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Hardware implementation of neural networks with memristors can break the “von-Neumann bottleneck,” offer massive parallelism, and hence
substantially boost computing throughput and energy efficiency. In this review, we first explain the design principles and switching mechanism of a
Ta/HfO2 memristor. We show that the device meets most key requirements on device properties for in-memory computing. We then introduce the
integration of the memristor with foundry-made metal-oxide-semiconductor transistors and the programming of the one-transistor-one-resistance
switch (1T1R) arrays. We demonstrate that the crossbar arrays can be used in various neural networks. Finally, we discuss the remaining
challenges of scaling up the memristive neural networks for larger scale real-world problems. © 2022 The Author(s). Published on behalf of The
Japan Society of Applied Physics by IOP Publishing Ltd
Content from this work may be used under the terms of the Creative Commons Attribution 4.0 license. Any further distribution of this
work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.
© 2022 The Author(s). Published on behalf of
SM0802-1 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SM0802 (2022) PROGRESS REVIEW
Fig. 1. (Color online) The two-terminal memristor device, usually with a switching layer sandwiched between two electrodes, has multilevel conductance
modulated by an electric stimulus. Organized into a crossbar architecture, they can perform analog vector-matrix multiplication within the array using physical
laws. With necessary supporting peripheral circuits, they implemented a neural network that can solve real-world problems.17)
Fig. 2. (Color online) The schematics with exemplary TEM images showing three typical mechanisms responsible for conductance tuning in conduction-
channel based memristors, including the modulation of the width of a conduction-channel, the gap between the channel and an electrode, and the composition
of the conduction-channel. Reprinted from Ref. 17.
typical resistance switching mechanisms in conduction- Fig. 3. The composition analysis of the conduction channel
channel-based memristors.17) The device conductance could suggests that Ta has moved inside of the HfO2 matrix, and
be changed by modulating the diameter of a conduction- oxygen vacancy is also playing a critical role.
channel, e.g. in the conduction-bridge type memristor by Consequently, the electronic conduction mechanism at the
applying different levels of compliance.22) However, in such high-resistance and low-resistance states are distinctly dif-
a case, the reset step is usually strong and abrupt due to the ferent. As shown in Fig. 4(a), both LRS and HRS showed a
existence of a metallic bridge. In addition, efficient contin- linear I–V relationship at low voltages, indicating no tun-
uous conductance tuning could be achieved by modulating neling gap between electrodes and the conduction channel,
the distance of a tunneling gap between the conduction which is different from the well-studied TiOx−based devices
channel and an electrode.23–25) Since the conduction me- where a tunneling gap was present and responsible for the
chanism is tunneling-dominated, the IV relationship of each switching behavior. Although the linear I–V relationship can
state is nonlinear. Consequently, the most promising ap- also be achieved for a metal/insulator/metal (MIM) junction
j
proach to obtaining multiple conductance states with the when the applied voltage is very small (≈0 V or = e , where
linear IV behavior is the modulation of the conduction- j is the barrier height and e is the charge of the electron),29) it
channel composition.26–28) In choosing the matrix material, a is highly unlikely for our case here since the current is
simple binary system with only a conductive and an relatively high for our device even at HRS.25) We measured
insulating phase at the switching temperature is beneficial the device resistance as a function of temperature at both
for higher endurance.26) Based on these principles, we HRS and LRS. The device at LRS showed a typical metal-
designed a Ta/HfO2 memristor device that operates on the like behavior as its resistance linearly increased with tem-
motion of mobile species (oxygen vacancies and tantalum perature. In contrast, the device at HRS showed a typical
ions) in an amorphous HfO2 matrix, with the analog behavior for non-metallic materials in that the resistance
switching behavior enabled by the modulation of Ta:O ratio increased with temperature [Fig. 4(b)]. The measured tem-
in the localized conduction channel. perature coefficients of resistance (TCR) were 8.75 × 10−4/K
The composition change during the switching is confirmed and −4.37 × 10−4/K for LRS and HRS, respectively. The
with electron energy loss spectroscopy (EELS) of a sub-10 different signs of the TCR at LRS and HRS suggest that the
nm Ta-rich and O-deficient conduction channel. As shown in modulation of the chemical composition in the conduction
© 2022 The Author(s). Published on behalf of
SM0802-2 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SM0802 (2022) PROGRESS REVIEW
(a) (b)
Fig. 3. (Color online) Direct observation of a Ta-rich and O-deficient conduction channel. (a) Comparison of core-loss EELS spectra collected at the pristine
HfO2 layer, conduction channel region and Ta electrode. It indicates the conduction channel is Ta-rich. (b) O-K edge EELS spectra taken at three areas, which
clearly show the conduction channel is also O-deficient.28)
(a) (b)
Fig. 4. (Color online) (a) Linear IV curves for the device at both LRS and HRS. (b) The dependence of the normalized resistance change
(ΔR = (R−R(300 K))/R(300 K)) on temperatures, from where the TCR is measured to be 8.75 × 10−4/K for LRS and −4.37 × 10−4/K for HRS. Reprinted from Ref. 28.
channel rather than the size should be responsible for the switching behavior under quasi-DC voltage sweeps after an
switching in our Ta/HfO2 memristor. The continuous mod- electrical forming step, turning on when a positive voltage is
ulation of the conduction-channel composition leads to applied to the Ta electrode and off when the voltage polarity
multiple resistance states. It should be noted that if the reset switches [Fig. 5(a)]. With a smaller device size, the opera-
step is too strong, we may achieve a HRS with a much lower tional current of the device is much reduced [Fig. 5(b)]. We
conductance but poor IV linearity, which is not within the first achieved multiple conductance states from the Ta/HfO2
interested conductance range in our current studies. memristor using different compliance currents and stop
Since the most suitable application for a memristor-based voltages during SET and RESET, respectively, as shown in
AI accelerator is inference, we chose mobile species with Fig. 5(c). In addition, like the potentiation/depression beha-
reasonably high activation energy in our device design. vior of a biological synapse, we can gradually increase and
Table I lists the activation energy of a few ionic species in decrease the device conductance with a train of electrical
different transition metal oxides. Higher activation energy pulses. For example, Fig. 5(d) plots the conductance change
means the mobile species will not move around once set into of the Ta/HfO2 memristor in response to 39 electric pulses
a particular position, suggesting high stability of the resis- (pulse width: 100 ns), including 26 consecutive positive
tance state. Although a relatively higher program voltage pulses with the amplitude increased from 0.75 to 1 V, and
may be needed during programming, an inference system is 13 consecutive negative ones with the amplitude decreased
not trained intensively, so the overall energy footprint is still from −1.05 to −1.17 V (step size: 10 mV step).
low. The different resistance states are all stable even at higher
temperatures. We programmed the device into eight states
3. Electrical properties of the Ta/HfO2 memristors using different compliance currents to examine the stability
Our Ta/HfO2 memristor has a simple MIM consisting of an of different conductance states. They showed no evident
inert metal Pt (or Pd/Ru) as the bottom electrode (BE), Ta as current fluctuation and drift for over 104 s at 150 °C
the top electrode (TE). A 5 nm atomic layer deposition [Fig. 6(a)]. To fully evaluate the retention properties,
prepared HfO2 blanket layer is sandwiched in between as temperature (T) dependent retention measurements were
the switching material. The device exhibits typical resistance performed, and the device failure time (t) at HRS was
Table I. The activation energy of typical mobile species in different oxide matrices.
(a) (b)
(c) (d)
Fig. 5. (Color online) (a) Typical IV curves for the Ta/HfO2 device by quasi-DC voltage sweeps (step size: 50 mV) after an electrical forming step (at 2 V)
for a 10 μm device and (b) 100 nm device. The black arrows indicate the switching polarity. (c) Analog resistance tuning in the 10 μm device achieved by
using quasi-DC voltage sweeps with different compliance currents. (d) The gradual modulation of the device conductance can also be achieved using pulse
train consisting of 26 positive pulses (100 ns, 0.75 to 1 V, 10 mV step) and 13 negative pulses (100 ns, −1.05 to −1.17 V, 10 mV step), akin to the potentiation
and depression behavior of a biological synapse.28) The results of (c) and (d) are from the 10 μm devices.
(a) (b)
Fig. 6. (Color online) (a) Retention of eight different conductance states at 150 °C for over 104 s. (b) The fitting plot of measured HRS retention time at
250 °C, 275 °C, 300 °C, 325 °C and 350 °C with the Arrhenius equation (red line). The activation energy of mobile species (Ea) is extrapolated to be 1.55 eV and
the extrapolated retention time is 70258 years at 85 °C and 10 years at 162 °C. Reprinted from Ref. 28. The results here were measured from the 10 μm devices.
2.7 × 105, 7.5 × 104, 1.4 × 104, 2.7 × 103, and 1.3 × 103 s at
250, 275, 300, 325, and 350 °C, respectively [Fig. 6(b)]. The
Arrhenius equation can well fit the t–T relation. The extra-
polated retention time was 7 × 104 years at 85 °C, and
beyond 10 years even at 162 °C. The exceptional stability
was attributed to the relatively higher activation energy of
mobile species (1.55 eV) extrapolated from our Ta/HfO2
when compared with other material systems, as listed in
Table I.
The device also exhibits high endurance, ensuring suffi-
cient programming cycles for the training for many applica-
tions. As shown in Fig. 7, over 1.2 × 1011 open-loop digital
Fig. 7. (Color online) Over 1011 billion digital switching cycles achieved
switching cycles were achieved from the device without any from the Ta/HfO2 memristor with pulses of 1.3 V/100 ns for SET and
feedback or power-limiting circuits, which is the highest −3.05 V/100 ns for RESET. The device states were read at 0.1 V. Reprinted
reported endurance for a single-oxide-layer memristive from Ref. 28. The results here were measured from a 10 × 10 μm2 device.
© 2022 The Author(s). Published on behalf of
SM0802-4 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SM0802 (2022) PROGRESS REVIEW
(a) (b)
(c)
Fig. 10. (Color online) (a) A typical example of programming our Ta/HfO2 memristor to a desired conductance with the feedback tuning algorithm.9) (b) The
histogram of the writing error (the difference between target conductance value and final value) with a standard deviation of 6 μS when the writing tolerance of
±10 μS was used. (c) Experimental conductance writing result of the discrete-cosine transform (DCT) pattern into a 64 × 64 array. Device size: 4 × 4 μm2.
Reprinted from Ref. 6.
(σ) of 6 μS when the writing tolerance of ±10 μS was used to difficult for most two-terminal memristive devices because of
program the array. The small σ value suggests that more than the intrinsic device nonlinearity and that conductance change
64 conductance levels or 6 bits of digital precision can be is history-dependent. With the 1T1R architecture, linear and
achieved from our Ta/HfO2 devices within a device con- symmetric weight updating with one-shot programming
ductance range of 100–900 μS, sufficient for many edge becomes feasible. As shown in Fig. 11(a), two synchronized
computing tasks. The equivalent bit-precision, primarily electric pulses (VTE/VBE to memristors and Vgate to transis-
limited by the intrinsic device noise, could be further tors) are applied, with the VTE staying the same while the gate
increased by defining a narrower tolerance during program- voltage increases in each set cycle. For the reset operation, a
ming and/or using a larger number of closed-loop iteration large reset pulse is first applied on the BE with the transistor
cycles. With the write-verify scheme, arbitrary conductance gate open, and the following conductance tuning is imple-
maps corresponding to different algorithms can be written mented with the VTE and a decreasing transistor gate voltage
into the 1T1R array with high precision. For example, [Fig. 11(b)]. With this scheme, the device conductance can be
Fig. 10(c) shows the conductance map of a 64 × 64 array linearly increased with the gate voltage for Vgate between
after the discrete-cosine transform (DCT) algorithm was 0.6 and 1.6 V [Fig. 11(c)]. The linear and symmetric weight
successfully written. updating with our developed scheme also reduces cycle-to-
4.3. Programming scheme for in situ training of a cycle and device-to-device variations [Figs. 11(d), 11(e)],
1T1R array demonstrating it is a reliable scheme for in situ training.
While an inference system can afford multiple pulses at each A simple model can be built to understand the linear and
cell during programming because once trained, the system symmetric weight updating.38) When the voltage across a
R
can be used for a long time, making the overall energy memristor (Vmem = R mem VAppl ) in the 1T1R cell drops
mem + Rtrans
landscape reasonable. However, for a system that needs below a threshold voltage (Vmin), the switching process
frequent training, one-shot programming is desired to reduce terminates. Here, Rmem , Rtrans, and VAppl is memristor resis-
power consumption. Furthermore, to better map machine tance, transistor channel resistance, and the total applied
learning algorithms into the conductance map of the array, voltage, respectively. The assumption is similar to the theory
linear and symmetric weight updating is essential. This is proposed by Ulrich B. et al. recently.39) After the 1T1R
(a) (b)
(c) (d)
(e)
Fig. 11. (Color online) The developed two-pulse scheme to gradually (a) set and (b) reset the device. (c) 20 cycles of linear and symmetric weight updating
from a representative cell and each cycle contains 200 pulses. (d) Single such weight updating cycle collected from all responsive devices in the array and the
median conductance is indicated by the yellow line. (e) Over 20 such weight updating cycles from all responsive devices in the array. Device size: 4 × 4 μm2.
Reprinted from Ref. 7.
(a) (b)
Fig. 12. (Color online) Column or row-wise parallel programming of the 1T1R crossbar array. (a) During reset, a reset pulse is applied to the bottom
electrodes of an entire column simultaneously, while the top-electrode voltages control which devices are reset. (b) For the set process, a set pulse is applied on
the top electrodes of an entire row, and the different transistor gate voltages determine the how much each memristor’s conductance is changed.7)
most typical neural network topographies. However, such Figure 13 shows an exemplary system that also has a digital
neural networks are mixed-signal systems, which would not computer and a microcontroller, in which the computer is
be possible without peripheral circuitry such as DACs used to run scripts from different algorithms, and the
(digital-analog converters) for generating driving pulses and microcontroller controls all the circuit components. These
ADCs (analog-digital converters) for collecting the measure- peripheral circuit components are critical to ensure the
ment data. Sample and hold circuits may be used to synchronization of the signals (such as the voltages on the
synchronize all the output signals better, and trans-impedance memristor electrodes and transistor gates), and a professional
amplifiers to convert the sensed current into a voltage signal.
Fig. 13. (Color online) An exemplary system consisting of a 1T1R memristor crossbar array and peripheral circuitry that supports the operation. The proper
design of such a system calls for both device knowledge and mixed-signal circuit expertise. Reprinted from Ref. 7.
© 2022 The Author(s). Published on behalf of
SM0802-8 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SM0802 (2022) PROGRESS REVIEW
design is required to utilize the advantages of both the of printed circuit boards (PCBs) that contain the hardware
traditional and emerging technologies. neurons built with off-the-shelf electronic components. The
To implement neural networks with more than one layer, fully hardware-based neural network was used in demon-
the data flow is a critical issue. Previously we have used strating high-accuracy object classification. By substantially
different partitions of the same array as separate layers in a reducing the resource-demanding data shuttling and analog-
neural network. For example, by partitioning a 128 × 64 digital conversions, it delivers much-improved power and
array into two layers, we built a two-layer perceptron that area efficiencies, as estimated based on the 65 nm CMOS
was used to classify MNIST handwritten digits with high node.
accuracy.7) By partitioning the array into three fully con-
nected layers, we implemented the reinforcement learning 6. Summary and perspective
algorithm.12) Similar techniques were adopted to demonstrate Guided by the fundamental physical principle and the
recurrent neural networks with long short-term memory units required device properties for computing, we have developed
for time-sequence data analysis8) and convolutional recurrent a Ta/HfO2 memristor that meets most of the requirements for
neural networks.40) in-memory computing in artificial neural networks. The
For the aforementioned multilayer networks, the output of device exhibits stable multilevel conductance states, analog
one layer should be nonlinearly activated before being fed to tunability, high endurance, long retention, and decent IV
the subsequent layer. This could be implemented in software, linearity within certain conductance ranges. Integrated with a
in which the analog signals from the earlier layer are transistor into a 1T1R crossbar array, the conductance of each
converted to digital before they can be nonlinearly activated. cell can be precisely tuned for an inference system and
This step usually is a bottleneck that limits the system modulated linearly and symmetrically with one-shot pro-
performance. To address this issue, a two-layer perceptron gramming for an online training system. Taking the resource-
with both hardware neurons and synapses was designed and demanding tasks, the vector-matrix operation, the 1T1R
built (Fig. 14).41) In this proof-of-concept system, two memristor crossbar array brings advancement in energy
128 × 64 1T1R arrays were used as the first and second efficiency and computing throughput, owing to the capability
fully connected layers in the perceptron, connected by a stack of parallel analog computing in the physical domain.
Fig. 14. (Color online) A two-layer all hardware perceptron. The upper panel shows the circuit schematic of the perceptron. The lower panel shows the
optical images of a 1T1R crossbar for the first layer, a stack of PCBs of the hidden neurons (ReLUs), and a second crossbar for the second fully connected
layer. The hardware neurons contain a total of 64 channels of ReLU activation functions and 64 inverters to support 64 differential pairs for the second layer.
Scale bar, 1 mm. Reprinted from Ref. 41.
© 2022 The Author(s). Published on behalf of
SM0802-9 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SM0802 (2022) PROGRESS REVIEW
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