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Name of the student- Nitish Saini Registration No.- 10PP18A32037
Faculty of Study- Physical Sciences Year of Submission- 2023
CSIR Lab- National Physical Laboratory, Name of Supervisor- Dr Ajeet Kumar
New Delhi
Title of thesis- Bio-inspired Memristive Devices for
Neuromorphic Computation & Its Application
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The limitations of conventional computing, specifically the von Neumann bottleneck, have
hindered technological advancement due to data transfer inefficiencies and processing speed
limitations. Neuromorphic computing, which mimics the structure and function of the human
brain, offers a potential solution. Neuromorphic computing relies on memristive devices that can
perform digital and analogue computations, making it highly efficient. This approach has the
potential to optimize futuristic devices without the need for extensive programming.
A functional layer of poly(3,4-ethylenedioxythiophene) (PEDOT) polymer is deposited by electro-
polymerization using cyclic voltammetry. Here, we studied Pt/PEDOT/Al based memristor, which
exhibited excellent artificial synapse like plasticity. We discuss the basic function of remembering
and forgetting devices through synapticity and plasticity. The devices show excellent plasticity
behavior mimicking bio synaptic behavior, which makes them a suitable system for
neuromorphic applications.
Spike time-dependent plasticity (STDP), is the most important Hebbian learning rule for learning.
Modulation in synaptic strength and output is observed in PEDOT based memristors upon
stimulations from different waveform signals, which showed to mimic various Hebbian learning
rules of a biological synapse. The synaptic plasticity is directly correlated to the temporal
ordering of pre-and post-synaptic spikes. We demonstrated that the square, triangle, and
complex waveforms, their duration as well as the waveform spike pairing connections affect the
STDP learning window of the devices. The plasticity modulation with second order spiking signal
is also demonstrated. The characteristics observed in the devices can be crucial steps toward
designing a neural network mimicking a biological synapse.
A functional layer of methylammonium lead iodide (CH3NH3PbI3, MAPbI3) perovskite as a
switching material is deposited via thermal deposition. The resulting Al/MAPbI3/ITO-based
memristor demonstrates impressive bipolar resistive switching behavior. The device shows
stable characteristics of retention and endurance. The device also showed memorization
characteristics for both sweep and pulse cycles. The device exhibits multilevel digital
characteristics for a successive increase in voltage pulse and beyond a limit, it shows a transition
to analog switching behavior.
The simultaneous real time processing and interpretation of data is a challenging task.
Memristor enabled reservoir computing (RC) has shown great promise toward real time neural
signal analysis. Here, we demonstrate a PEDOT polymer based memristor behaviour towards
real time neural spike. The readout function is trained for classification and temporal analysis.
Brain like hardware featuring recognition of neural input patterns is reported. This concept is
further expanded for practical application to automate traffic surveillance.
List of Publications
Journals
1. Nitish Saini, Arti Bisht, Asit Patra, and Ajeet Kumar. Synaptic plasticity in
electro-polymerized pedot based memristors for neuromorphic application. J.
2. Nitish Saini, Rashi Kedia, Asit Patra, Ajeet Kumar. Synaptic Spike Time
3. Nitish Saini and Ajeet Kumar. Real time traffic surveillance based on neural
firing pattern recognition technique.
4. Kalpana Agarwal, Nitish Saini, Arti Bisht, Ajeet Kumar and Ritu Srivas-
tava. Voltage dependent multilevel digital to analogue transition in perovskite
memristor device.
5. Harshit Sharma, Nitish Saini, Ajeet Kumar, and Ritu Srivastava. Agbis2
quantum dot based multilevel resistive switching for low power electronics.J.
Mater. Chem. C, 2023. doi.org/10.1039/D3TC01050C
6. Arti Bisht, Nitish Saini, Komal Bhardwaj, Rachna Singh and Ajeet Ku mar.
Two-Stage Filamentary Mechanism in High-Performance Organic Resistive
Switch. J.Mater. Chem. C, 2023. doi.org/10.1039/D3TC02348F
7. Harshit Sharma, Nitish Saini, Lalita, Divya Kaushik, Ajeet Kumar. Ritu
Srivastava. CuInS2 quantum dots-based unipolar resistive switching for non-
volatile memory application. RSC Adv., 2024
106
List of Publications
2. IEEE-ICEE 2020
107
J Mater Sci: Mater Electron
1
CSIR-National Physical Laboratory, Dr. KS Krishnan Marg, New Delhi 110012, India
2
Academy of Scientific and Innovative Research (AcSIR), Ghaziabad 201002, India
https://doi.org/10.1007/s10854-022-09368-2
holes [12]. A memristor is a two terminal device dependent plasticity (STDP), which is the most
having a thin functional layer sandwiched between important Hebbian learning rule for learning and
two electrodes. Memristors store data by internal memory showed up to 75% change in synaptic
reconfiguration of charged particles in the functional weight under wide range of input signals, which
layer, which stabilizes in variable resistance states makes it a suitable material for neuromorphic com-
when subject to different external inputs [13]. To putation applications [31].
mimic biological synapse, memristor’s top and bot-
tom electrodes serves as pre- and post-synaptic
neurons, respectively. The pre-neural and post-neu- 2 Experimental
ral are connected through a unique synaptic weight
which makes it capable of addressing information 3,4-Ethylenedioxythiophene (EDOT) (97%) and
like a human brain [14, 15]. anhydrous tetrabutylammonium hexafluorophos-
The potential functional layer to achieve efficient phate (TBAPF6 ) were purchased from Sigma Aldrich.
artificial synapse is categorized as inorganic and Acetonitrile (99%, RG) was purchase from Sisco
organic materials [16]. Most of the work on memris- research laboratories Pvt.Ltd. Electrochemical studies
tor have been done on inorganic materials such as were carried out with Metrohm AUTOLAB-PGSTAT
HfO2 [17], Nb2 O5 [18], WO3 [19], etc. These materials using a three-electrode assembly with platinum-
lack bio-compatibility, biodegradability and flexibil- coated silicon wafer as the working electrodes. Pt
ity, which are needed for various applications [20]. wire was used as counter electrode a Ag/Agþ was
The organic polymer poly(3,4-ethylenedioxythio- used as a reference electrode. The measurement was
phene) (PEDOT) based memristors proved to be an performed under N2 atmosphere and before each
excellent material for such applications. It has been measurement N2 was purged through the solution
widely used in photo-electrical devices due to its for 10min to deoxygenate the system. Fer-
properties such as, ability to form a uniform, trans- rocene/ferrocenium couple was used as external
parent, conductive, and thermally stable thin film, standard for the cyclic voltammetry system.
which strengthens the adhesion to the organic layer, An electro-polymerized PEDOT thin film 50 nm
good energy conversion efficiency, low-cost mass was deposited on a Pt/SiO2 /Si substrate using cyclic
production [21], bio-compatible and biodegradable volametry. The room temperature basic electronic
[22] and works great for stretchable and flexible characterization of Pt/PEDOT/Al device and
electronics applications [23–25]. A lot of research is synaptic behavior were investigated with two probe
done on water soluble poly(3,4-ethylenedioxythio- using Keithley-2450 source meter. The labview pro-
phene) polystyrene sulfonate (PEDOT:PSS) complex gram is made to study synaptic behavior using pulse
thin film instead of water insoluble PEDOT thin film signal.
[26]. The PEDOT based devices shows unipolar or
bipolar resistive switching is observed based on
electrode combination [27–29]. The PEDOT is a con- 3 Results and discussion
ductive and thermally stable conducting polymer
Different strategies for deposition of thin film on
[30]. However, neuromorphic study on electro-poly-
substrates have been well reported, such as solution-
merized PEDOT polymer has not been reported so
processable, thermal and electrochemical deposition
far.
and so forth. Among these, electrochemical deposi-
In the present study, we report fabrication of
tion method is a potential technique to control the
memristor with electropolymerized PEDOT as the
morphology, thickness, and doping level of the film,
functional layer. The electropolymerized thin film is
which are essential parameters for the device per-
uniform throughout the surface. This uniformity
formance. It is worthy that electrochemical poly-
reduces cell-to-cell measurement variation. The basic
merization yielded pure, metal-free, least chemically
memristor electronic characterization of SET/RESET,
defect material and better film adhesion on substrate.
retention, and endurance is reported. We demon-
The high quality thin film of PEDOT was deposited
strated the synaptic properties like short term plas-
on the substrate of platinum-coated silicon wafer by
ticity (STP), long term plasticity (LTP), and spike-
electrochemical polymerization, as depicted in
rate-dependent plasticity (SRDP). Spike time
Fig. 1b. Monomer 3,4-ethylenedioxythiophene in resistance is observed due to the formation and
(EDOT) was used for polymerization by cyclic rupture of conduction filament which is correlated to
voltammetry (CV) scanning from - 0.5 to 1.5 V at oxidation and reduction of functional layer, respec-
scan rate 50 mV/s. Electropolymerization was carried tively [29]. When positive bias is applied on the top
out using 0.01 M EDOT as a monomer, 0.1 M tetra-n- electrode (Al), holes were injected into the film.
butylammonium hexafluorophosphate (TBAPF6 ) as a Under the influence of electric field, the charge ions
supporting electrolyte and MeCN as a solvent. The get accumulated. In this case, PEDOTo which act as a
thickness of the deposited PEDOT films on substrate charge trapping site is oxidized to PEDOTþ (PED-
was controlled by the number of electropolymerized OT0 þ hþ ! PEDOTþ ) which is a low resistance state
cycles and monomer concentration. The electropoly- [33]. This leads to space charge accumulation of
merization of PEDOT film was characterized by CV charged ion PEDOTþ across the electrode. When an
and absorption spectra (Figs. S1 & S2 in Supple- adequate amount of charges accumulate, a sudden
mentary Information). The results are in agreement increase in the conductivity (SET) was observed due
with our previously reported characteristics of to the formation of conduction path in the PEDOT
PEDOT films [32]. The resulting electrochemically film. This accumulation of charges is responsible for
deposited film was washed with monomer-free sol- LRS behavior. When the top electrode was negatively
vent and keep at ambient conditions for drying for biased, electrons were injected into the film. The
device fabrication. PEDOTþ is reduced to PEDOT0 (PEDOTþ ? e !
The electropolymerization deposited structure of PEDOT0 ) which is a high resistance state [34]. The
Pt/PEDOT/Al is investigated for memristor behavior conduction path was destroyed across the electrode
as shown in Fig. 2a. Platinum (Pt) and aluminum and an abrupt decrease in conductivity (RESET) was
(Al) are used as bottom and top electrodes, respec- observed. The device endurance characteristics were
tively. The current–voltage (I–V) memristive charac- studied by continuously applying SET/RESET pulses
teristics are shown in Fig. 2b. The device exhibits of 1.5/- 2 V of 100 ms and a read voltage (0.01 V, 100
bipolar resistive switching, the device could be SET ms). We observed resistance fluctuation, while
and RESET with the change in bias polarity. In step 1, switching from one state to another, was more in the
the voltage is swept from 0 V to positive bias, the HRS state than in the LRS state. The breakdown of
rapid increment in current was observed resulting in conduction filament is an abrupt process which can
attaining compliance value, i.e., 0.0005 A at around 1 cause current fluctuations.
V and turned the device ON (SET). The conduction The conductance of the device can be regarded as a
filament was formed. In step 2, the voltage swept synaptic weight. The synaptic weight is continuously
back to 0 V, the device remained ON. In step 3, the adjusted equivalent to the device conductance [35].
voltage swept from 0 V to negative bias, the current The various activity like forgetting and memorizing
decreased instantly and switched (RESET) the device are based on the synaptic weight change of a bio-
from ON to OFF state. In this process, the breakdown logical synapse. The Pt/PEDOT/Al memristor con-
in conduction filament occurs. In step 4, when the ductivity changes with every consecutive voltage
voltage swept back to 0 V, the device remained in sweep. To study the above behavior, a positive volt-
OFF state. The positive bias potential shows a sym- age sweep after every sweep from 0 to 0.8 V is
metric behavior with higher conductivity. A change
Fig. 1 a Electrochemical
polymerization of EDOT in
solvent-electrolyte medium.
b SEM image of
electropolymerized PEDOT
thin film
Fig. 2 a Pt/PEDOT/Al memristor and biological synapse current was set to 0.0005 A for 0 to ? 1.5 V sweep and 0.0004 A
structural analogy. b I–V plot of Pt/PEDOT/Al exhibiting for 0 to - 1.5 sweep, respectively, where the arrow represents the
bipolar resistive switching of up to 5 cycles. The compliance direction of the voltage
applied and a gradual increase in current was 1 V amplitude is calculated by fitting equation y ¼
observed. The synaptic weight increased gradually
a ðx cÞb where b is non-linear parameter having
after every successive run, shows memorizing
value - 0.088. The amount of space charge accumu-
behavior of the device as shown in Fig. 3a. Similarly,
lation increases gradually at the electrode after every
a multiple successive negative voltage sweep from 0
successive positive pulse. With each successive pos-
to (- 0.8 V) is applied and a gradual decrease in
itive pulses, the charge accumulates at the electrode
current was observed. The synaptic weight decreased
lower the interface barrier and hence, increased the
gradually after every successive run, shows forget-
conductivity of the device. The accumulation of
ting behavior of device as shown in Fig. 3b. The
charge at the interface is very rapid initially and
similar approach can be explained by applying volt-
saturate at a later stage. The amount of space charge
age pulses. In this study, a series of 50 identical
accumulation decreases at the electrode after every
positive pulses (1 V, 600 ms) followed by similar
successive negative pulse. The recombination of
series of 50 negative pulses (- 1 V, 600 ms) were
accumulated charge annihilates the conduction fila-
applied to the device. A read voltage (0.01 V) was
ment and decreased conductivity was observed. The
applied after each pulse and the read current was
change in conductivity was non-linear. This non-lin-
measured and non-linear function was fit as shown in
ear gradual increase and decrease in conductivity are
Fig. 3c. The non-linearity for 1 V amplitude is cal-
called potentiation and depression, respectively. We
culated by fitting equation y ¼ a xb where b is non- can infer from the above results, our device is capable
linear parameter having value 0.147. Similarly, for -
Fig. 3 Memorization characteristics of PEDOT based memristor. measured by series of 50 pulses of 600ms width at ?/- 1 V
a The hysteresis current increases with every voltage sweep of 0 to respectively. The read current was measured at 0.01 V and non-
0.8 V. b The hysteresis current decreases with every voltage sweep linearity function was fit (solid lines). The increment and
of 0 to - 0.8 V. c The potentiation and depression characteristic is decrement of current was observed
of emulating analogue electronic characteristics of synaptic weight drops rapidly, and if t [ [ s the
memristor. synaptic weight varies gently. Thus, the relaxation
The human brain memory shows two kind of time constant plays an important role. Fig. 4c shows
plasticity, short term plasticity (STP) and long term the synaptic weight with respect to time for different
plasticity (LTP). In STP, the synaptic connections input pulse trains and the fitting curve. The
persist for a very short duration, i.e., for few seconds stable synaptic weight and relaxation time constant
or minutes and then fades away. In LTP, permanent was obtained from the fitting curve. This was then
change in synaptic connection is observed, which plotted with respect to a number of pulses in Fig. 4c.
may last for hours or years [36]. However, STP can be As shown, as the number of input voltage pulses
reshaped to LTP through continuous stimulations increases the relaxation time increased. Thus, the
[37]. Transition for the devices was observed from current takes longer time to decay. Also, the
STP to LTP (shown in Fig. 4b). A sequence of dif- stable synaptic weight increases which indicates the
ferent pulse train (1 pulse train = 5 to 30 voltage decrease in volatility of device and also indicates a
pulses) having a fixed amplitude 1 V, width and confirmation from STP to LTP transition of the
interval as shown in Fig. 4a were applied to the device.
memristor. After a different number of voltage pul- Spike-timing-dependent plasticity (STDP) is one
ses, the current was recorded at 0.01 V for 50 seconds, the most important and the fundamental Hebbian
so that the device relaxes back to attain an equilib- learning rule for learning and memory, which states
rium state. The current was measured and inter- that the change in synaptic weight is correlated to
preted as synaptic weight. For stimulation N = 5 and temporal synchronization between pre- and post-
10 voltage pulses, the device relaxes back to the HRS synaptic spikes [38]. If the temporal synchronization
state and the lifetime value becomes insignificant. For of pre-synapse is before post-synapse (Dt \ 0), it
N = 20 and 30, the adequate amount of charge carrier results in increment in synaptic weight (i.e., long-
gets accumulated. Thus, the device attains synaptic term potentiation or LTP). In reverse temporal paring
weight which indicates a transition of STP to LTP. (Dt [ 0), results in decrement in synaptic weight (i.e.,
The synaptic weight retention curve as shown in long-term depression or LTD).
Fig. 4b indicates that current drops rapidly at the To stimulate STDP, precise temporal pair of pre-
beginning, then moderately, and stabilizes at last. The and post-synaptic spike with 1 V/- 1 V amplitude
recombination of the charge carrier could be a reason with the pulse width of 100 ms was applied to the top
for the decay in the retention curve. The exponential and bottom electrodes of the memristor respectively.
decay function was fit to analyze relaxation time in The time interval Dt is defined as the difference of
Fig. 4b. time elapsed between the pre- and post-synaptic
I t = I 0 ? Aexp (- t/s) spike respectively, as shown in Fig. 5a. The read
I 0 represents steady stable current, A is a constant current (0.01 V) was measured before and immedi-
and s is the relaxation time constant. If t \ s, the ately after the spike. The percentage change [39] in
Fig. 4 a A sequence of different input voltage pulse train applied relaxation time. The number of pulses in (a) and the corresponding
to the device at t \ 0. b The change in synaptic weight at t[0 is synaptic weight in (b) are time correlated. c The stable synaptic
plotted after different numbers of a voltage pulses were applied. weight after different number of voltage pulses and the relaxation
The exponential decay function was fit (solid lines) to analyze the time constants after different number of a voltage pulses
the relative synaptic weight was calculated and i.e 20 s and 10 s, the accumulation of space charge is
plotted as shown in Fig. 5b. As discussed above, the not adequate and the current difference is small. The
increment (decrement) of relative synaptic weight conductivity of the memristor increases for 5 s pulse
was observed when the pre-synaptic spike was interval. Further reduction in pulse interval to 1 s,
applied before (after) post-synaptic spike. The device significant increase in current was observed with
exhibit excellent STDP functional property mimick- successive pulse. Thus, when the time interval
ing biological neural network. between the successive pulses is shorter than the
Another important characteristic of biological decay constant of effective charge diffusion, the cur-
synaptic plasticity is spike-rate-dependent plasticity rent increases with each pulse. As the following
(SRDP). The time interval between two successive stimulus overlaps the current decay which leads to a
pulses also affects the change in the efficacy of a net increase in charge carrier at the electrode as
synapse [40]. The pre-synaptic spiking rate determi- shown in Fig. 6a. The relative change in current was
nes the strength of synaptic plasticity. In our mem- calculated and plotted with respect to the time
ristor, the top and bottom electrode mimicks pre- intervals between two successive pulses as shown in
synaptic and post-synaptic neuron, respectively. The Fig. 6b. Hence, to a great extent, the strength of
spiking rate effect on synapse was studied by synaptic plasticity is dependent on the pre-synaptic
applying a fixed number (N = 10) of identical voltage spiking rate.
pulses of 1 V and width 0.1s with varying time
interval between successive pulses (1 to 20 s).
The read current was measured after each voltage
pulse at a read voltage 0.01 V. For the large intervals
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development of neuron selectivity: orientation specificity and such publishing agreement and applicable law.
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