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Hybrid organic–inorganic halide

perovskites for scaled-in neuromorphic


devices
P.C. Harikesh, Benny Febriansyah, Rohit Abraham John, and
Nripan Mathews
Hybrid organic–inorganic halide perovskites have been recently explored as memristive
devices that can be programmed to two or more stable conductance states for analog
computing. The wide variety and range of optoelectronic phenomena these materials portray
offer immense potential to develop scaled-in neuromorphic devices and architectures
with multibit memory storage and multimodal accessibility. This article provides a general
summary of the structural and optoelectronic characteristics of this material class that could
be utilized for neuromorphic computing, discusses insights into the underlying switching
mechanisms, and reviews recent developments in the field of halide perovskite-based
neuromorphic devices.

Introduction per cell (e.g.,  expanding from binary conductance states [on
With the end of Moore’s Law projected, conventional com- and off] to a range of intermediate conductance states that can
puting architectures face challenges, including the heat wall, encode more than 1 bit) without escalating the amount of mate-
the memory wall, and latency wall. To fulfil the ever-growing rials and chip area being utilized, is more feasible and bears
appetite for information processing, new concepts of brain- closer resemblance to the plasticity of biological synapses.1
inspired computing are being envisioned to overcome the pre- New approaches in materials, device, architecture, and
viously mentioned bottlenecks of traditional von Neumann algorithm design are necessary to emulate the scale, connec-
hardware architectures. tivity, and energy efficiency of biological neural networks.
Neuromorphic electronics—an approach in which devices Increasing attention has therefore been given to organic mate-
and circuits merge memory and processing, analogous to syn- rials, such as small molecules and polymers whose optoelec-
apses and neurons in the human brain—promises to signifi- tronic and charge-transport properties can be tuned through
cantly improve the efficiency of artificial neural networks by chemical synthesis and functionalization, while endowing
in-memory computing. Memristors (memory + resistor), which them with facile and low-cost processability.2,3 These mate-
are thin-film devices that “remember” their resistance history, rials also intrinsically incorporate richer dynamics in their
are key enablers for this concept because they allow multi- switching behavior when compared to their inorganic counter-
ply accumulate operations (a benchmarking step in comput- parts. For example, many of these materials portray short-term
ing) to be performed in parallel at the location of data. The volatile switching behavior that can be consolidated to long-
first generation of neuromorphic synaptic devices were based term conductance/weight changes, bearing close resemblance
on oxide memristors and have demonstrated advantages in to temporal responses such as the calcium effect in biology,
scalability, speed, and power consumption. However, “scal- and providing additional temporal nodes to implement cor-
ing up” toward a practical system size by “scaling down” relations and computing.
device dimensions is increasingly challenging. Alternatively, Hybrid organic–inorganic neuromorphic devices based on
“scaling-in”—an approach to boost the information space
­ halide perovskites (HPs) are one such technology platform

P.C. Harikesh, Nanyang Technological University, Singapore; harikesh001@e.ntu.edu.sg


Benny Febriansyah, Nanyang Technological University, Singapore; benn0005@e.ntu.edu.sg
Rohit Abraham John, Nanyang Technological University, Singapore; rohitabrahamjohn@ntu.edu.sg
Nripan Mathews, Nanyang Technological University, Singapore; Nripan@ntu.edu.sg
doi:10.1557/mrs.2020.193

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

that offers large degrees of freedom or state variables. Similar All of these phenomena result in a modulated hysteretic
to organic semiconductors, halide perovskites (see  MRS operation, which can be tuned on demand to meet the analog
Bulletin, June 2020, for more information) allow facile depo- switching requirements of weighted synapses in an artificial
sition via solution processing/vacuum techniques while main- neural network.5 Additionally, their facile solution-based low-
taining excellent semiconducting properties. In addition, the temperature fabrication would facilitate large-scale realization
organic cation in the hybrid structure enables structural tun- of dense crossbar arrays (a collection of switches arranged in a
ability allowing modulation of charge transport and bandgap matrix configuration) at a low cost. Since this material class is
of the material. Unique to halide perovskites is the coexis- a debutant in the field of memristor technology, this article pri-
tence and coupling of ionic and electronic components of the marily focuses on the unique material characteristics of HPs,
current, resulting in tunable majority carrier concentrations, recent developments in HP neuromorphic devices, provides
above bandgap photovoltages and formation of local n- and insights into their switching mechanisms, and considers fur-
p-doped regions. This is enabled by its unique orbital charac- ther material and device development strategies.
teristics with an antibonding valence-band maximum (VBM)
and a bonding conduction-band minimum (CBM) resulting in Structure of hybrid halide perovskites
defect tolerance.4 Hence, any crystallographic defects induced Halide perovskites typically feature a three-dimensional (3D)
by ionic migration and accumulation will only induce shallow structure with the general formula ABX3.6 They comprise
traps in the material, allowing doping and hence local modula- an anionic network of corner-sharing octahedra that are cre-
tion of carriers. ated by simple cubic arrangement of divalent B-site cations,

Figure 1.  (a) ABX3 perovskite structure; (b) tuning the dimensionality of a perovskite using organic spacers; (c) common organic cations used
in mixed dimensional perovskites. Reprinted with permission from Reference 13. © 2019 Nature Publishing Group. (d) The band structure of
a perovskite showing defect tolerance. (e) Bandgap tuning. Reprinted with permission from Reference 47. © 2017 AAAS. (f) Carrier tuning via
compositional engineering. Reprinted with permission from Reference 8. © 2014 AIP Publishing. (g) Halide and cation migration in perovskites.
Reprinted with permission from Reference 9. © 2016 American Chemical Society. Large-scale facile processing techniques for printing
perovskite layers: (h) spray coating, (i) evaporation, and (j) slot die coating.15 Note: CB, conduction band; VB, valence band.

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

bridged by halide anions (X = Cl–, Br–, I–). Monovalent A-site connections based on relative timing between pre- and post-
cations occupy cuboctahedral cavities in the B-X sublat- synaptic action potentials) were demonstrated for 5–7 meta-
tice, providing charge balance (Figure 1a–c). While halide stable conductance states.
perovskites containing Pb2+ at the B-site have attracted intense Ren et al.18 followed with the first demonstration on 2D
interest in recent years, other B-site metals have been incor- perovskite, but with limited analysis of the synaptic char-
porated, especially isovalent Sn2+ and Ge2+. The A-site can be acteristics. In 2018, Mathews et al.5 coupled fast electronic
occupied by an alkali metal cation such as Rb+ or Cs+, but in transitions with slow drift-diffusive ionic kinetics of HPs to
most cases, small organic cations such as methylammonium enable energy-efficient analog-like switching of five meta-
(MA+) or formamidinium (FA+), are incorporated, resulting in stable conductance states. A combination of ion migration
hybrid organic–inorganic structures. and carrier injection barrier modulation explained the differ-
Prototypical 3D lead-halide perovskites are direct-band- ence in the degree of synaptic plasticity, more notable for the
gap semiconductors with VBM composed primarily of  halide larger organic ammonium and formamidinium cations than
p orbital and lead s orbital, and CBM having mostly lead the inorganic cesium counterpart, reporting the first system-
p orbital character (Figure 1d).7 This allows for tuning of the atic investigation on the effect of cation compositional space
bandgap by changing the halide ion (Figure 1e). In addition, on memristive and synaptic characteristics. This report also
the antibonding nature of the VBM results in defect toler- demonstrated the first mini array of HP memristors, and
ance (the crystallographic defects do not induce deep traps in the first simulation of a neural network to recognize hand-
the material) as previously discussed and enables facile car- written digits selected from the Modified National Institute
rier tuning (p- to n-type) by slight modulations in the metal of Standards and Technology database (a large database of
cation to halide ratios8 (Figure 1f). The connected lattice and handwritten digits that is commonly used for training vari-
the defect tolerance allow the ions to move without signifi- ous image processing systems) based on HP memristor data.
cantly degrading the semiconducting property (Figure 1g).9 Based on the STDP characteristics of HP synapses, 6000
Meanwhile, the A-site cations do not contribute to the images trained in simulation resulted in an accuracy of 80.8%.
band extrema. However, they can still affect electronic prop- This field has since then witnessed numerous impressive
erties via indirect steric or hydrogen-bonding interaction demonstrations, including, but not limited to, the first dem-
with the halometallate octahedra. Moving to relatively larger onstration of crossbars of evaporated HP memristors,19 uni-
A-site organic cations yields lower-dimensional 2D, 1D, or polar memristor crossbar array accessed with one diode–one
0D derivatives, depending on the size, conformation, and resistor (1D–1R) schemes,20 and photonic synapses using
functionality of the organic species.10,11 In addition, alloying perovskite quantum dots.21 State-of-the-art reports on halide
2D and 3D perovskites can result in intermediate materials perovskite memristors claim an on-off of ∼109 22 retention =
called Ruddlesden–Popper or Dion–Jacobson HPs featuring 5 × 104 s23 and endurance of 2700 cycles.24
contiguous multiple inorganic layers (“n”) separated by the
organic spacer12–14 (Figure 1b–c). Such versatility provides a Operative mechanisms
large compositional parameter space that can be tweaked to Despite these demonstrations, the dependence on the com-
tune memory and synaptic behaviors for neuromorphic com- position of cations and anions in the ABX3 structure, the
puting. Furthermore, the presence of organic cation and the morphology of the thin films, dimensionality, choice of
ionic nature of the material allows dissolution of the material interfaces, the applied electric fields, and scanning rates are
in common polar solvents allowing facile large area deposi- yet to be clearly established to maximize the memristive
tion (Figure 1h–j).15 performance of halide perovskites. Most halide perovskite-
based device architectures try to emulate the biological
State-of-the-art halide perovskite synaptic structure and behavior (Figure 2a). The follow-
neuromorphic devices ing discusses the mechanisms (Figure 2b–d), which enable
State-of-the-art memristive HP neuromorphic devices include conductivity tuning, and hence memristive and synaptic
demonstrations on iodide and bromide compositions of 3D characteristics in HPs.
perovskites, utilizing electrochemical metallization, ionic-
electronic coupling, local and interfacial doping, and ion and Electrode interfacial reactions
vacancy migration. Huang et al.16 and Lee et al.17 reported The simplest mechanism modulating the conductivity of HP
demonstrations of HP-based artificial synapses in 2016 util­ memristors is based on the electrochemical reaction of HPs with
izing vacancy-driven halogen migration as the underlying the metallic electrodes leading to filament formation by metal
mechanism. Apart from the conventional DC memristor I–V ion diffusion (Figure 2b). Studies have revealed redox reactions
(current-voltage) characteristics, synaptic features such as between perovskite and the metal contact, which result in the
short- and long-term plasticity with frequency and amplitude reduction of perovskite phase resulting in formation of metallic
dependent modulations, including spike-timing dependent lead (Pb0) within the HP active layer25 and simultaneous oxida-
plasticity (STDP) (a biological process that forms the basis tion of metallic contact dependent on the chemical potential of
for associative learning by adjusting the strength of synaptic the metal. Au shows a lower reactivity compared to Ag, Cr, Yb,

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

Figure 2.  (a) Schematic of chemical synaptic transmission. An action-potential causes selective endocytosis and exocytosis of Na+, K+,
and Ca2+ determining the extent of membrane polarization.5 Similar functions are emulated by halide perovskite (HP)-based artificial
synapses where the two electrodes form pre- and post-neurons, and conductance of the HP film acts as the synaptic weight. (b) Filament
formation modulating the conductivity of the perovskite channel via metal ion/halide diffusion. (c) Application of electric field changes the
material properties locally through ionic migration, also leading to interfacial doping of the HP-transport layer interfaces in turn modifying
the (d) charge injection efficiency, and thus modulating the conductivity of the channel in a synaptic device. Note: PEDOT:PSS, poly​
(3,4-ethylenedioxythiophene)-poly(styrene sulfonate).

or Al as revealed by x-ray photoelectron spectroscopy (XPS) conduction in methyl ammonium lead iodide using galvano-
(Figure 3a). Some metals such as Ag can react with halide static and electromotive force (emf) measurements29,30 indi-
species in the material to form silver halides26 through an inter- cated a net ionic conductivity of 10–9 S/cm, which is of similar
mediate reaction involving HI or HBr. Since HBr and Br2 are order as its electronic conductivity in ambient atmosphere. The
less volatile compared to their iodide counterparts, the reaction connected perovskite structure has been shown to facilitate
is slower in case of the bromide-based perovskites enabling anionic conduction in several oxide perovskites as well.
possible modulation of the rate of conductance change and Experiments on a Pb/MAPbI3/AgI/Ag reaction cell (Figure
hence the learning rate of artificial synapses by modulating 3b–d) indicated that the application of a negative bias at
the anionic compostion. Although there are several reports on the Ag electrode resulted in the formation of PbI2 at the
memristive and neuromorphic devices based on this mecha- Pb/MAPbI3 interface, proving that iodide ions are the fastest
nism with perovskite directly exposed to metals,27,28 the role moving species. The reduction in ionic conductivity with
of HP in such cases seem to be to primarily act as a scaffold increasing partial pressure of iodine (Figure 3e) suggested that
for filament formation. Although this configuration portrays a iodide vacancies are the major ionic charge carriers. This was
minimal electrode-HP-electrode structure without additional also corroborated by energy-dispersive spectroscopy (EDS)
layers, the long-term cyclability of these devices could be an mapping, which showed accumulation of iodide ions at the
issue considering the limited reversibility of such reactions positive electrode side (Figure 3f–g).31
with byproducts such as AgI facilitating further degradation.26 Such halide vacancy migration can create low resistance
paths on application of higher voltages by formation of fila-
Intrinsic ion migration ments leading to increased electronic conductivity. These
Anomalous polarization phenomena in perovskite solar cells filaments can be broken on demand by applying voltages
such as photocurrent hysteresis, giant dielectric constants and of opposite polarity, resulting in strong memresistance
switchable photovoltaic effects gave the first clues for the pres- (Figure 2b). Since additional layers can be inserted between
ence of ionic migration in HPs. Direct measurement of ionic the perovskite and electrode layer limiting the reaction

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

Figure 3.  (a) Pb 4f x-ray photoelectron spectroscopy spectra of samples with Al, Yb, Cr, Ag, and Au metals on various perovskite films.
All perovskite/metal interfaces show evidence of redox chemistry indicated by the presence of a Pb0 peak except for Au. Reprinted with
permission from Reference 25. © 2016 ACS Publications. (b) Schematic of the emf cell + Pb|MAPI|AgI|Ag−, (c) image and (d) x-ray diffraction
analysis of the A and B interfaces of the reaction cell after flowing finite amount of current, showing formation of PbI2 at the Pb|MAPI
contact. Reprinted with permission from Reference 29. © 2015 Wiley. (e) Variation of ionic conductivity (red line) and electronic conductivity
(black line) of MAPbI3 with iodine partial pressure. Increased iodine partial pressure reduces the ionic conductivity by passivating the iodine
vacancies and leading to better electronic conductivity. Reprinted with permission from Reference 30. © 2019 American Chemical Society.
(f, g) Scanning electron microscope and energy-dispersive spectroscopy images showing halide ion accumulation at the interfaces on
application of a bias. Reprinted with permission from Reference 31. © 2017 Wiley. (h, i) PTIR images showing the accumulation of the
organic cation in MAPbI3 scale bar is 20 mm, and (j) locally induced n- and p-regions observed through Kelvin probe force microscopy
(KPFM). Scale bar = 6 mm. Reprinted with permission from Reference 34. © 2015 Wiley. (k) PPF index variation with increasing pulse
interval: comparison of MAPbBr3, FAPbBr3, and CsPbBr3. (l) Hebbian spike-timing dependent plasticity (STDP) variant realized in halide
perovskite synapses, widely considered as the first law of synaptic plasticity.5 Note: LTP, long-term plasticity.

with electrodes, devices operating through this mechanism layer can slow down the back diffusion of ions enabling
can be much more stable compared to interfacial reaction long-term temporal effects.
mechanism. The phenomenon can also be fine-tuned by The methylammonium cation in MAPbI3 is known to
additional organic layers such as poly(3,4-ethylenedioxy- migrate slower than the halide ion. The upper limit for the MA+
thiophene) poly(styrene sulfonate) (PEDOT:PSS), which diffusion coefficient obtained from 1H NMR and tracer diffu-
could trap mobile ions leading to subtle changes in conduc- sion experiments was 4 × 10–15 cm2/s,32 about six orders slower
tivity enabling emulation of more complex synaptic behav- than iodide diffusion (2.4 × 10–8 cm2/s).29 Transient capaci-
ior. Such devices can emulate several synaptic functions, tance studies33 corroborate this observation and reveal that
including short- (e.g., paired-pulse facilitation/PPF—an even though the concentration of MA+ ions is one order higher
important form of plasticity that contributes to filtering than iodide ions, they exhibit slower diffusion (∼10–12 cm2/Vs)
and localization) and long-term plasticity (e.g., spike- as opposed to the iodide ions (10–9 cm2/Vs). Nevertheless,
timing-dependent plasticity/STDP—an important form of photothermal-induced resonance (PTIR) microscopy studies
plasticity that contributes to associative learning and con- (Figure 3h–i) on thin films have indicated aggregation of MA+
ditioning). While the fast halide ion migration could be ions under electrical bias and illumination, indicating that
attributed to short-term temporal effects, the organic cation MA+ ions may migrate at high enough fields.34 Although this
in mixed dimensional perovskites as well as PEDOT:PSS may not be sufficient to induce low-resistance paths through

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filament formation, it could lead to doping and modulation of maximize the switching performance. Systematic investiga-
injection, thus causing subtle changes in conductivity neces- tions are required to evaluate lead-free alternatives37 such as
sary for synaptic devices. bismuth, antimony, and tin-based systems to address toxicity
issues and evaluate stability of the switching materials. The
Interfacial doping concept of ionic-electronic coupling for application in neu-
Filament formation via halide migration/electrode reaction as romorphic devices can be extended to other halide perovskite
previously discussed will lead to abrupt changes in resistance inspired defect tolerant compounds such as NaSbS2.38 Other
of the material and is more suitable to resistive memories with properties that could be exploited include the tendency for
limited number of states. Neuromorphic devices, on the other halide perovskites to undergo phase transitions at lower
hand, demand multiple conductance states that need to be applied temperatures. For example, MAPbI3 has three struc-
accessed on demand via temporally correlated signals (input tural phases: a cubic Pm-3 m phase above 330 K, a tetrago-
voltage pulses that are related to each other when considered nal I4/mcm phase from 160 to 330 K, and an orthorhombic
as a series collected over time from a fixed sampling point) Pnma phase below 160 K.39 The phase-transition process is
or blind update schemes (symmetric voltage write-pulses of typically accompanied by changes in other physical features,
constant magnitude that are applied to devices to achieve a such as absorption and photoluminescence behaviors of the
linear change in conductance without the need for an addi- materials. Since such transitions can also be induced by
tional read operation). Halide perovskites exhibit a unique other external stimuli (e.g., pressure and light), they can, in
property called defect tolerance that maintains the excellent principle, be used for all-optical “write–read–erase” memory
semiconducting properties despite the presence of crystallo- and neuromorphic devices.
graphic defects due to the presence of ns2 electrons (These From a materials design perspective, most of the investigations
outer shell s electrons can hybridize with halide orbitals to rely on 3D perovskites optimized for photovoltaics and often
form antibonding valence-band maximum), a high dielectric overlook the more resistive lower-dimensional perovskites.40 As
constant, and the presence of the heavy element at the B site.4 indicated earlier, the use of a large organic cation results in the
This property allows motion of ions to subtly change the elec- formation of lower-dimensional 2D, 1D, or 0D halide perovskites.
tronic conductivity and injection as demonstrated in switch- A majority of the templating organics in low-dimensional HPs
able photovoltaic devices32,35,36 (Figure 2c–d). For example, feature frontier orbitals not capable of “interacting” with those
PTIR and KPFM studies have shown MA+ ion accumulation of inorganic lattices, and thus the semiconducting nature of the
near the electrodes (Figure 3h–j) resulting in n-type doping materials is dictated mainly by the inorganic B–X components.
near the electrodes. Similar ionic-electronic coupling effects Specifically, as the dimensionality decreases, the bandgaps
leading to doping has been observed in lead-free perovskites are found to increase from 3D to 0D HPs as there are fewer
and compounds with similar orbital structures36 and has been atomic orbitals of B2+ and X– available to contribute to the
implemented as low-power artificial synapses recently where bands of the material.41 In addition, the insulating nature of the
synaptic weights were tuned based on the size of the cationic organic cations in low-dimensional HPs also provides dielectric
species.5 Larger organic cations of methylammonium and for- “barriers” to the inorganic lattices leading to strengthened
mamidinium exhibited higher modulatable short-term plas- excitonic binding energy and oscillator strength, relative to
ticity (STP), long-term plasticity (LTP), and STDP functions 3D materials,42,43 which can be engineered to suit different
compared to the inorganic cesium, in correlation with their memory applications44 with diverse switching mechanisms. If
activation energies for ion migration (Figure 3k–l). Field- the templating organic cation in low-dimensional HPs features
assisted ionic drift and built-in voltage-assisted ionic back a small HOMO-LUMO gap, the relatively close overlap
diffusion resulted in self p- and n-doping of the perovskite between energetic levels enables charge-transfer interactions
active layer and the transport layer interfaces upon application between the organic and inorganic components.45,46 As such,
and removal of poling voltages, modulating the carrier injec- the absorption,47 electronic, and conductivity properties of the
tion barriers and hence the conductivity. Permanent pinning overall material can be modulated. The low ionic conductivity
of ions at the PEDOT:PSS/perovskite and bathophenanthro- and better stability of the low-dimensional perovskites can
line (BPhen)/perovskite interfaces at sufficiently large spike influence the intrinsic ion migration mechanism and the
widths and numbers resulted in LTP, while the interplay of interfacial reactions. In addition, the difference in interaction
drift-diffusive ionic kinetics induced temporal correlations of the orbitals in these materials compared to 3D perovskites
within the device, as evident from PPF and STDP functions. can alter the defect tolerance properties and hence influence
interfacial doping. Although the present report primarily
Future directions focuses on electronic-ionic coupling-induced phenomena,
Despite the promising results previously discussed, HP-based halide systems also demonstrate other interesting ­phenomena
memristive implementations still lag in terms of the switch- such as optical polarization,48 piezoelectricity,49 spin-dependent
ing speed, cycling endurance, and data retention time with charge transport,50 and ferroelectricity and ferromagnetism,51
respect to their mature oxide counterparts and require further which could make them relevant for neuromorphic devices
methodical studies to establish material-design criteria to based on alternative photonic or spintronic architectures.

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

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P.C. Harikesh  is a research staff member Benny Febriansyah is a research staff member
in the Energy Research Institute at Nanyang in the Energy Research Institute at Nanyang
Technological University (NTU), Singapore. Technological University (NTU), Singapore. He
He received his PhD degree from the received his BS degree in chemistry and bio-
Interdisciplinary Graduate School, NTU, in logical chemistry in 2015 and his PhD degree
2020. His research included antimony-based in 2020 from NTU. His current research focuses
perovskite-inspired compounds for photo- on understanding the structure−optoelectronic
voltaics. His current research focuses on the properties correlations in functional low-
investigation of ionic-electronic-coupled semi- dimensional hybrid perovskites, and improving
conductors for novel optical and electronic the stability and large-scale processability of
applications. Harikesh can be reached by email perovskite photovoltaics. Febriansyah can be
at harikesh001@e.ntu.edu.sg. reached by email at benn0005@e.ntu.edu.sg.

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Hybrid organic–inorganic halide perovskites for scaled-in neuromorphic devices

Rohit Abraham John  is a research fellow at Nripan Mathews  is an associate professor


Nanyang Technological University (NTU), and Provost’s Chair in Materials Science and
Singapore. He received his PhD degree Engineering in the School of Materials Science
from NTU in 2019. His research focuses and Engineering at Nanyang Technological
on neuromorphic electronic devices, oxide University (NTU), Singapore. He obtained
semiconductors, thin-film transistors, and his bachelor’s degree in materials engineer-
memory devices. John can be reached by email ing from NTU and his MSc degree under
at rohitabrahamjohn@ntu.edu.sg. the Singapore-Massachusetts Institute of
Technology Alliance. After obtaining his PhD
degree from Paris VI University, France, he
was a visiting scientist at École Polytechnique
Fédérale de Lausanne, Switzerland. His
research interests focus on the development
of novel and inexpensive electronic materials
through cost-effective techniques for electronics and energy conversion. These
include organic−inorganic halide perovskites, metal oxides, and organic thin
films. Mathews can be reached by email at Nripan@ntu.edu.sg.

MAY 2021

Submission Deadline—October 1, 2020

Understanding and Mitigating


Materials Instabilities
Materials stability in the nonequilibrium environment of an electrochemical energy storage
CALL FOR PAPERS

system is a critical issue for device operation and reliability. The shelf life of primary and
rechargeable cell chemistries, together with the cycle life of rechargeable systems, are
specifically dependent on the mechanical, crystallographic, morphological, and chemical
stability of the electrodes and the separators. The acceleration of research and development
activities into new battery chemistries to safely increase energy densities and operational
lifetime has emphasized the need to understand the root cause of cell degradation over time
and use. Examples of recent active research fronts include the chemical and crystallographic
stability of lithium-nickel oxide electrode materials, the mechanical stability of lithium-silicon
negative electrode materials, the chemical and mechanical stability of the solid electrolyte
interface (SEI) layer, and the morphological stability of both metallic sodium and lithium,
particularly with respect to dendrites and failure of the associated separator/electrolyte.
This Focus Issue will highlight approaches to understanding and solving materials instability
problems in battery systems utilizing characterization, modeling, or materials design.

Electrode phase stability and stabilization during storage and cycling


Electrode defect formation and structural degradation during cycling
and remediation approaches
SEI formation, stability and control methodologies
Solid (ceramic or polymer) electrolyte material structural and chemical stability
Characterization and control strategies for electrode-solid electrolyte interface interactions

GUEST EDITORS
Erik G. Herbert, Michigan Technological University, USA
Stephen A. Hackney, Michigan Technological University, USA
Nancy J. Dudney, Oak Ridge National Laboratory, USA
Y. Shirley Meng, University of California, San Diego, USA

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