRAM, flash memory,
and PCM) and (b) an electrochemical synaptic device. Reproduced with permission.36 Copyright 2018, John Wiley & Sons. (c) PPF and PTP characteristics
of a WO3-based artificial synapse. Reproduced with permission.37 Copyright 2018, John Wiley & Sons. (d) High-angle annular dark-field scanning-
transmission electron microscope (HAADF-STEM) image of brownmillerite SrCoO2.5 and perovskite SrCoO3 d. (e) Percentages of conductance change
by applying gate voltage pulses. Reproduced with permission.183 Copyright 2019, John Wiley & Sons. (f) Schematic illustration of Li-ion based synaptic
transistors. (g) Gradual conductance change of the devices using consecutive current pulses. (h) Projected energy consumption with scaling down of the
synaptic device. Reproduced with permission.38 Copyright 2017, John Wiley & Sons.
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An electrochemical device was proposed using a tungsten mobile ions.40,185 2D van der Waals (vdW) layered crystals
oxide (WO3) thin film and an ionic liquid.37 WO3 was chosen as including WSe2, NiPS3, and FePSe3 were used in synaptic
the channel material because it is a pseudo-perovskite oxide in transistors (Fig. 11a).40 Incorporation of lithium ions into the
which the A-site cation is absent; this absence allowed inter- channel layer led to an ionic gating effect, which shifted the
calation and extraction of mobile ions from the WO3 layer. STP Fermi level upward to the conduction band, and synaptic
was realized by ion dynamics in electrolyte under low electrical behavior could be achieved by incorporation of lithium ions
bias, whereas LTP was achieved by proton insertion into the into the channel layer; STP occurred when lithium ions were
absent A-site of WO3 at high electrical bias. The artificial adsorbed to the surface of channel layer, whereas LTP occurred
synapse emulated PPF and post-tetanic potentiation (PTP), when they were intercalated into the vdW materials. STP was
which are phenomena in which EPSCs are evoked by the second emulated when a voltage spike (5 V, 50 ms) was applied and the
and the tenth pulse, respectively (Fig. 10c).37,186 They act to STP was changed to LTP by applying successive trains of voltage
decode temporal information in auditory or visual signals.37,187 pulses (Fig. 11b). Also, these electrochemical reactions pro-
Electrochemical synaptic transistors composed of SrCoOx films vided STP and LTP with an energy consumption of 30 fJ per
with ionic liquids were proposed.183 The brownmillerite SrCoO2.5 synaptic event. Graphene has been used in an electrochemical
structure consisting of alternating [CoO4]-tetrahedral and [CoO6]- device for an artificial synapse.36 Lithium ions were chosen as
octahedral layers with oxygen vacancy channels allowed insertion the guest ions for the graphene channel layer because they
and extraction of oxygen ions. The insertion and extraction of could diffuse rapidly into the bilayer graphene at room tem-
oxygen ions by electrolyte gating caused a reversible phase perature. The synaptic weight of graphene was controlled by the
transformation between brownmillerite SrCoO2.5 and perovskite concentration of lithium ions in the graphene layers. Reversible
SrCoO3 d, with consequent change in conductance (Fig. 10d); this electrochemical intercalation yielded analogue tunability of the
change could realize the emulation of synaptic functions and channel conductance with 250 nonvolatile states and endurance for
multilevel conduction by application of gate voltage pulses 500 cycles with small cycle-to-cycle variations. STDP was obtained
(Fig. 10e). Artificial synapses that use lithium ions have been by adjusting the time difference between two intercalation-
proposed.38,184,188 A proposed synaptic transistor that used programming-pulse schemes (Fig. 11c).
lithium ions was composed of a LiCoO2 channel layer and LiPON A quasi-2D a-phase molybdenum oxide (a-MoO3) could
as a solid electrolyte (Fig. 10f).38 Reversible intercalation of emulate an artificial synapse.185 Ultrathin a-MoO3 nanoflakes
lithium dopants into a LiCoO2 channel induced resistance change were deposited on a substrate by mechanical exfoliation of an
behavior without large structural transformations such as the a-MoO3 single crystal that was synthesized by vapor-phase
formation of filaments or amorphous-to-crystalline phase change. transport. The channel conductance was modulated by electro-
Lithium intercalation into the channel layer yielded tunable chemical proton doping of a-MoO3. Reversible and nonvolatile
channel conductance with a linear response to an application of conductance change yielded synaptic functions including EPSC,
current pulses (Fig. 10g). The switching energy of this transistor PPF, and potentiation/depression characteristics. All-solid-state
was 1 fJ per synaptic event and could be reduced to o10 aJ by electrochemical synaptic transistors were achieved using 2D
device scaling down (Fig. 10h). Another electrochemical artificial a-MoO3 nanosheets and lithium-ion-doped PEO.41 Large
synapse was proposed using a layered SnS2-reduced graphene hysteresis behavior was observed, with a conductance change
oxide (rGO) composite with sodium-doped polyethylene oxide ratio of E1700% in ID–VG curves (Fig. 11d). The behavior might
(PEO) electrolyte.43 This artificial synapse was operated by rever- be a result of lithium ion intercalation in the MoO3 nanosheets;
sible insertion and extraction of sodium ions into SnS2. A Nafion this process yielded free electron carriers because intercalated
film was used as a physical barrier between the SnS2–rGO lithium ions reacted as dopants in the MoO3. The synaptic
composite channel layer and electrolyte to prevent inserted transistors using the reversible lithium ion intercalation process
sodium ions in SnS2 from returning to their initial position to showed linear and symmetric weight updates with a low channel
neutralize the charge gradient. The synaptic transistor showed conductance (Fig. 11e). The electrochemical device was investi-
STP and LTP. In addition, the spatiotemporal characteristics of gated using simulation to confirm the possible application to
nervous systems were emulated using multi-gate inputs. Organic artificial neural networks. The artificial synapse using a-MoO3
materials can also be used as channel layers of an electrochemical nanosheets showed long-term potentiation and depression by
artificial synapse.39 It was implemented using a pre-synaptic application of pulses.41 A simulated neural network that had
electrode composed of poly(3,4-ethylene-dioxythiophene):poly- these characteristics in a crossbar array structure showed 94.1%
styrene sulfonate (PEDOT:PSS), and a post-synaptic electrode recognition accuracy of hand-written digits.
composed of PEDOT:PSS/poly(ethylenimine) (PEI). The synaptic
behaviors were induced by applying a voltage pulse to insert or 3.5. Floating-gate transistors
extract protons from the channel layer. The synapse device A floating-gate transistor is composed of a tunneling oxide, a
exhibited 4500 nonvolatile states and a low energy consump- floating gate, a blocking oxide, and a control gate.189 Conven-
tion of B10 pJ. tional field-effect transistors have a fixed threshold voltage at a
2D materials have been introduced as electrochemical-based constant drain voltage. However, floating-gate transistors can
artificial synapses because of their interlayer spacing, which store charges in floating gates. Programming operations store
can be a preferred site for electrochemical intercalation of electrons in the floating gate and erase operations move them
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Fig. 11 Electrochemical synapse based on 2D materials. (a) Schematic illustration of the synaptic transistor based on WSe2. (b) STP and LTP
characteristics with the number of applied pulses (5 V, 50 ms). Reproduced with permission.40 Copyright 2018, John Wiley & Sons. (c) Change in
resistance with the time difference of a graphene-based artificial synapse. Reproduced with permission.36 Copyright 2018, John Wiley & Sons. (d) Change
in current with gate voltage sweep ( 1.5 V to 1.5 V). (e) Continuous change in analogue channel conductance with 50 repeated positive voltage pulses
(2.5 V, 10 ms) and 50 repeated negative voltage pulses ( 2.5 V, 10 ms). Reproduced with permission.41 Copyright 2018, John Wiley & Sons.
back to the substrate. The channel conductance depends on indicate that large DG could improve the recognition accuracy.
whether or not the charge carriers are stored in the floating The symmetry and linearity of potentiation and depression
gate, so programming and erase operations can change the characteristics are important synaptic properties.3,194 Therefore,
threshold voltages.190 Also, the number of charge carriers researchers have attempted to improve the linearity of the
stored in the floating gate can be controlled by a gate-voltage responses of synaptic floating-gate transistors. A synaptic
pulse.191,192 By exploiting these characteristics, analogue floating-gate transistor with a double floating gate structure
memory characteristics for artificial synapses can be achieved was suggested to improve the linearity of potentiation and
in floating-gate transistors. depression properties.45 This device was composed of double
Floating-gate transistors have been evaluated as synaptic floating gates with stacking MoS2/hexagonal boron nitride
devices.44–47,193 A synaptic floating-gate transistor was proposed (hBN)/MoS2 layers on hBN/Au layers. For comparison, a single-
using a semiconducting carbon-nanotube channel and a gold floating-gate device with a MoS2/hBN/MoS2 stack on an hBN layer
floating gate (Fig. 12a).44 A thin film of Au was used as a floating was also used (Fig. 12d). The device with double floating
gate to control both the linearity and dynamic range DG, which is gates showed more symmetric and linear potentiation/depression
the ratio of the maximum to minimum conductance. In this characteristics than the synaptic floating-gate transistor with a
device, the conductance of the carbon-nanotube channel was single floating gate. When negative voltage pulses were applied to
controlled by the number of trapped charges at the Au floating the gate electrode, the conductance increased steadily in the
gate. The number of trapped charges was adjusted by the device with double floating gates, but more slowly in the device
polarity and amplitude of the gate voltage pulse. Potentiation with the single floating gate. Furthermore, when the positive
and depression properties were realized by exploiting these voltage pulse was applied, the conductance of the device with
characteristics. The nonlinearity and total DG of potentiation/ double floating gates decreased linearly, whereas the conductance
depression characteristics were controlled by the amplitude of of the device with a single gate decreased nonlinearly (Fig. 12e
the applied gate voltage pulse. Application of a gate voltage pulse and f). The improved synaptic properties were attributed to the
with a high amplitude to the synaptic floating-gate transistor device structure with double floating gates. For the device with
yielded a high nonlinearity of 0.82 and DG of 57.5 (case 1) double floating gates, electron transfers could occur between the
(Fig. 12b). When the amplitude of the gate voltage was reduced, floating gate MoS2 and the channel MoS2, as well as between
the nonlinearity was reduced to 0.59, but DG was reduced to 9.4 the floating gate MoS2 and Au. Therefore, the stored charge in the
(case 2) (Fig. 12c). In pattern recognition simulation using case-1 MoS2 floating gate might saturate more slowly in a device with
devices, the carbon nanotube synaptic floating-gate transistor double floating gates than in a device with a single floating gate.
showed an approximately 70% recognition rate using 28 28 The results suggested that precisely-controlled electron tunnel-
MNIST images. The recognition rate was lower in pattern ing and injection could improve the linearity of potentiation
recognition simulation using case-2 devices. These results and depression properties.
View Article Online

Fig. 12 Artificial synapse that uses a floating-gate transistor. (a) Schematic image of a synaptic floating-gate transistor that uses carbon nanotubes (CNT)
and an Au floating gate. Potentiation and depression characteristics demonstrated by applying gate voltages with amplitudes of (b) 8 V and (c) 6 V.
Reproduced with permission.44 Copyright 2017, American Chemical Society. (d) Device structure of a MoS2-based floating-gate transistor with a single
floating gate and double floating gates. Potentiation and depression characteristics of (e) a single-floating-gate transistor and (f) a double-floating-gate
transistor. Reproduced with permission.45 Copyright 2018, American Chemical Society.
4. Summary and outlook

that result from their switching mechanism, so these charac-
Brain-inspired neuromorphic computing has the potential in teristics can reduce the recognition accuracy. Also, RSM devices
next-generation computing systems. For signal transmission, that entail filament formation show abrupt resistance change
memory, and learning functions, biological neural networks are during the set process. This phenomenon causes asymmetric
operated with analogue changes that are induced by synaptic and nonlinear responses, which can limit the recognition
plasticity; this paradigm is distinct from conventional comput- accuracy in artificial neural networks. PCM devices have been
ing systems that use binary operation with ‘‘0’’ and ‘‘1’’ for proposed as artificial synapses due to their fast switching, good
computation. To emulate the structure and function of bio- endurance, and high device density. However, they require high
logical neural networks for new computing systems, various reset power, and use a quench-melting process that causes
materials and structures have been evaluated. This paper large variations in electrical characteristics; these problems
reviewed recent advances in application of emerging memory need to be solved before PCM can be used in artificial synapses.
devices to artificial synapses. Devices that use ferroelectric materials have favorable charac-
RSM devices have been considered as artificial synapses due teristics for artificial synapses, such as linear and symmetric
to their advantages including their simple two-terminal struc- synaptic weight updates, large dynamic ranges, fast operation
ture, good scalability, and compatibility with CMOS processes. speed, and small cycle-to-cycle variations. However, when ferro-
Various materials and structures have been evaluated to emu- electric synaptic devices are scaled down, the number of
late synapses. Inorganic metal-oxides have been widely used for domains that are included in the ferroelectric layer decreases,
RSM. Organic materials have also been introduced as artificial so the analogue memory characteristics may be difficult to
synapses. The organic materials can be easily formed at low maintain. Therefore, future research may be required to imple-
cost. Also, they have mechanical flexibility and ductility, which ment high-density integrated neuromorphic hardware that uses
enable applications as flexible and wearable devices. Biomater- ferroelectric synaptic devices. Devices that use electrochemical
ials have also been evaluated as artificial synapses. These reaction have considerable advantages. The devices show linear
materials can be deposited as thin films by a simple solution and symmetric conductance changes, which lead to high
process, and are environmentally benign. Recently, HP materi- accuracy for pattern recognition. However, devices that exploit
als have emerged as artificial synapses that exploit the hyster- ion migration show relatively slow operation speed compared
esis in the I–V curves and have been used to emulate synaptic to other emerging devices. Also, highly-reactive ions (e.g., Li+)
functions. Also, the exceptional optical and electrical character- can be a problem in CMOS process compatibility. Floating-gate
istics of HPs enable their application to optical synapses. transistor devices have controllable and reliable conductance
Artificial synapses that exploit RSM have been greatly states with a high on/off ratio, which is advantageous for
improved, but have some issues that limit their use in neuro- long-term potentiation and depression. However, floating-gate
morphic systems. RSM devices have stochastic characteristics transistor devices consume high power due to their high
View Article Online
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18 M.-K. Kim and J.-S. Lee, ACS Nano, 2018, 12, 1680–1687.
There are no conflicts to declare. 19 D. Kuzum, R. G. D. Jeyasingh, B. Lee and H. S. P. Wong,
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20 Y. Zhong, Y. Li, L. Xu and X. Miao, Phys. Status Solidi RRL,
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This research was supported by the National Research Foundation 21 M. Suri, O. Bichler, D. Querlioz, O. Cueto, L. Perniola,
of Korea (NRF-2016M3D1A1027665 and 2019R1A2C2084114). This V. Sousa, D. Vuillaume, C. Gamrat and B. DeSalvo, 2011
work was also supported by the Industrial Strategic Technology International Electron Devices Meeting, 2011, pp. 4.4.1–4.4.4,
Development Program (20003968) funded by the Ministry of DOI: 10.1109/IEDM.2011.6131488.
Trade, Industry & Energy (MOTIE, Korea). In addition, this work 22 M. Suri, O. Bichler, D. Querlioz, B. Traoré, O. Cueto,
was partially supported by the Brain Korea 21 PLUS project L. Perniola, V. Sousa, D. Vuillaume, C. Gamrat and
(Center for Creative Industrial Materials). B. DeSalvo, J. Appl. Phys., 2012, 112, 054904.
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Emerging Memory Devices For Artificial Synapses

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Emerging memory devices for artificial synapses

1. Introduction information, with ultralow energy consumption.5,6 A human

Youngjun Park received his BS Min-Kyu Kim received his BS

Review Journal of Materials Chemistry C

two-terminal devices such as resistive switching memory

switching behaviors, spike-rate-dependent plasticity (SRDP),

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

an electric field, then maintained even without an external electric

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

4. Summary and outlook

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

Review Journal of Materials Chemistry C

Journal of Materials Chemistry C Review

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