Recent advances in flexible alternating

current electroluminescent devices

Cite as: APL Mater. 9, 030701 (2021); https://doi.org/10.1063/5.0040109
Submitted: 10 December 2020 • Accepted: 17 February 2021 • Published Online: 05 March 2021

Xin Zhang and Feng Wang

COLLECTIONS

Paper published as part of the special topic on Advanced Materials and Devices for Medical Applications

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APL Mater. 9, 030701 (2021); https://doi.org/10.1063/5.0040109 9, 030701

© 2021 Author(s).
 APL Materials ARTICLE scitation.org/journal/apm

Recent advances in flexible alternating current

electroluminescent devices
Cite as: APL Mater. 9, 030701 (2021); doi: 10.1063/5.0040109
Submitted: 10 December 2020 • Accepted: 17 February 2021 •
Published Online: 5 March 2021

Xin Zhang and Feng Wanga)

AFFILIATIONS
Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Hong Kong, China and City
University of Hong Kong Shenzhen Research Institute, Shenzhen 518057, China

a)
Author to whom correspondence should be addressed: fwang24@cityu.edu.hk

ABSTRACT
Since its first discovery by Destriau in oil dispersion of ZnS:Cu phosphors, alternating current electroluminescence (ACEL) has found
enormous applications in lighting, full-color displays, and optoelectronics. ACEL materials are particularly useful for constructing flexible
light-emitting devices owing to their low cost and easy integration with flexible electrodes and polymer substrates. ACEL devices utilizing
the phosphor-elastomer composite as the emissive layer are intrinsically stretchable/deformable, in contrast to direct current light-emitting
diodes that are often built on rigid panels. In this Research Update, we summarize recent advances in the design and preparation of various
flexible-panel ACEL devices. Emerging applications enabled by these flexible ACEL devices are also highlighted.
© 2021 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license
(http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0040109., s

I. INTRODUCTION layers.6 The new device structure renders high luminance and a
long lifetime. With the continuous improvement of performance,
Electroluminescence (EL) is the generation of light from mate- a full-color thin-film ACEL device had been successfully demon-
rials in response to the passage of an electric current or a strong strated and applied to display applications.7–10 In parallel develop-
electric field.1,2 The EL involving current flow is named injection EL, ments, steady improvements on powder-type ACEL had also been
in which electrically excited electrons and holes recombine at the p– achieved since the 1990s owing to the elimination of moisture-
n junction in light-emitting diodes (LEDs) to produce light.3,4 The induced phosphor degradation, which is critical to ensure sufficient
EL induced by an electric field is called high-field EL or alternating lifetimes.11
current electroluminescence (ACEL), as it is generally powered by A thin-film ACEL device differs from what was originally pro-
an alternating current electrical source at high voltages (>10 V). The posed by Destriau in terms of device structure and dimension.
electrical excitation in ACEL results from the localized oscillation The emissive layer (tens of micrometers) for a powder-type ACEL
of charge carriers, which process is tolerant to defects. As a result, [Fig. 1(a)] typically consists of blended composites of EL phosphors
ACEL devices can be fabricated outside of cleanroom facilities at low and an organic binder, which can be easily processed through screen
costs, which is advantageous over LEDs. printing or blade coating. By contrast, the light-emitting layer of a
The phenomenon of ACEL was discovered in 1936 when Des- thin-film ACEL device is much thinner (several hundred nanome-
triau observed luminescence from a suspension consisting of ZnS:Cu ters) [Fig. 1(b)], which is often formed by costly deposition tech-
phosphors in castor oil under a high electric field, which is now niques such as electron beam deposition and atomic-layer epitaxy.12
known as powder-type ACEL.5 However, the ACEL systems in Partly owing to the high production cost, thin-film ACEL devices
early studies were unsuitable for practical use because of the insuf- are losing their competitiveness in lighting and display applica-
ficient luminance and stability as well as the inadequate lifetime tions due to the recent development of highly bright and efficient
(several hundred hours). The breakthrough in ACEL research was LEDs.13–15
made in the 1970s, when a thin-film ACEL device was devised By virtue of the simple device configuration and cost-effective
by sandwiching a ZnS:Mn2+ film between two Y2 O3 insulating production on large scales, powder-type ACEL devices still hold

APL Mater. 9, 030701 (2021); doi: 10.1063/5.0040109 9, 030701-1

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FIG. 1. Schematic illustrations of the

multi-layered (a) powder-type ACEL
device and (b) thin-film ACEL device.

promise in certain areas, especially in the fabrication of flexible In a thin-film ACEL device, the semiconductor phosphor
light-emitting devices. For example, ACEL phosphors can be easily layer is sandwiched between two insulator layers [Fig. 1(b)]. In
incorporated into an elastomeric matrix and attain intrinsic flexi- this case, enormous interfacial states are formed with energy lev-
bility, which is hardly achievable for LEDs.16–21 Benefiting from the els distributed in the forbidden bandgap of the semiconductor.
rapid development of flexible ACEL devices, a diversity of intrigu- Under an extremely high electric field of over 106 V/cm, electrons
ing applications have emerged in recent years, such as stretch- trapped at these interfacial states are injected into the conduc-
able/deformable displays, visual readout units on arbitrary shapes, tion band due to field emission (tunneling) and/or Poole–Frenkel
and epidermal health monitoring devices.22–25 emission (field-enhanced thermal excitation of trapped electrons).11
In this Research Update, we focus on recent advances in the Injection of carriers from the interfacial states is the generally
preparation and application of flexible ACEL devices. We begin with accepted electron injection mechanism for this type of ACEL device
a brief interpretation of ACEL mechanisms in Sec. II, which is the [Fig. 2(a)].
theoretical basis for the construction of efficient ACEL devices. In In the case of powder-type ACEL, luminescence occurs when
Sec. III, we introduce the state-of-the-art flexible ACEL devices com- an average electric field reaches 104 V/cm–105 V/cm, which is two
posed of a judiciously designed electrode, substrate, dielectric com- orders of magnitude lower than that of thin-film type. Since semi-
ponent, emitting layer, and device structure. In Sec. IV, emerging conductor phosphors such as ZnS are fully embedded in a polymer
applications of flexible ACEL devices are overviewed. binder, the individual particles are insulated from each other.29 The
electron is thought to be injected from the conducting Cux S nee-
II. ACEL MECHANISMS dles that are embedded within the ZnS lattice based on the fact that
EL is only observed when Cu is added in the phosphors’ prepara-
The excitation of luminescent centers in ACEL is generally tion process. Cux S needles not only facilitate the formation of the
understood as the impact ionization or impact excitation theories.26 Schottky barrier between Cux S and semiconducting ZnS but also
In the impact ionization model, a high electric field of over 106 V/cm concentrate the local electric field by 1 and 2 orders of magnitudes.
produces and accelerates hot electrons to collide with the phos- At a high local electric field, electrons and holes are injected from
phor lattice, leading to the creation of electron–hole pairs [process 1, two ends of the Cux S needles through tunneling, respectively (bipo-
Fig. 2(a)].27 Luminescence is generated as a result of the recombina- lar field-emission model) [Fig. 2(b)].30–32 The injected electrons and
tion of electrons and holes. Impact excitation is associated with the holes are captured at luminescent centers known as donors (Al or Cl)
direct collision of hot electrons with localized luminescent centers.28 and acceptors (Cu) in ZnS:Cu/Al or ZnS:Cu/Cl. Subsequent recom-
The ground state electrons will be excited to higher energy levels, bination of electrons and holes results in electroluminescence. The
yielding luminescence [process 2, Fig. 2(a)]. The impact excitation donor–acceptor pairs may also transfer their energy to additional
mechanism is widely used to interpret the luminescence of Mn2+ or dopants such as Mn2+ in the host lattice, giving rise to tunable optical
trivalent lanthanide ions in a thin-film ACEL device. However, from emissions.
the physical point of view, powder-type ACEL and thin-film ACEL In general, the display performance of an ACEL device can be
differ in the carrier injection process. evaluated through the luminance vs voltage (L–V) plot according to

FIG. 2. (a) Energy band diagram of

a dielectric material and a semicon-
ductor in contact. Arrows illustrate the
excitation of luminescence centers in
the ACEL devices. (b) Schematic band
model showing the simultaneous injec-
tions of electrons and holes from
the opposite ends of a Cux S needle
into the surrounding ZnS:Cu/Cl lattice.
GS = ground state, ES = excited state,
CB = conduction band, and VB = valence
band.

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III. STATE-OF-THE-ART FLEXIBLE ACEL DEVICES

ACEL devices based on blended composites of phosphors and
the polymer matrix are intrinsically flexible, in stark contrast to
LEDs that require extrinsic structural designs to gain flexibility.
Similar to the conventional rigid counterparts, the basic architec-
ture of a flexible ACEL device comprises a light-emitting layer
sandwiched between two electrodes, which are both transparent to
light (Fig. 3). The separate dielectric layers usually found in a rigid
ACEL device are not necessary as the elastomer matrix that con-
stitutes the emissive layer has sufficient permittivity. In general, a
FIG. 3. General schematic illustration of a flexible-panel ACEL device, in which a
luminescent phosphor-elastomer composite is sandwiched between two transpar- high-performance ACEL device should possess the following: (1) A
ent electrodes. durable device structure tolerable to repetitive mechanical actions
(over 1000 cycles) under large strain (>100%), (2) free of electric
breakdown during the service period or the electric breakdown
the following equation:6 that can be self-healed, (3) a safe operation condition for wear-
1
able electronics (<36 V) with sufficient brightness (e.g., 100 cd/m2 –
V0 2 200 cd/m2 ), and (4) long lifetime (>50% of initial brightness for
L = L0 exp(−( ) ),
V over 3000 h). To meet these requirements, a variety of flexible ACEL
devices have been constructed by modification and optimization of
where L0 and V 0 depend on the physical properties of the emis- individual components in the flexible ACEL devices over the past
sive layer, such as the fraction of the phosphor in the composites, few years.
the particle size of the emitting phosphor, the dielectric constant of
the embedding medium, and the device thickness. One of the key A. Flexible electrode
parameters, the threshold voltage (Vth), defined as the voltage where
the luminance of 1 cd/m2 is achieved, can be extracted from the L–V Indium tin oxide (ITO) featuring high transparency (>80% in
plot. The efficiency of a typical ACEL device is usually in the range the 400 nm–700 nm region) and low resistance (∼20 Ω/sq) is the
of 1 lm/W–5 lm/W, which can be expressed by η = L1/2 V −2 . The most commonly used electrodes for optoelectronic devices. How-
lifetime, defined as the time required for the luminance to decrease ever, its applications in flexible devices are limited by the poor
to half of its initial value, is another important value to evaluate the compatibility with polymeric substrates and the low processability.
ACEL device for practical use. With continuously increasing control In addition, ITO is generally deposited on a rigid glass substrate
over moisture and improved driving techniques, the lifetime of an via sputtering techniques. Therefore, the configuration of the elec-
ACEL device producing 200 cd/m2 has been extended to more than troluminescent device is invariant (bottom emission type) as long
3000 h.6 as ITO is involved. Difficulties usually arise when using ITO to

TABLE I. Comparison of flexible ACEL devices consisting of various transparent electrodes.

Electrode Sheet resistance (R) Transparency (T) Flexibility Device performance References

ITO-PET 10 Ω/sq >80% in 400 nm– A significant increase in Luminous efficiencies 42

700 nm resistance after 1000 cyclic at 200 V 400 Hz: 1.50 lm/W
bending–recovery testing
SWCNT 5.8 kΩ/sq ∼75% at 600 nm Withstand bending or Turn-on at 35 V, (1 kHz). 34
stretching Trade-off between R and T
Graphene-PET 230 kΩ/sq (single layer) >80% in visible region Stable at a bending strain Turn at 80 V; 1140 cd/m2 at 40
(single layer) of 5.4% 480 V (16 kHz); 5.0 lm/W
Ag NW-PET 10 Ω/sq Greater than ITO in A slight change in Luminous efficiencies at 42
400 nm–700 nm resistance after 1000 cycles of 200 V 400 Hz: 1.53 lm/W
bending–recovery testing
Ag NW-PDMS N/A; PDMS constrains Resistant to twisting Turn-on at 60 V 22
Ag NWs on their or stretching; stable at a
N/A
locations and maintains stretching strain of up to 100%;
the conductivity stable performance under
the cycling test
Ionic conductor N/A ∼100% in 350 nm– Stable after 1000 cyclic Maximum luminance 23
850 nm stretching to 700% ≈95 cd/m2 , at 2 kHz

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fabricate top-emitting devices as its deposition process may dam- mechanical actions such as bending or stretching without losing
age the underlying device component.33 Although flexible ITO conductivity or emission efficiency, which overcomes the problem
based on the polyethylene terephthalate (PET) substrate is com- of brittleness for ITO-based flexible ACEL devices [Fig. 4(a)]. More-
mercially available, the low-temperature deposition technique often over, the low-temperature spray coating method is cost-effective
results in high sheet resistance and surface roughness. To overcome and can be conducted on an abundance of available substrates
the limitations of ITO, various flexible transparent electrodes such that are incompatible with sputter techniques or high-temperature
as single-walled carbon nanotubes (SWCNTs), graphene, and sil- treatments.
ver nanowires (Ag NWs) have been developed. These electrodes Graphene possesses superior optoelectronic properties, excel-
exhibit comparable electric conductivity to that of ITO, on top of lent flexibility, and high chemical stability in comparison with ITO.
overwhelming superiorities in terms of mechanical robustness and Graphene films grown by chemical vapor deposition (CVD) were
stretchability (Table I). used as the electrodes in ACEL devices.38,39 Wang et al. demon-
SWCNT was first introduced by Kaskel and co-workers as the strated that single-layer graphene-based ACEL devices showed the
alternative electrodes for ACEL devices.34 Transparent SWCNT thin optimum performance as the transparency decreased when increas-
films had been previously applied to several types of flexible devices ing the stacked layers.40 The as-fabricated device has a turn-on volt-
such as organic light-emitting diodes, polymer solar cells, and trans- age of 80 V and a brightness of 1140 cd/m2 at 480 V (16 kHz).
parent transistors.35–37 An aqueous solution of SWCNT obtained The bending test revealed good mechanical stability of graphene as
by the ultra-sonification method was easily cast by spray coating the sheet resistance and luminance of the device are largely pre-
to form a transparent thin film. SWCNT with a sheet resistance of served under a strain of 5.4% [strain ≈ (ts − tp )/2rc (ts , tp ≫ tf )]. By
50 kΩ/sq is sufficient to activate electroluminescence. Further reduc- contrast, the ITO-based counterpart failed because of the increased
ing sheet resistance will first enhance and then decrease the emis- crack density [Figs. 4(b) and 4(c)].
sion intensity due to the loss of transparency. The flexible ACEL Ag NWs with a low sheet resistance (10 Ω/sq) have been
devices based on SWCNT electrodes exhibit several advantages. widely used in the fields of electronics and microelectronics.41 Ag
The mechanically robust structure can tolerate various devastating NWs can be synthesized by wet chemical routes and coated to a

FIG. 4. (a) Photographs of SWCNT-based flexible ACEL devices, reprinted with permission from C. Schrage and S. Kaskel, ACS Appl. Mater. Interfaces 1(8), 1640 (2009).
Copyright 2009 American Chemical Society. (b) Schematic illustration of a bending graphene-based ACEL device: t s is the thickness of the PET substrate; t f is the thickness
of the graphene film; t p is the total thickness of the phosphor layer, dielectric layer, and silver electrode; r c is the radius of curvature. (c) The sheet resistance and luminance
(480 V) of the graphene-based ACEL device as a function of strain, where strain ≈ (t s − t p )/2r c (t s , t p ≫ t f ), reproduced with permission from Wang et al., ACS Nano
5(9), 7149 (2011). Copyright 2011 American Chemical Society. (d) Comparison of sheet resistance between ITO and the Ag NW with increasing bending–recovery cycles,
reproduced with permission from Park et al., J. Lumin. 165, 216 (2015). Copyright 2015 Elsevier B.V. All rights reserved. (e) Photographs of the Ag NW-based ACEL device
under mechanical manipulations of stretching and twisting. (f) Photographs of the Ag NW-based ACEL device stretched to strains of 0%, 40%, 60%, and 100%, reproduced
with permission from Wang et al., Adv. Mater. 27(18), 2876 (2015). Copyright 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

APL Mater. 9, 030701 (2021); doi: 10.1063/5.0040109 9, 030701-4

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flexible substrate at ambient temperatures. Kim and co-workers the ZnS:Cu–Ecoflex emissive layer was sandwiched between the bot-
experimentally compared the durability of bar-coated Ag NW-PET tom and top ionic conductors. Due to the large capacitance of the
with ITO-PET sheet. Both electrodes were bent to concave and con- electrical double layers formed at the ionic conductor/external elec-
vex curvatures with a 5.0 mm radius. After 1000 cycles of bending trode interfaces on each side of the device, most of the voltage was
and recovery tests, Ag NW-PET showed a slight change in sheet coupled onto the emissive layer. As a result, high luminescence
resistance [Fig. 4(d)]. By contrast, a substantial drop in conductiv- efficiency and high electrochemical stability of the ionic conductor
ity was observed for ITO-PET owing to the crack of the ITO elec- were simultaneously achieved [Figs. 5(b) and 5(c)].45 The ionic gel
trode during the cyclic test. The comparison validated the mechan- showed no noticeable changes in resistance after being repetitively
ical compliance of Ag NW electrodes.42 However, the ACEL device stretched to 700% for 1000 cycles, demonstrating great mechanical
based on both Ag NWs and ITO failed to sustain EL performance compliance of the ionic conductor. In addition, high transparency
even after 100 cycles of bending and recovery tests. The inferior (almost 100%) of the ionic conductor is independent of its conduc-
durability of the ACEL device was ascribed to the delamination of tivity. By contrast, a trade-off between transparency and conductiv-
individual functional layers at the interface, which can be solved ity is generally encountered by flexible electronic conductors such
by using a single elastomeric substrate to form a compatible struc- as CNTs and graphene [Fig. 5(d)]. The intrinsically flexible ionic
ture.43 Accordingly, Wang and co-workers demonstrated a highly conductor facilitates the fabrication of ACEL devices with excellent
stretchable and deformable ACEL device based on a single poly- mechanical robustness and stable device performance.46,47
dimethylsiloxane (PDMS) substrate and Ag NWs as both top and
bottom electrodes [Fig. 4(e)].22 The stretchable EL device was fabri-
B. Dielectric components
cated with a simple all-solution processing method and fully embed-
ded in the PDMS network. PDMS covered the whole device structure The dielectrics in ACEL devices function as the protection layer
to maintain the conductivity of the Ag NWs and the luminescence to prevent the device from catastrophic electric breakdown since
of EL phosphors. Moreover, the single substrate exerted a strong short circuits and arcing may occur in volume voids within the
bonding force to reinforce the interfaces, which opposes repeated device structure.29 Conventional structures generally comprise an
deformations such as compressing, twisting, and flexing. Excel- intentionally designed dielectric layer, which prevents the device
lent stability under large strain (up to 100%) cycles was achieved from electric breakdown. In order to ensure enough electric field in
[Fig. 4(f)]. the emitting layer, the dielectric layer should be as thin as possible
The transparent electrodes composed of SWCNT and Ag with a high dielectric constant according to the relationship of the
NWs can hardly maintain their conductivity at a tensile strain of capacitor series (C1 V1 = C2 V2 ). In addition, a thin dielectric layer
over 100%.23,44 To overcome this limitation, Lee and co-workers can also be a reflector to promote light extraction through transpar-
proposed to use intrinsically stretchable ionic conductors such ent electrodes. However, most recent designs of the flexible ACEL
as lithium percolate for the fabrication of flexible ACEL devices devices have integrated the dielectric function into the active layer
[Fig. 5(a)]. The device was based on a simple configuration, in which for reducing device thickness and achieving emissions on both sides.

FIG. 5. (a) Photographs of the ionic

conductor-based ACEL device stretched
to different strains. (b) Schematic illustra-
tion of the ionic conductor-based ACEL
device. The equivalent circuit of the
EL device shows three capacitors con-
nected in series. (c) The capacitance
of the electrical double layer and emis-
sive layer under different frequencies.
(d) Transmittance spectrum of the ionic
conductor on a glass slide, reproduced
with permission from Wang et al., Adv.
Mater. 28(22), 4490 (2016). Copyright
2015 WILEY-VCH Verlag GmbH & Co.
KGaA, Weinheim.

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improved brightness of the EL device of up to 700% compared to a

reference display with only EL particles [Fig. 7(a)].49 More than
a twofold increase in the effective dielectric constant was demon-
strated in the high permittivity composite compared to the pure
PDMS matrix [Fig. 7(b)]. As a consequence, the turn-on voltage was
decreased to 85 V (400 Hz) for EL–BaTiO3 –PDMS composite, in
contrast to 125 V (400 Hz) for the EL–PDMS composite [Fig. 7(c)].
On a side note, the emission from the EL–BaTiO3 –PDMS composite
displayed uniform emission at the microscale and maintained a good
mechanical property as verified by the stretching test, attributed to
the dense packing of the BaTiO3 –EL binary particles.
The silicone-based dielectric matrices used in most ACEL
devices are non-polar and reliant on high operating voltage to
achieve sufficient emission brightness. By using an intrinsically polar
thermoplastic elastomer (PVDF-HFP) with high permittivity (over
FIG. 6. The electric field strength of luminescent particles as a function of the ten in the frequency range for ACEL excitation), Kong and co-
volume ratio of the particles at given dielectric constants. workers realized enhanced light emission at low driven voltages.50,51
The stretchable ACEL devices are capable of providing sufficient
brightness (144 cd/m2 ) for indoor lighting at a driving voltage of
100 V (20 kHz). As an added benefit, due to the thermoplastic prop-
To attain high ACEL brightness, the local electric field around
erty of the elastomers, a strong bond between laminated layers can be
the luminescent particles should be essentially high, which can be
formed during the device fabricating process by heating and pressing
estimated through the following equation:29
treatment, resulting in a highly robust structure to endure repeated
3ε2 mechanical actions.
EZnS = Ea , In a follow-up study, the same group further boosted the
2ε2 + ε1 − φ(ε1 − ε2 )
permittivity of polar elastomers (PVDF-HFP) by filling surface-
where Ea is the average electric field across the entire emissive modified ceramic nanoparticles (BaTiO3 –PVP).24 The nanoparticle
layer (Ea = U/d), ε1 is the dielectric constant of EL phosphor, ε2 additives considerably enhanced the dielectric constant of the com-
is the relative dielectric constant of the surrounding matrix, and φ posite by threefolds in comparison with the base elastomer, result-
is the volume ratio of the phosphor particles in the emissive layer. ing in an extremely high permittivity (>30) in a large frequency
The plots of local field vs volume fraction at given dielectric con- range (100 Hz–20 kHz) [Fig. 7(d)]. As a result, the nanocomposite
stants (ε1 and ε2 ) are shown in Fig. 6. A high permittivity sur- ACEL device showed a turn-on voltage at only 10 V and an achieved
rounding matrix permits a strong local field around EL phosphors, brightness of 113 cd/m2 at 35 V [Fig. 7(e)]. Based on the achieve-
leading to improved excitation efficiency at a given input voltage ment, an epidermal stopwatch with compliant mechanical proper-
(Table II).48 Meanwhile, an obvious trade-off between the local elec- ties for seamless integration with the human body was demonstrated
tric field and the EL phosphor fraction is displayed; hence, a balance [Fig. 7(f)]. The results highlight the potentials of flexible ACEL
between the local electric field and particle packing density should devices for wearable applications.
be considered to render enough brightness. In a parallel development, Tee and co-workers chose high per-
By modifying the emissive composite with high permittiv- mittivity poly(vinylidene fluoride) (PVDF) as the dielectric matrix.
ity (ε) additives (BaTiO3 ), Stauffer and Tybrandt achieved an A small amount of non-ionic fluorinated surfactant (FS300) was

TABLE II. Comparison of flexible ACEL devices composed of modified dielectrics.

Strategy Dielectric property Flexibility Device performance References

High ε BaTiO3 additives Over a twofold increase in ε Stable emission over Decreased turn-on voltage (85 V); 49
500 strain cycles a sixfold increase in brightness
High ε elastomer ε > 10 over the frequency Uniform emission Stable emission within the frequency 50
(e-PVDF-HFP) range of ACEL use under different tensile range from 400 Hz to 20 kHz;
strains (0%–100%) luminance reaches 785 cd/m2
at 180 V, 20 kHz
High ε elastomer with Largely boosted ε (>30) Stable emission by Turn-on at 10 V; luminance reaches 24
BaTiO3 nanofillers from 100 Hz to 20 kHz tensile deformations 113 cd/m2 at 35 V, 17 kHz
High ε elastomer with High ε value between Stable emission up to Turn-on at 23 V, <1 kHz 5 cd/m2 , 52
surfactant 10 and 27 a maximum of 800% strain at 100 V, 50 Hz

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FIG. 7. (a) Schematic illustration of the BaTiO3 modified ACEL device. The display stacks comprise a bottom Ag NW electrode, a layer containing EL particles and BaTiO3
particles, and a top Ag NW electrode. (b) Measured frequency-dependent dielectric constants of PDMS, EL–PDMS, and EL–BaTiO3 –PDMS. (c) Luminance as a function
of voltage (400 Hz square wave) for EL–BaTiO3 –PDMS- and EL–PDMS-based EL devices, reprinted with permission from Stauffer and Tybrandt, Adv. Mater. 28(33), 7200
(2016). Copyright 2016 Author(s) licensed under a Creative Commons Attribution 4.0 license. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Frequency-
dependent dielectric constants of the nano-BaTiO3 filled and pristine PVDF-HFP elastomer. The inset shows a schematic describing the composition of the nanocomposite
consisting of BaTiO3 (BT)/poly(vinyl pyrrolidone) (PVP) core–shell nanoparticles embedded in a PVDF-HFP elastomer. (e) Luminance vs driving voltage (17 kHz square
wave) for nano-BaTiO3 modified and pristine PVDF-HFP-based EL devices. (f) Photographs of the epidermal stopwatch, reprinted with permission from Zhou et al., ACS
Mater. Lett. 1(5), 511 (2019). Copyright 2019 American Chemical Society.

added to enhance the stretchability. The fluorosurfactant also providing guidance for the development of green and sustainable
improved ε through the realignment of its dipole centers under an flexible electronics.54,59,60
electric field. Owing to the high ε dielectric composite, the thin To solve the problem of poor reliability, self-healing sub-
ACEL device was turned on at 23 V and attained a luminance of strate materials have been developed. In a fascinating demon-
5 cd/m2 at 100 V (50 Hz).52 stration by Liang et al., a self-healable polyacrylic acid hydro-
gel and self-healable polyurethane were chosen as the electrode
and the phosphor encapsulation matrix, respectively. The device
C. Substrate materials
was able to renovate and revive its performance after undergo-
Despite the improved performance of light emission and ing cyclic cuts, demonstrating considerably enhanced reliability
mechanical stability, the reliability of flexible ACEL devices is [Figs. 8(a) and 8(b)].61
still unsatisfactory. For example, device failure often results from Hydrogen bonds are generally believed to account for self-
repeated mechanical actions. Moreover, the extensive use of poly- healing properties. By destructing the hydrogen bond, however, Cho
meric substrates in soft electronics also raises environmental issues and co-workers showed that pristine elastomeric poly(urethane)
by producing electronic wastes.53,54 To this end, the upgrading of (PU) could be tailored to the viscoelastic and gum-like composite
substrate materials is also constantly reported.55–57 for attaining self-healing properties as well.62 This was enabled by
In an early demonstration, Kim et al. evaluated the possibil- the introduction of a certain amount of triton X-100 (TX) as a plas-
ity to deposit ACEL devices on paper substrates, which are, unlike ticizer. TX blocked the cross-linking of the hard segments in PU,
the plastic substrates, disposable.58 A spin-on-glass layer was served and the breaking of hydrogen bonds was verified by the decrease in
as the protecting layer to avoid moisture and thermal damage. The absorption at 3340 cm−1 corresponding to hydrogen-bonded N–H
device exhibited equal ACEL performance compared to a PET-based stretching in the Fourier transform infrared (FT-IR) spectra. Most
counterpart and showed no deterioration in luminance and flexibil- importantly, the electric field breakdown could be consecutively
ity performance, making it possible to fabricate sustainable paper- recovered, substantially boosting the reliability and lifetime of the
based EL devices at low costs. Considering the environmental friend- EL device [Fig. 8(c)].
liness, flexible ACEL devices that utilized degradable PVA, sliced Self-healing was also reported for high permittivity elas-
veneer, and even fish gelatin films as substrates were demonstrated, tomer PVDF by the introduction of a surfactant (FS300) with

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FIG. 8. (a) Demonstration of cutting–

healing process of the healable EL
device and (b) the assembly of two
EL devices into a single “T” light-
emitting letter, reprinted with permission
from Liang et al., Light: Sci. Appl. 7,
102 (2018). Copyright 2018 Author(s),
licensed under a Creative Commons
Attribution 4.0 license. (c) Schematic
illustration of the self-recovery of the self-
healing EL device after consecutive elec-
trical breakdowns, reprinted with permis-
sion from Cho et al., Adv. Opt. Mater.
7(3), 1801283 (2019). Copyright 2018
WILEY-VCH Verlag GmbH & Co. KGaA,
Weinheim. (d) Photographs showing that
the damaged self-healing EL device can
re-illuminate immediately after placing
the interfaces together and applying gen-
tle pressure. The red rectangle indicates
the cut and healed region of the sam-
ple, reprinted with permission from Tan et
al., Nat. Mater. 19(2), 182 (2020). Copy-
right 2019, The Author(s), under exclu-
sive license to Springer Nature Limited.

abundant fluorine groups [Fig. 8(d)].52 The synergistic inter- on the multicolor tuning of ACEL devices are mainly based on the
molecular interactions between the fluoroelastomer chain and use of phosphor mixtures.
the surfactant were responsible for the self-healing properties. Wood and co-workers demonstrated a full-color ACEL dis-
Furthermore, the dielectric elastomer could heal at a low tem- play by combining ZnS-based electroluminescent phosphor and
perature (−20 ○ C) owing to its extremely low glass transition the photoluminescent quantum dots (QDs).64 The device resem-
temperature (−25 ○ C). bles a phosphor-converted LED, in which CdSe/ZnS QDs re-absorb
The use of self-healing substrate eliminates the concern about the blue electroluminescence from ZnS:Cu phosphors and gener-
the failure of the ACEL device. Self-healable materials can substan- ate additional emission bands in the green and red spectral regions
tially enhance the reliability of an ACEL device as they can self- [Fig. 9(a)].65 In addition, the colloidal QDs could be readily incor-
repair mechanically and electronically and at the same time attain porated into a polymer matrix and form luminescent inks, which
comparable electroluminescence performance with the device based allowed for inkjet printing of large-area patterns for multi-color
on common silicone substrates such as PDMS. Specifically, PVDF flexible ACEL displays [Fig. 9(b)].
modified with a surfactant (FS300) gains boosted permittivity (also In another recent development, Zuo et al. demonstrated a
self-healable), thus permitting enhanced ACEL performance of the color-tunable electroluminescent device based on an elaborately
fabricated device.52 designed device composed of double-stacked emissive layers with
The use of flexible electrodes and stretchable elastomer sub- different dielectric constants.66 The color tunability stems from
strates endows ACEL device flexibility. With a continually improved the dielectric difference between the polymer matrices, which
structural design and upgraded materials of each functional parts, leads to redistribution of the electric field within the active lay-
the ACEL devices become more and more immune to mechanical ers [Fig. 9(c)]. As a consequence, real-time color tuning through
stimulation and even mechanical damage. On the one hand, these orange–white–blue was attained by controlling the driving voltage
ACEL devices can withstand repeatable mechanical actions with- [Fig. 9(d)].
out changes in shape and performance. On the other hand, the
devices can even be repaired from deadly damage (cut or electrically E. Device structure
breakdown) once a self-healing substrate is involved.
The performance of ACEL devices has been largely improved
as a result of advances in the functionalities of the individual com-
D. Emitting layer ponent. Meanwhile, efforts have also been devoted to exploiting
The search for novel phosphor materials has been met with reformative device configurations, which may bring up improved
very limited success since the discovery of ACEL 80 years back. To performance and novel functions to meet requirements for various
date, ZnS is still the only available ACEL phosphor in the market.63 applications.67
Although multiwavelength emissions have been achieved in ZnS by In an encouraging report, Ma et al. enhanced the brightness
doping different ions (e.g., Cu/Cl at 450 nm, Cu/Al at 540 nm, and of the ZnS:Cu-based ACEL device by inserting a vertical copper
Cu/Mn/Al at 590 nm), the emission intensities are not equally high, oxide (CuO) nanowire array between the back electrode and the
and the emission profile can hardly be tuned further. Recent efforts phosphor layer [Fig. 10(a)].68 This design was set up on the bipolar

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FIG. 9. (a) Schematic illustration of

the ACEL device structure with QD-
polyisobutylene pixels and (b) the corre-
sponding blue, green, and red electro-
luminescence spectra, reproduced with
permission from Wood et al., Adv. Mater.
21(21), 2151 (2009). Copyright 2009
WILEY-VCH Verlag GmbH & Co. KGaA,
Weinheim. (c) Schematic illustration of
the ACEL device with double-stacked
emissive layers between two electrodes.
(d) Photographs of the ACEL device
showing the color change from orange
to white and to blue at different applied
electric fields (top) and the real-time
color change in a flexible ACEL device
with a chameleon shape with increas-
ing electric fields from 1 V μm−1 to
7 V μm−1 (bottom), reproduced with per-
mission from Zuo et al., Adv. Funct.
Mater. 30, 2005200 (2020). Copyright
2020 WILEY-VCH Verlag GmbH & Co.
KGaA, Weinheim.

field-emission model of ZnS:Cu, in which Cux S nanoprecipitates emission could also result from directly finger touching on the sur-
enhanced the local electric field and ejected electrons/holes to the face of the panel, showing a great potential in the fabrication of
ZnS lattice. An extrinsically designed CuO nanowire array plays interactive electronic devices [Fig. 10(f)].
the same role as Cux S, thus enhancing the electric field near the Song and co-workers reported another type of novel flex-
nanowire tip. The CuO nanowire was synthesized by direct oxida- ible device based on textile-fiber-electrodes that are embedded
tion of a pure copper plate substrate, followed by sedimentation in light-emitting composites.78 The conductive fibers were par-
of ZnS:Cu phosphor microparticles. PMMA was used to stabilize allelly arranged and alternatively connected to two terminals of
the device structure. A stable heterogeneous junction structure was an AC power source to generate in-plane AC fields [Figs. 10(g)
formed between CuO nanowires and ZnS:Cu phosphors, resulting and 10(h)]. By virtue of the radially distributed electric field,
in lower threshold voltage and improved brightness [Fig. 10(b)]. this design bypassed the stringent requirement for a thin emit-
The same concept was applied to light up an oxide-based ting layer and could achieve strong EL intensities in thick lay-
Zn2 GeO4 :Mn phosphor, resulting in significantly reduced thresh- ers. As a result, simultaneously high EL and mechanolumines-
old voltage [Fig. 10(c)].69 The electric field enhancement was veri- cence intensities were achieved. Moreover, patterned EL could be
fied by two-dimensional (2D) static electric field simulations (Agros easily achieved by directly arranging the placement of the fiber
2D 3.2), revealing a 250-fold field enhancement at the tips of the electrodes.
nanowires. As field enhancement effects are widely found in a diver- ACEL wires with a coaxial structure have also been constructed
sity of nanostructures such as ZnO nanowires,70 tetrapod-like ZnO to attain the features such as adaptability and wearability.79 In a rep-
whiskers,71 SiC whiskers,72 and shortened CNTs,73,74 this design resentative demonstration, Liang et al. developed an electrolumines-
may be developed as a general approach for constructing efficient cent wire by coaxially depositing ACEL components on a PET fiber
ACEL devices using various phosphors.75,76 substrate [Fig. 10(i)]. Ag NWs were used as both inner and outer
In addition to modifications of the planar structure, novel electrodes, and the device was encapsulated by silicone elastomers,
device configurations are also reported. In an intriguing example, Xu which electrically insulated the ACEL constitute from the environ-
et al. devised a polar-electrode-bridged ACEL (PEB-ACEL) device ment. The electroluminescent fiber could safely work in water and
geometry, which was free of transparent electrodes and could emit on the human skin. Due to the excellent flexibility and mechanical
light through a polar material [Fig. 10(d)].77 Unlike a sandwich stability, a wearable fabric was demonstrated.80
structure, the two electrodes were placed in parallel and coplanar.
A modulating electrode layer composed of polar materials or elec-
trically conducting films was used to bridge the coplanar electrodes IV. EMERGING APPLICATIONS OF FLEXIBLE ACEL
and excite the luminescence process. During the measurement, polar DEVICES
liquids (such as water, NaCl solutions, ethanol, and ethanol gly- Flexible ACEL is the only mature technology for uniform light
col), conductive solid (graphite, Al or Au film, and Zn powder), emission over large surfaces. The intrinsically flexible ACEL devices
and transparent hydrogel film could play the role of electrode bridge exhibit good mechanical compliance and can be adaptive to any
and initiate light emission [Fig. 10(e)]. More interestingly, light mechanical actions. These appealing attributes together with the

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FIG. 10. (a) Schematic of the ZnS:Cu phosphor particles accommodated on the top of the vertically aligned CuO nanowire array that is synthesized by thermal oxidation. (b)
Comparison of the measured luminance between ZnS:Cu-based ACEL devices with and without an aligned CuO nanowire array, reused with permission from Ma et al., ACS
Appl. Electron. Mater. 2(7), 1855 (2020). Copyright 2020, American Chemical Society. (c) Electroluminescence spectrum of the Zn2 GeO4 :Mn-based ACEL device with a CuO
nanowire array, reprinted with permission from Ma et al., Angew. Chem., Int. Ed. 57(35), 11267 (2018). Copyright 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (d)
Schematic illustration of the PEB-ACEL device with two parallel electrodes. (e) Photographs of the panel PEB-ACEL device that emits light when pouring drinking water onto
the upper surface. (f) Light emission of the panel PEB-ACEL device resulting from the use of a human hand as a polar electrode bridge, reproduced with permission from
Xu et al., Adv. Mater. 29(41), 1703552 (2017). Copyright 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (g) Schematic illustration and (h) photograph of light
emission of the textile-fiber-electrodes embedded ACEL device. The fibers are parallelly arranged and alternatively connected to two terminals (marked with block letters “A”
or “B”) of the AC power source, reproduced with permission from Song et al., Mater. Today 32, 46 (2020). Copyright 2019 Elsevier Ltd. All rights reserved. (i) Photograph
of the as-fabricated ACEL fiber, reprinted with permission from Liang et al., Adv. Electron. Mater. 3(12), 1700401 (2017). Copyright 2017 WILEY-VCH Verlag GmbH & Co.
KGaA, Weinheim.

low costs in production and power consumption have inspired a electric field.22 The assembled device displayed a shape change as
great number of novel applications such as dynamic shape dis- a function of the applied bias and achieved an area strain of up
plays, wearable electronics, and self-powered electroluminescent to 55%. Meanwhile, the upper EL device maintains stable light-
devices.81–83 emitting performance under various strained conditions [Figs. 11(a)
and 11(b)].
In another intriguing demonstration, Larson and co-workers
A. Dynamic shape display
constructed a crawling robot coated with an electroluminescent
Stretchable EL devices can maintain their functionalities when skin, which was constructed by bonding together an electrolumi-
they are subjected to various mechanical deformations such as fold- nescent device with a pneumatic actuator.85 The pneumatic actua-
ing, bending, flexing, twisting, and stretching.83,84 Specifically, the tor with a series of inflatable chambers could create an undulating
assembly of a stretchable EL device with an elastomer actuator offers gait when the chambers are alternatively inflated. Dynamic shape
the structure a new feature of the dynamic shape display. Wang and displays and active color changes were demonstrated through this
co-workers demonstrated a self-deformable EL device by deposit- design [Fig. 11(c)]. Furthermore, tactile sensing was also realized by
ing a stretchable ACEL device on a dielectric elastomer actuator monitoring the capacitance change as a function of the externally
(DEA), which could generate motions in response to an applied applied pressure.

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FIG. 11. (a) Schematic illustration of the self-deformable EL device and (b) emission photographs of the device at various area strains under increasing driving voltages,
reproduced with permission from Wang et al. Adv. Mater. 27(18), 2876 (2015). Copyright 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Photographs of the
crawling robot with a color skin, reprinted with permission from Larson et al. Science 351(6277), 1071 (2016). Copyright 2016, American Association for the Advancement
of Science. (d) Photographs of a soft robotic rover mounted with a colorimetric sensor. UV radiation sensing is demonstrated, reprinted with permission from Lee et al.
Adv. Mater. 32(22), 1907477 (2020). Copyright 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) Schematic illustration of the interactive skin display and (f)
photographs of the EL intensity variation with sweat concentrations of 10 × 10−3 m (left) and 160 × 10−3 m (right), reproduced with permission from Kim et al., Adv. Sci.
6(13), 1802351 (2019). Copyright 2019 Author(s), licensed under a Creative Commons Attribution 4.0 license. (g) Photographs of the self-powered flexible ACEL device at
“off” (left) and “on” (right) states, reprinted with permission from Fang et al., Nano Energy 20, 48 (2016). Copyright 2015 Elsevier Ltd. All rights reserved. (h) Schematic of the
droplet-driven self-powered device and (i) electroluminescent photos of droplets striking from four falling heights, reprinted with permission from Zhao et al., Nano Energy 75,
104823 (2020). Copyright 2020 Elsevier Ltd. All rights reserved.

B. Bionic electronic skin crystal, surface morphology control, radiative reflection, and chemi-
cal fluorophore. Flexible electronics provide a solution to artificially
Organisms can change their skin color for camouflage, protec- imitate this feature of biological systems. In a recent demonstra-
tion, or signaling through a host of mechanisms including photonic tion, Lee and co-workers reproduced a radiation-responsive color

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change by leveraging ACEL of ZnS and its efficient photolumines- diversity of flexible electronic systems in the role of light emission
cence under UV excitation.86 The electroluminescence and photo- components and visualization sensors.
luminescence can be independently adjusted by AC frequency and Despite the considerable achievements, the full requirements
UV power, resulting in a wide range of color variations. Visual on flexible ACEL devices have yet been fulfilled. To continuously
encryption/sensing electronic skins were demonstrated to mimic the improve the performances of the device, future attention should
camouflage and signaling functions in nature [Fig. 11(d)]. be directed to boosting the permittivity (dielectric constant) of the
substrate, modifying the local structure around the EL particles
C. Visual health monitoring devices (enhance the local electric field), and reducing the size of the elec-
troluminescent phosphors (smaller particle for more uniform and
The development of epidermal health monitoring devices void-free layers). As the primary concern of a flexible ACEL device is
hinges on electronic devices that could detect and visualize the epi- the flexible reliability, mechanical compliance and self-healing capa-
dermal environment change in human bodies. To this end, Kim and bility should be the issues of most concern in selecting substrate
co-workers demonstrated an interactive skin display comprising an materials.
epidermal electrode, which can directly sense and visualize a vari- To further release the potential of ACEL, novel phosphor mate-
ety of epidermal stimuli, such as temperature, sweat gland activity, rials are also urgently needed. Currently, efficient ACEL is chiefly
and pressure.25 The device was composed of a patterned elastomeric reliant on ZnS crystals, which render very limited color output. The
PDMS-ZnS composite and two in-plane placed transparent elec- small cation sites in the host lattice can only accommodate a small
trodes in a simple two-layer architecture [Fig. 11(e)]. The sensing number of well-selected dopant ions for optical tuning. Future stud-
mechanism was based on a variation of capacitance and impedance ies may be directed to host materials with a larger cation site that per-
that affects the AC electric field distribution and, thus, the EL inten- mits lanthanide doping. The enormously complex 4f energy levels of
sity. Epidermal stimuli can be directly visualized by the electrolumi- lanthanide ions could enable full-color ACEL devices, in addition to
nescence upon placing the device on the human skin, demonstrat- providing a general platform for the mechanistic investigation of the
ing great superiority for multi-functional and multi-mode health electroluminescence process. The existing EL theories are primarily
monitoring [Fig. 11(f)]. based on observations from specially prepared ZnS crystals. Care-
ful characterization of various material compositions and structures
D. Self-powered electroluminescent devices could shed additional light on EL processes and may reveal new EL
Owing to their high adaptability, flexible ACEL devices can be routes, which, in turn, could inspire the design of more efficient EL
integrated with triboelectric nanogenerators (TENGs) to realize self- materials and device architectures. The use of innovative method-
powered electroluminescence.87–89 TENGs can convert ubiquitous ologies such as in situ single-particle studies may be helpful in this
mechanical energy from the ambient environment into electricity effort.
for driving the ACEL display, thereby eliminating the need for other
power sources.90 In a recent work, Fang and co-workers demon- ACKNOWLEDGMENTS
strated an integrated ACEL device comprising a built-in TENG.
The TENG was based on nylon and PTFE friction layers and could This work was supported by the Research Grants Council of
induce a local electric field of up to 106 V/m around the ZnS:Cu/Al Hong Kong through a Research Fellowship Scheme (Grant No.
particles, which is sufficiently high to excite the electroluminescence RFS2021-1S03).
process [Fig. 11(g)].91 In another development, Zhu and co-workers
developed a self-powered EL device, which enables droplet-impact- DATA AVAILABILITY
driven light emission.92 The device was based on a simple flexible Data sharing is not applicable to this article as no new data were
configuration, with an EL layer sandwiched between two fluori- created or analyzed in this study.
nated ethylene propylene (FEP) thin films. The layered structure was
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