Molecules: Recent Advances in The Polymer Dispersed Liquid Crystal Composite and Its Applications

molecules
Review
Recent Advances in The Polymer Dispersed Liquid
Crystal Composite and Its Applications
Mohsin Hassan Saeed 1,† , Shuaifeng Zhang 2,† , Yaping Cao 1 , Le Zhou 1 , Junmei Hu 2 ,
Imran Muhammad 1 , Jiumei Xiao 3 , Lanying Zhang 1, * and Huai Yang 1, *
1 Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, Department of Materials
Science and Engineering, College of Engineering, Peking University, Beijing 100871, China;
mohsin@pku.edu.cn (M.H.S.); 1701111605@pku.edu.cn (Y.C.); zhoule@pku.edu.cn (L.Z.);
imrankhanization@pku.edu.cn (I.M.)
2 Beijing Advanced Innovation Center for Materials Genome Engineering, Department of Materials Physics
and Chemistry, School of Materials Science and Engineering, University of Science and Technology Beijing,
Beijing 100083, China; shuaifengustb@163.com (S.Z.); junmeihu2019@163.com (J.H.)
3 Department of Applied Mechanics, University of Sciences and Technology Beijing, Beijing 100083, China;
jiujiu@sas.ustb.edu.cn
* Correspondence: zhanglanying@pku.edu.cn (L.Z.); yanghuai@pku.edu.cn (H.Y.)
† These authors contributed equally to this work.

Received: 27 October 2020; Accepted: 13 November 2020; Published: 25 November 2020
Abstract: Polymer dispersed liquid crystals (PDLCs) have kindled a spark of interest because of
their unique characteristic of electrically controlled switching. However, some issues including high
operating voltage, low contrast ratio and poor mechanical properties are hindering their practical
applications. To overcome these drawbacks, some measures were taken such as molecular structure
optimization of the monomers and liquid crystals, modification of PDLC and doping of nanoparticles
and dyes. This review aims at detailing the recent advances in the process, preparations and
applications of PDLCs over the past six years.
Keywords: polymer-dispersed liquid crystals; polymerization induced phase separation; doping; applications
1. Introduction
Polymer dispersed liquid crystals (PDLC) were identified as electrically switchable materials four
decades ago and have since then remained a topic of intense scientific curiosity. PDLC composite
films consist of micrometer or nanometer size liquid crystal (LC) droplets embedded in a polymer
matrix. In general, these films exhibit a milky white scattering state due to the random orientation of
LC droplets in the polymer matrix [1–3]. Once an electric field of sufficient strength is applied, the
film becomes transparent and this phenomenon is attributed to the alignment of LC droplets along
the direction of the electric field (Figure 1), if the ordinary refractive index no of LC matches with
the refractive index np of the polymer matrix [4]. Spurred by the employment of PDLC in display
technologies, research on these materials has rapidly grown in recent decades and is now extending
into areas beyond smart windows [5] and displays [6], including diffuse film [7], antipeeping film,
quantum dots (QDs) film [8] and components of organic light emitting diode (OLEDs) [9], field effect
transistors (FETs) [10], energy storage [11] and solar-energy harvesting [12].
Molecules 2020, 25, 5510; doi:10.3390/molecules25235510 www.mdpi.com/journal/molecules

Molecules 2020, 25, 5510 2 of 22
Molecules 2020, 25, x FOR PEER REVIEW 2 of 23
(a) (b)
Figure 1.1. Operating

Operatingprinciple
principleofofa common
a common polymer
polymer dispersed
dispersed liquid
liquid crystal
crystal (PDLC)
(PDLC) device.
device. (a) off-
(a) off-state,
state,
(b) (b) on-state.
on-state.
PDLCs can can bebe prepared

preparedby byemulsion
emulsionororphase phaseseparation
separationmethods
methods [13–15].
[13–15].However,
However, thethe
latter is
latter
widely reported in the literature as it allows great control of the morphology,
is widely reported in the literature as it allows great control of the morphology, and thus the and thus the characteristics,
of the final film.ofThis
characteristics, themethod
final film. canThis
be induced
methodby canthermal
be inducedaction, bysolvent
thermal evaporation and/or
action, solvent monomer
evaporation
polymerization.
and/or monomerThe formed LC droplets
polymerization. The formed exhibitLCgreat variation
droplets exhibitdepending on thedepending
great variation method of on phasethe
separation employed. For thermally induced phase separation
method of phase separation employed. For thermally induced phase separation (TIPS), LC is mixed (TIPS), LC is mixed with a polymer
at high
with temperature,
a polymer at highthen the mixturethen
temperature, is allowed to coolisatallowed
the mixture a specificto rate
cool to at cause phase
a specific separation
rate to cause
and, as the polymer hardens, the LC domains appear. For the solvent-induced
phase separation and, as the polymer hardens, the LC domains appear. For the solvent-induced phase phase separation (SIPS)
process, both the LC and polymer are dissolved in the same
separation (SIPS) process, both the LC and polymer are dissolved in the same solvent. The solvent. The evaporation of solvent at
aevaporation
specific rateofinducessolvent phase separation.
at a specific For thephase
rate induces polymerization-induced phase separation (PIPS)
separation. For the polymerization-induced
method, the LC is mixed with a monomer/prepolymer
phase separation (PIPS) method, the LC is mixed with a monomer/prepolymer solution to form a homogenous
solution tosolution.
form a
As the polymerization
homogenous solution. As continues the polymercontinues
the polymerization and LC separate
the polymer from andeachLCother by liquid-liquid
separate from each other or
liquid–gel
by liquid-liquidphaseor [16,17]. The LC
liquid–gel phase molecules
[16,17]. come
The LC outmolecules
of the solution
come out and offormthe droplets
solution thatand growform
until
dropletspolymerization
that grow until is finished, i.e., whenisthe
polymerization polymeri.e.,
finished, matrix
whenbecomes
the polymersolid enough [18]. The solid
matrix becomes PIPS
method
enough could[18]. The be further dividedcould
PIPS method into thermal-initiated
be further divided polymerization and ultraviolet
into thermal-initiated (UV)-initiated
polymerization and
polymerization. Although the former method offers good processability,
ultraviolet (UV)-initiated polymerization. Although the former method offers good processability, less contamination and strong
bonding energy, it requires
less contamination and stronghigh temperatures
bonding energy, and long durationhigh
it requires [19,20]. The latter, however,
temperatures and longisduration
prompt,
solvent-free and ecofriendly
[19,20]. The latter, however, is for the production
prompt, solvent-freeof PDLC films [21]. for the production of PDLC films
and ecofriendly
[21]. Despite the stability and durability of the PDLC films prepared by UV- polymerization, nuances
in UV-irradiation,
Despite the stability molecular weight and
and durability solubility
of the PDLC films of the constituting
prepared by UV-LCs and polymers
polymerization, could
nuances
lead to distinct morphologies
in UV-irradiation, molecular weight [22]. Thereby, degreeofofthe
and solubility phase separation
constituting LCs andandrate of polymerization
polymers could lead
are influences
to distinct which control
morphologies [22].the morphology
Thereby, degree of of LC
phasedroplets. Inside
separation and the LCofdroplet,
rate the director
polymerization are
configuration
influences which is mainly determined
control by boundary
the morphology ofconditions
LC droplets. (surface anchoring),
Inside the LCLC materialthe
droplet, parameters
director
and droplet shape
configuration and size.determined
is mainly External factors (electric orconditions
by boundary magnetic fields,(surfacetemperature,
anchoring), stressLCand so on)
material
change
parameters the orientational
and droplet structure
shape and which
size.affects
Externalthe factors
light-scattering
(electric byor LC dropletsfields,
magnetic and, consequently,
temperature,
the light
stress and transmission
so on) change of the
the PDLC film [23–30].
orientational structureIn addition, a slight
which affects thedifference in the refractive
light-scattering by LC dropletsindex
(RI)
and, consequently, the light transmission of the PDLC film [23–30]. In addition, a slight difference of
of both the phases (LCs and polymer) has a significant effect on the light scattering properties in
the PDLC
refractivefilms. Moreover,
index (RI) ofthe bothfilmthe thickness
phases also(LCscrucially
and polymer)impactshas the amorphology
significant andeffectelectro-optical
on the light
(E-O) properties
scattering propertiesof theofPDLCthe PDLCfilms [31].
films.Studies
Moreover, on these issues
the film can be useful
thickness in developing
also crucially impacts PDLC the
films for typical applications.
morphology and electro-optical (E-O) properties of the PDLC films [31]. Studies on these issues can
be useful in developing PDLC films for typical applications.
Here, we review the recent developments in preparation, experimental investigation and
application of PDLCs, and focus specifically on UV-polymerization. Instead of going into deep
Molecules 2020, 25, 5510 3 of 22
Here, we review the recent developments in preparation, experimental investigation and

application of PDLCs, and focus specifically on UV-polymerization. Instead of going into deep details,
only specific recent papers between 2014–2020 which are particularly related to UV polymerization,
details, only specific recent papers between 2014–2020 which are particularly related to UV
modification techniques related to the process and material to enhance the E-O properties of PDLCs
polymerization, modification techniques related to the process and material to enhance the E-O
(Figure 2) are cited. However, some papers were exceptionally important and are cited. Furthermore,
properties of PDLCs (Figure 2) are cited. However, some papers were exceptionally important and
previous reviews related to these materials [32–38] can be referred to gain a full understanding of
are cited. Furthermore, previous reviews related to these materials [32–38] can be referred to gain a
the topic.
full understanding of the topic.
Figure2.2. An
Figure Anillustration
illustrationof
ofthe
thepreparation,
preparation,electro-optical
electro-opticalproperties
propertiesoptimization
optimizationand
andapplications
applications
ofPDLC.
of PDLC.
2.
2. Preparation
Preparation of
of Conventional
Conventional PDLC
PDLC Composite
Composite Film
Film
(Meth)acrylate
(Meth)acrylatemonomers
monomersare aregenerally
generallyutilized to prepare
utilized to preparePDLC PDLCfilms by UV-polymerization
films by UV-polymerization [39].
The
[39].modulation
The modulation of theof morphology
the morphology andandE-OE-O
properties
propertiesareare
limited
limited ininthe
theflexible
flexible(meth)acrylate
(meth)acrylate
monomers. Therefore, some unique structures such as hydroxy, epoxy, branched
monomers. Therefore, some unique structures such as hydroxy, epoxy, branched methylene/methyl, methylene/methyl,
cyclic
cyclic methylene,
methylene, phenyl
phenyl and
and bisphenol
bisphenol werewere incorporated
incorporated into
into the
the conventional
conventional acrylates
acrylates [40–44].
[40–44].
Once these structures were incorporated into the polymer matrix, the E-O
Once these structures were incorporated into the polymer matrix, the E-O properties of PDLC properties of PDLC composite
films could be
composite optimized
films could bybe varying
optimized the hydrogen-bond
by varying the interaction,
hydrogen-bond the viscosity of acrylate
interaction, monomers,
the viscosity of
the refractive
acrylate index the
monomers, of polymer
refractivematrix
index ofand polymer
polymer network
matrix morphologies
and polymer network [45]. Among them,
morphologies [45].
the presence
Among them,ofthethepresence
hydroxyl ofgroup promoted
the hydroxyl thepromoted
group formationthe of formation
a thin polymer layer
of a thin at the surface
polymer layer at
of PDLC films even at low LC loadings, attributed to improving the E-O
the surface of PDLC films even at low LC loadings, attributed to improving the E-O properties properties [46]. Recently,
[46].
aRecently,
low-voltage driven PDLC
a low-voltage system
driven PDLC was achieved
system wasthrough
achievedanthrough
elegantly an simple
elegantlyandsimple
uniquelyanddesigned
uniquely
acrylate
designedmonomer (A3DA) featuring
acrylate monomer a benzenea moiety
(A3DA) featuring benzenewith
moietya dodecyl terminalterminal
with a dodecyl chain [47]. In [47].
chain our
recent
In ourstudy,
recentwe focused
study, on the comparison
we focused of methylofand
on the comparison acrylate
methyl and monomers as well asasterminal
acrylate monomers well as
structures [48]. We found that the asymmetrical substitution of the methyl
terminal structures [48]. We found that the asymmetrical substitution of the methyl group on the group on the quaternary
carbon
quaternaryin the maininchain
carbon increased
the main the stericthe
chain increased hindrance which reduced
steric hindrance which reducedthe polymerization
the polymerizationrate.
The
rate.contrast ratio (CR)
The contrast ratiowas
(CR) improved
was improvedmany-fold by changing
many-fold the monomer
by changing structurestructure
the monomer from flexible
from
to rigid. Similarly, when the monomer with siloxane was incorporated
flexible to rigid. Similarly, when the monomer with siloxane was incorporated into the polymer into the polymer matrix,
matrix, the mechanical properties were enhanced without sacrificing the E-O properties [49]. Table 1
lists some of the (meth)acrylate monomers employed for the preparation of PDLC composites.
Molecules 2020, 25, 5510 4 of 22
the mechanical properties were enhanced without sacrificing the E-O properties [49]. Table 1 lists some
of the (meth)acrylate monomers employed for the preparation of PDLC composites.
Table
Molecules 2020, 25, x1. Some
FOR (meth)acrylate
PEER REVIEW monomers used for the fabrication of various PDLC composites.4 of 23
Molecules Table
2020, 1. xSome
25,
Table25,
(meth)acrylate
FOR PEER
1.xSome REVIEW monomers
(meth)acrylate
used for the fabrication of various PDLC composites.
monomers used for the fabrication of various PDLC composites. 44 of
of 23
Molecules Table
2020, FOR PEER REVIEW
Molecules 2020,No.1. xSome
25, FOR (meth)acrylate
PEER REVIEW monomers used for the fabrication
Monomers Chemical Structure Reference 4 of 23
of various PDLC composites. 23
No.Table 1. Some (meth)acrylate
Monomers Chemical Structure
monomers used for the fabrication Reference
of various PDLC composites.
Molecules
No.2020, 25,
Table 1. xSome
FOR PEER REVIEW
Monomers
(meth)acrylate monomers used for the Chemical of
fabrication Structure
various PDLC Reference4 of 23
composites.
Molecules
No. 2020, 25,
Table 1. xSome
FOR PEER REVIEW
Monomers
(meth)acrylate Chemical Structure
monomers used for the fabrication Reference4 of 23
No. Monomers
Table 1. Some (meth)acrylate Chemicalof
monomers used for the fabrication Structure Reference
various PDLC composites.
No.Table 1. Some (meth)acrylate Monomers Chemical Structure
monomers used for the fabrication Reference
1
No. 1 Lauryl acrylate
Lauryl
Monomersacrylate Chemical Structure [48]
[48]
Reference
No. 1Table 1. Some (meth)acrylate
Lauryl
Monomers
monomers used for the fabrication
acrylate of various PDLC composites.
Chemical Structure [48]
Reference
1
No. Lauryl acrylate
Monomers Chemical Structure [48]
Reference
No. 1 Lauryl acrylate
Monomers Chemical Structure [48]
Reference
1 Lauryl acrylate [48]
21 Lauryl methacrylate
Lauryl acrylate [50]
[48]
2 2 Lauryl methacrylate
Lauryl methacrylate [50]
[50]
2 Lauryl methacrylate [50]
322 Lauryl methacrylate
Hydroxypropyl
Lauryl methacrylate
methacrylate
[50]
[49,50]
[50]
3 Hydroxypropyl methacrylate [49,50]
3 3 Hydroxypropyl
Hydroxypropyl methacrylate
methacrylate [49,50]
[49,50]
43 Hydroxypropyl
3, methacrylate
5, 5-trimethelhexyl acrylate [49,50]
[51]
43 Hydroxypropyl
3, methacrylate
[51]
43 Hydroxypropyl
3, methacrylate
[51]
4 4 3, 3,
5, 5,
5-trimethelhexyl
5-trimethelhexyl acrylate
acrylate [51][51]
4 3, 5, 5-trimethelhexyl acrylate [51]
4 3, 5, 5-trimethelhexyl acrylate [51]
54 3, 5,Glycidyl
methacrylate [51]
[49]
54 3, 5,Glycidyl
methacrylate [51]
[49]
54 3, 5, 5-trimethelhexyl
Glycidyl methacrylateacrylate [51]
[49]
5 Glycidyl methacrylate [49]
5 5 Glycidyl methacrylate
Glycidyl methacrylate [49]
[49]
65 Glycidyl methacrylate
Tetrahydrofurfuryl acrylate [49]
[48]
56 Glycidyl methacrylate
Tetrahydrofurfuryl acrylate [49]
[48]
6 Tetrahydrofurfuryl acrylate [48]
6 6 Tetrahydrofurfuryl
Tetrahydrofurfuryl acrylate
acrylate [48]
[48]
7 6 Tetrahydrofurfuryl acrylate
Tetrahydrofurfuryl methacrylate [48]
[48,49]
67 Tetrahydrofurfuryl
Tetrahydrofurfuryl acrylate
methacrylate [48]
[48,49]
7 Tetrahydrofurfuryl methacrylate [48,49]
7 7 Tetrahydrofurfuryl
Tetrahydrofurfuryl methacrylate
[48,49]
87 Benzyl methacrylate
Tetrahydrofurfuryl methacrylate [48,49]
[48,49]
8 Benzyl methacrylate [48,49]
8 8 Benzyl
Benzylmethacrylate
[48,49]
98 Benzyl methacrylate
Cyclohexyl methacrylate [48,49]
9 Cyclohexyl methacrylate [48,49]
PDLC 9 films composed
Cyclohexyl of methacrylate
thiol-ene monomers are usually prepared by UV-polymerization.
[48,49]
PDLC9 films
9 composed
Cyclohexyl ofmethacrylate
Cyclohexyl thiol-ene monomers are usually prepared by UV-polymerization.
[48,49]
Norland PDLC optical
filmsadhesives
composedare ofgood
thiol-eneexamples monomersof these arekinds of monomers.
usually prepared by These monomers have
UV-polymerization.
Norland PDLC optical
filmsadhesives
composed areofgood examples
thiol-ene monomers of these are kinds of monomers.
usually prepared by These monomers have
UV-polymerization.
high
Norland conversion
PDLC filmsefficiency,
optical composedfast
adhesives are speed,
ofgood
thiol-ene water
examples resistance,
monomers of these are excellent
kinds of thermal
usually monomers.
prepared insulation,
These
by better inertness
monomers
UV-polymerization. have
high
Norland conversion
PDLC filmsefficiency,
optical composedfast
adhesives of speed,
are good
thiol-ene water
examples resistance,
monomers of these areexcellent
kinds
usuallyof thermal
monomers.
prepared insulation,
byThese better inertness
monomers
to
highoxidation
Norland conversion and
optical less light
efficiency,
adhesives initiator
fast
are speed,
good dosage
water
examples than ofthe
resistance, acrylates
these
PDLC films composed of thiol-ene monomers are usually prepared by UV-polymerization. kinds system
excellentof thermal[52–54].
monomers. The
insulation,
These thiol-ene
better
monomers reaction
inertness
have
to
highoxidation
Norland conversion
PDLC opticalandadhesives
films less light initiator
efficiency,
composed fast
are speed,
ofgood dosage
water
examples
thiol-ene than
monomers ofthe
these arekinds system
excellent thermal
of monomers.
usually [52–54].
prepared The
insulation,
These
by thiol-ene reaction
better inertness
monomers
usually
to
highoxidation
Norland PDLC occurs
conversion
opticalandin
films lesstwo light
efficiency,
adhesives
composed ways:fast
are ofthe
initiatorspeed,
good radical-mediated
dosage
thiol-ene water
examples than ofthe
resistance,
monomers these anti-Markovnikov
acrylates
are system
excellent
kinds of thermal
usually monomers.
prepared addition
[52–54]. The
insulation,
These
by and
thiol-enetheinertness
better
monomers
UV-polymerization. base
reaction
have or
usually
to oxidation
high
Norland occurs
conversion
optical
PDLC and in two
less
efficiency,
adhesives
films ways:
light
composed fast the
initiator
are speed,
good radical-mediated
dosage
waterthan
examples
of addition.
thiol-ene ofthe
resistance,
monomers these anti-Markovnikov
acrylates
excellent
kinds
are system
of thermal
monomers. addition
[52–54].
insulation, The
These and
thiol-ene
bettertheinertness
monomers base
reaction
haveor
nucleophile-initiated
usually
to
highoxidation
Norland occurs
conversion
opticalandin lesstwo thiol-Michael
light
efficiency,
adhesives ways: the
initiator
fast good
are speed, radical-mediated
dosage
waterthan
examples In the
ofthe
resistance, former,
acrylates
these kindstheusually
initiator
anti-Markovnikov
system
excellentof thermal
prepared
absorbs
addition
[52–54].
monomers. The
insulation,
These
by and
energy UV-polymerization.
from
thiol-ene
better
monomers light
theinertness
base
reaction
have or
usually
to oxidation
high occurs
conversion
Norland and in
optical lesstwo thiol-Michael
light
efficiency, ways:
adhesives initiator
fastare speed,addition.
thegood water In the
radical-mediated
dosage than
examples the offormer,
these thesystem
excellent
kinds initiator
anti-Markovnikovthermal
of absorbs
[52–54].
monomers. addition The
insulation, energyand from
thiol-ene
These better
monomers light or
theinertness
base
reaction or
have
heat
usually and
to oxidation
high produces
occurs
conversion andin free
two
less
efficiency, radicals
thiol-Michael
ways:
light fast the
initiator to initiate
speed, addition. the
radical-mediated
dosage
water Inreaction
than the
theformer,
resistance, [53]. However,
the initiator
anti-Markovnikov
acrylates system
excellent thermal the latter
absorbs
addition
[52–54]. The
insulation, employs
energyand
thiol-ene a base
from
the
better light
base
reaction
inertness oror a
heat
to and
oxidation
high produces
usually occurs and
conversion in free
two
less radicals
thiol-Michael
ways:
light
efficiency, the
initiator
fastto initiate
addition. the
radical-mediated
dosage
speed, than
water reaction
In the
the [53].
former, However,
the initiator
anti-Markovnikov
acrylates
resistance, system
excellent the latter
absorbs
addition
[52–54].
thermal Theemploys
energy
insulation,and from
the
thiol-ene a
better base light
base
reactionor or
or
inertness a
nucleophile
heat
usually
to andoccurs
oxidation which
produces
andinless could
free
two weaken
radicals
thiol-Michael
lightways:
initiator tothe
the bondthe
initiate
addition. energy
radical-mediated
dosage than theof
Inreaction
the the
former, alkene
[53]. the double
However,
initiator
anti-Markovnikov
acrylates system bond
the latter
absorbs
addition
[52–54]. to
The start
employs
energyand the reaction
a base
from
thiol-enethe light
base
reaction ina
oror
nucleophile
heatto and
usually occurs
oxidation which
produces could
in two
and free weaken
radicals
thiol-Michael
less ways:
light the the
initiator bond
to addition.
initiate
dosage energy
the reaction
Inthan
radical-mediated of
the former,
thethe alkene
[53].the double
However,
systemthe
initiator
anti-Markovnikov
acrylates bond
absorbs
addition
[52–54]. to start
latterenergy
employs
The andthefrom
thereaction
thiol-enea base
light
base in
oror
ora
reaction
mild
heat conditions.
nucleophile
and
usually occurs which
produces inIn China,
could
free
two radicalsWang
weaken
thiol-Michael
ways: tothe
the et al.
bond
initiate
addition.[55–58]
energy
the
radical-mediated from
Inreaction
the of Sichuan
the alkene
[53].
former, university,
double
However,
the initiator
anti-Markovnikov thebond in to
latter
absorbs
addition their
startvarious
employs
energyand thefrom
the studies,
areaction
base
light
base in
oror a
mild
heat conditions.
nucleophile
and
usually which
produces
occurs Infree
in China,
could radicals Wang
weaken
thiol-Michael
two ways: to theet al.
bond
initiate
addition.
the [55–58]
theenergy
In from
reaction
radical-mediatedthe of Sichuan
the
[53].
former, alkene university,
However,
the double
initiator
anti-Markovnikov the bond inaddition
latter
absorbs their
to start
employs
energy various
the
from
and studies,
areaction
base
thelight oror
base in
a or
employed
mild
nucleophile
heat and the
conditions.
produces
nucleophile-initiated thiol-Michael
which Incould
China,
free weaken
radicals
thiol-Michaeladdition
Wang totheet to produce
al.
bond
initiate
addition.[55–58]
energy
the Inreaction
the dye-doped
from
of Sichuan
the
former, alkene
[53]. PDLC double
However,
the initiator films
university,thebondwith
in to
latter
absorbs low
their
employs
energy driving
startvarious
thefrom voltage
studies,
areaction
base
light ina
oror
employed
mildand
nucleophile
heat the
conditions. thiol-Michael
which
produces In China,
could
free weaken
radicals addition
Wang tothe to produce
et bond
al.
initiate [55–58]
energy
the dye-doped
from
reactionof the Sichuan
alkene
[53]. PDLCdouble
However, films
university, bond
the with
latter low
intotheir
employs driving
startvarious
the reaction
a base voltage
studies,
orina
(V
milddr).and
employed
nucleophile
heat In our the
conditions. group
which
produces Zhong
thiol-Michael
Incould
China,
free radicalset
Wang
weaken al.tothe
addition[16] to
et bondemployed
al.
initiate produce
[55–58]
energy
the vinyl
dye-doped
from
reactionof the ether
Sichuan
alkene
[53]. and
PDLC thiol
films
university,
double
However, thetolatter
bond fabricate
with
in to low
their
start
employs PDLCs
driving
various
the areaction via or
voltage
studies,
base the
ina
(V
milddr). conditions.
employed
nucleophileIn our the group
which Zhong
thiol-Michael
Incould
China, etaddition
Wang
weaken al. the
[16]
et al. employed
to
bond produce
[55–58]
energy vinyl
dye-doped
fromof the ether
Sichuan
alkene and
PDLC thiol
films
university,
double to with
bond fabricate
in low
their
to start PDLCs
driving
various
the reaction via
voltage
studies, thein
Markovnikov
(V ).
employed In
mild conditions.
nucleophile
dr our
the reaction
group Zhong
thiol-Michael
which Incould and
China, investigated
et
weaken al.
addition
Wangthe [16] to
et bond the
employed
produce
al. [55–58] morphology
energy vinyl
dye-doped
from
of the and
ether
Sichuan
alkeneelectro-optical
and
PDLC thiol
films
university,
double bond to with properties
fabricate
in to low
their PDLCsof
driving
startvarious the
theofreaction viafilms.
voltage
studies,the
in
Markovnikov
(Vdr). conditions.
employed
mild In our reaction
the group Zhong
thiol-Michael
In China, and investigated
et al. [16]
addition
Wang et al. the
toemployed
producemorphology
[55–58] vinylSichuan
dye-doped
from and PDLC
ether electro-optical
and thiol
filmstowith
university, properties
fabricate
in their PDLCs
low various
driving the films.
via
voltage
studies, the
Zhang
Markovnikov
(V
employed
mild Inet our
al.the
dr). conditions. [59]
groupdemonstrated
reaction Zhong
thiol-Michael
In China, et that[16]
and investigated
al.
addition
Wang etthe thiol–acrylate
the
employed
to
al. produce
[55–58]morphologyvinyl systems
dye-doped
from ether
Sichuan could
and PDLC
and be
electro-optical
thiol
films
university, used
to with to produce
properties
fabricate
in PDLCs
low various
their PDLC
of
driving the via films
films.
voltage
studies,the
Zhang
Markovnikov
(V dr). In
employed etour
al.the
[59]
group demonstrated
reaction Zhong
thiol-Michael and et that
investigated
al.
addition[16]theto thiol–acrylate
the
employed morphology
produce vinyl systems
dye-doped andand
ether could
PDLC be
electro-optical
thiol
filmsused
to with to produce
properties
fabricate PDLCs
low driving PDLC
of the via films
films.
voltagethe
with
(Vdr). higher
Zhang
Markovnikov
employed Inet our
al.theCR,
[59] but
reaction
group theand
demonstrated
Zhong
thiol-Michael driving voltage
that
investigated
etaddition
al. theto
[16] was
the
employed
produce also vinyl
thiol–acrylate
morphologyhigh.
dye-doped Sun
andetPDLC
systems
ether al. [60]
could be studied
electro-optical
and thiol
filmsused
towith to the
properties
fabricate
low effects
produce PDLCsof
driving ofthe
PDLC various
via films
films.
voltage the
withdr). higher
Zhang
Markovnikov
(V al. CR,
Inetour [59] but
reaction
group the
demonstrated
and
Zhong driving voltage
that
investigated
et al. [16] wasmorphology
theemployed
the also vinyl
thiol–acrylate high. Sun
andetelectro-optical
systems
ether al. [60]
could
and bestudied
thiol used tothe
to fabricate effects
produce
properties PDLCs of
ofPDLCthevarious
via films
films.
the
with
Zhang higher
Markovnikov
(V dr). In et our CR,
al. [59] but
reaction
group the
demonstrated
Zhong driving
and investigated
et al. voltage
that[16] was
theemployed also
thiol–acrylate
the morphology high.
vinyl Sun
systems et
and and
ether al. [60]
couldthiol studied
be used
electro-optical to the effects
produce
properties
to fabricate PDLCs PDLC
of of various
thevia films
films.
the
Molecules 2020, 25, 5510 5 of 22
nucleophile-initiated thiol-Michael addition. In the former, the initiator absorbs energy from light or
heat and produces free radicals to initiate the reaction [53]. However, the latter employs a base or
a nucleophile which could weaken the bond energy of the alkene double bond to start the reaction
in mild conditions. In China, Wang et al. [55–58] from Sichuan university, in their various studies,
employed the thiol-Michael addition to produce dye-doped PDLC films with low driving voltage (Vdr ).
In our group Zhong et al. [16] employed vinyl ether and thiol to fabricate PDLCs via the Markovnikov
reaction and investigated the morphology and electro-optical properties of the films. Zhang et al. [59]
demonstrated that the thiol–acrylate systems could be used to produce PDLC films with higher CR,
but the driving voltage was also high. Sun et al. [60] studied the effects of various acrylate monomers
with thiols and optimized the microstructure which improved the CR and driving voltage of the
PDLC films.
Unlike the previous works focusing on the structures of the monomers, Zhang et al. [61–63] from
University of Science and Technology, Beijing, China, systematically investigated the effects of LC
molecule structures (fluorinated LC molecules, alkene-terminated LC molecules, and cyano-terminated
tolane LC molecules) on the morphology and E-O properties of PDLC composite films. The LC
component was obtained by doping fluorinated LC molecules into commercial LC (E8) and fixed 50.0
wt% in PDLC composite films. The doping contents and the terminal chain lengths of the fluorinated
LC molecules influenced the physical properties (such as dielectric anisotropy, refractive index and
viscosity) of LC and polymer network morphology and the E-O properties of PDLC composite films.
The results showed that the optimal 8.0 wt% doping fluorine LC molecules enabled them to realize
the significantly low driving voltage of the composite films. According to the above study methods,
the optimal E-O properties of PDLC composite films with low driving voltage, high CR and fast
response time were obtained by employing alkene-terminated LC molecules or cyano-terminated
tolane LC molecules.
3. Preparation of Modified PDLC Composite Film

In the past few years, the modified PIPS technique suggested by Chidichimo et al. [64] of Calabria
University, Italy, was further developed as a dual-step polymerization by our research group [65–70].
PDLC composite films could be prepared by UV-UV, UV-thermal, thermal-UV or thermal-thermal
polymerization in two steps. Liquid crystalline acrylate, vinyl-ether, or epoxy monomers were
frequently used. Among them, radical-initiated liquid crystalline acrylate and cationic-initiated
liquid crystalline vinyl-ether were usually used for UV polymerization, while liquid crystalline epoxy
initiated by UV or thermal could be used for UV or thermal polymerization. Here, a UV-UV dual
step polymerization method was taken as an example to introduce the specific method [66]. Figure 3
shows a schematic illustration of the preparation of polymer dispersed and polymer stabilized liquid
crystal (PD&PSLC) composite film. The key factor was the lower polymerization rate of the liquid
crystalline monomer (LCM) with a rigid structure than that of non-LCM. Thus, the non-LCM radical
polymerization was dominant. Further, the microphase separation between LC and the polymer matrix
occurred and a porous polymer network structure was formed in the first step, which was similar to
PDLC. Subsequently, under sufficient applied electric field and appropriate UV intensity conditions,
the oriented LCM was further polymerized to construct the homeotropically aligned polymer network
(HAPN) in larger porous structures as shown in Figure 4c, similar to PSLC. The resulting composite
film was referred to as PD&PSLC. In the said work, the LC with SmA-N* phase transition was used
and the resulting composite film could reversibly transverse a transparent and strong light-scattering
state under temperature controlled conditions. More importantly, the film combined the advantages of
large-area manufacturing and flexibility. Meanwhile, the dual-step polymerization was also carried out
for an electrically controllable PD&PSLC composite film. The results showed that the demonstrated
PD&PSLC composite film possessed better E-O properties and mechanical properties, besides good
film formation.
Molecules 2020,2020,
Molecules 25, x25,FOR
5510PEER REVIEW 6 of 226 of 23
Figure 3. Schematic illustration of the preparation of polymer dispersed and polymer stabilized
Figure 3. Schematic
liquid illustration
crystal (PD&PSLC) of the preparation
composite of polymerisotropic
film. (a) Homogeneous dispersed and polymer
mixture sandwichedstabilized
betweenliquid
crystal
two(PD&PSLC) composite
pieces of plastic sheets. (b)film. (a) Homogeneous
Microphase isotropicthe
separation between mixture sandwiched
liquid crystalline between
mixture and two
pieces of plastic
polymer sheets.
matrix. (b) Microphase
(c) Randomly orientedseparation between
liquid crystalline the liquid
mixture withincrystalline mixture
a liquid crystal (LC)and polymer
droplet.
(d) Perpendicularly
matrix. (c) Randomlyaligned liquid
oriented crystalline
liquid mixture.
crystalline (e) Homeotropically
mixture within a liquidaligned polymer
crystal (LC)network
droplet. (d)
(HAPN) formed
Perpendicularly within liquid
aligned an LC droplet. (f) The
crystalline N* phase
mixture. (e)gradually turns into the
Homeotropically SmA phase
aligned upon network
polymer the
consumption of photopolymerizable monomers. (g) Perpendicularly aligned
(HAPN) formed within an LC droplet. (f) The N* phase gradually turns into the SmA phase uponSmA phase within an LC the
droplet. (h) Focal-conic texture of the heat-induced N* phase within an LC droplet. (i) Photograph of
consumption of photopolymerizable monomers. (g) Perpendicularly aligned SmA phase within an
the transparent state of the film at a temperature below the phase-transition temperature of the LC.
LC droplet. (h) Focal-conic texture of the heat-induced N* phase within an LC droplet. (i) Photograph
(j) Photograph of the heat-induced light-scattering state of the film. Reproduced with permission from
of the
ref.transparent state2017,
[66]. Copyright of the
ACS film at a temperature below the phase-transition temperature of the LC.
Publication.
(j) Photograph of the heat-induced light-scattering state of the film. Reproduced with permission from
ref. [66]. Copyright 2017, ACS Publication.
Molecules 2020, 25, 5510 7 of 22
Figure 4. Scanning electron microscope (SEM) photographs of the polymer networks of the films
Figure 4. Scanning electron microscope (SEM) photographs of the polymer networks of the films
observed from a side view of the cells. (a) A porous structure of polymer networks of PDLC composite
observed from a side view of the cells. (a) A porous structure of polymer networks of PDLC composite
film. (b) The HAPN of PSLC composite film. (c) A coexistent structure of both the porous polymer
film. (b) The HAPN of PSLC composite film. (c) A coexistent structure of both the porous polymer
networks and the HAPN of PD&PSLC composite film. Reproduced with permission from ref. [66].
networks and the HAPN of PD&PSLC composite film. Reproduced with permission from ref. [66].
Copyright 2017, ACS Publications.
Copyright 2017, ACS Publications.
4. Preparation of Nanoparticles Doped PDLC Composite Film
4. Preparation of Nanoparticles Doped PDLC Composite Film
In conventional PDLCs, the LC, monomer and initiator are mixed. However, there are certain
In conventional
limitations PDLCs,
to an all-organic the LC,Doping
system. monomer and initiator(NPs)
of nanoparticles are mixed. However,
was attributed to there are certain
the enhancement
limitations to an all-organic system. Doping of nanoparticles (NPs)
of optical, thermal and mechanical stability of the polymer matrix and interaction with the LC. was attributed to NPs
the
enhancement
mainly influence of optical, thermal
the dielectric and mechanical
constant, stability
refractive index of the polymer
or anchoring forcesmatrix and interaction
at the polymer/LC with
interface.
the LC. NPs mainly influence the dielectric constant, refractive index or
Various types of NPs have been probed to prepare PDLC films with superior qualities. A few recent anchoring forces at the
polymer/LC interface. Various types of NPs have been probed
examples of the properties exhibited by NPs-doped PDLC are discussed below. to prepare PDLC films with superior
qualities.
PDLC A composite
few recentmaterials
examplesdoped of thewith
properties
ITO NPs exhibited by NPs-doped
were studied by variousPDLC groups aretodiscussed
optimize
below.
the films for applications in the field of energy saving due to their thermal insulation properties. In
China,PDLCWu composite materials
et al. [71] of Nanjing doped with ITO
University NPs1.5
doped were wt%studied by various
ITO powders ofgroups
submicron to optimize
size in the
the
films for applications in the field of energy saving due to their thermal insulation
mixture (E7 + NOA65) and found that the operating voltages decreased due to the effects of ITO on the properties. In China,
Wu et al. [71]ofofthe
morphology Nanjing
PDLC University dopedforce
as the anchoring 1.5 wt% ITO
at the powders of
polymer/LC submicron
boundary wassize in the Recently
lowered. mixture
(E7
Zhang+ NOA65)
et al. [72]and foundUniversity,
of Xijing that the operating
China, also voltages
used ITOdecreased
NPs with due to the effectsmonomers
acrylate-based of ITO onafterthe
morphology of the PDLC as the anchoring force at the polymer/LC boundary
surface treatment of NP with 3-methacryloxypropyltrimethoxysilan. However, they found that the was lowered. Recently
Zhang
drivingetvoltage
al. [72]was
of Xijing University,
increased and CR China, also used
was decreased withITOtheNPs with acrylate-based
increment of doping content monomers
at 0–20after
wt%
surface
of NPs treatment
loading, whileof NPthe with 3-methacryloxypropyltrimethoxysilan.
near infra-red (NIR) absorption property However, of films was theyenhanced
found that in the
the
driving voltage was increased
wavelength range of 1300 to 2500 nm. and CR was decreased with the increment of doping content at 0-20
wt% of NPsNPs
Silica loading,
hold while the near
significant infra-red
promise (NIR) absorption
to improve property ofoffilms
the E-O properties was enhanced
the PDLC [73]. In in the
India,
wavelength range
Jayoti et al. [74] of of
Dr.1300
B. R.toAmbedkar
2500 nm. National Institute of Technology, Jalandhar, showed the effects
of S-NPs on the morphology andpromise
Silica NPs hold significant to improve
E-O properties the E-O
of PDLC properties
by doping of the
S-NPs intoPDLC
the PDLC[73]. based
In India,
on
Jayoti et al. [74] of Dr. B. R. Ambedkar National Institute of Technology,
NOA65 and BL036 LC. They reported a significant decrease in the driving voltage by doping 1.5Jalandhar, showed the effects
wt%
of S-NPs on the morphology and E-O properties of PDLC by doping S-NPs into the PDLC based on
NOA65 and BL036 LC. They reported a significant decrease in the driving voltage by doping 1.5 wt%
Molecules 2020, 25, 5510 8 of 22
S-NP and also transmittance of the films was enhanced. The NPs located at the LC-polymer interface
modified the anchoring energy and thus effected the reorientation of LCs, which was attributed to
the voltage drop. The dual size S-NPs was accredited to steric hindrances and resulted in slow phase
separation during the photo-polymerization process. In Algeria, Beroguiaa et al. [75] of Université
Aboubakr Belkaïd, reported that high concentration of S-NPs caused their aggregation at the LC
polymer interface, which increased the anchoring energy and thus the reorientation voltage.
Other inorganic NPs such as ZnO, MgO, CuO, BTO, BaTiO3 , Fe3 O4 , TiO2 [76–82] were doped into
PDLCs and a decrease in driving voltage was observed. It was found that these particles tended to
impact the dielectric constant of the medium or created local field effects which consequently lowered
the driving voltage. The doping of ferroelectric NPs created spontaneous polarization which further
improved the E-O properties [82,83]. In India, Mishra et.al [76] of Mumbai University, reported the
fabrication of PDLC films by the SIPS method and embedded CuO, ZnO and Zn, NPs. A change in the
structural and optical properties in the films was observed due to the gradient in the phase transition
temperature confirmed by various characterization techniques such as Fabry Perot spectroscopic
studies, optical polarized microscopy, differential scanning calorimetry, and Abbe refractometry using
DSR Lamda. A change in the refractive index was noted because of the alteration of the orientational
ordering properties of LCs and polymer networks due to the temperature increase.
In recent years, studies showed that metallic NPs-doped PDLC films exhibited better E-O, dielectric
and optical properties. Particularly, Ag and Au-doped films possessed low driving voltages and
high CR. This was attributed to surface plasmon excitations at metal-LC interfaces which enhanced
the local electric fields [84,85]. A random lasing from dye-doped PDLCs containing Ag NPs was
observed due to the cumulative effect of light scattering from nano-sized LC droplets and the local
field enhancement around the silver NPs. In Taiwan, Chan et al. [86] of the National Central University,
prepared core-shell particles by coating a thin layer of Ag on polystyrene microspheres and reported
the effects of doping such particles on the operating voltage of PDLCs. The composite films contained
LC (E7) and an acrylate-based polymer. They found that the induced electric field between the particles
was enhanced upon the application of the external electric field and resulted in reduction of operating
voltage from 77 V to 40 V.
Although the NPs have the potential to modulate the morphology of the films due to their intrinsic
properties, it is difficult to predict how the NPs-doped PDLCs will perform relative to undoped PDLCs.
In addition, the interaction of nanoparticles with the various recipes of the PLDCs is not easy to
envisage and the performance comparison of NPs in a graphical or tabulated form to obtain the general
sketch is of no use because the PDLC composition varies.
5. Preparation of Dye-Doped PDLC Composite Film

In dye-doped PDLCs (D-PDLCs), dye molecules were found to increase light absorption and
decrease the power necessary for the optic effect [87]. D-PDLCs have been studied extensively by
several groups, and it has been found that a strong microscopic mutual interaction among the dye and
LC molecules influenced the LC refractive index, dielectric constant, orientational order and phase
transition temperature [88–92]. E-O properties of the films were significantly improved by doping
dyes due to their contribution to modifying the morphology of the PDLCs [93–96].
In India, Deshmukh et al. [94] of the Institute of Chemical Technology, Mumbai, reported the
growth in the size of LC droplets at a higher concentration of orange dyes. They noticed that during
photopolymerization, dye molecules absorbed some of the UV light available for polymerization and
slowed down the phase separation process. Sharma et al. [97,98] of Chitkara University, Jhansla, Rajpura,
India, also reported the incorporation of orange azo dichroic dye. Their finding revealed that higher
dye concentration varied the transition temperature which transpired trans-cis photoisomerization
of dye molecules as well as light absorption by the dye molecules to a slight extent. The azo dye
molecule exhibited a rod-like shape in the trans form, but was bent and banana-like in the cis form,
which weakened the intermolecular ordering interactions and order parameters of the LC. The
Molecules 2020, 25, 5510 9 of 22
which resulted in
polymerization increased
rate LC droplet
was reduced size
since the as shown
vicinities in occupied
were Figure 5. by
Thedye
studies showed
molecules, that resulted
which the LC,
polymer andLC
in increased dyedroplet
were chosen
size as such
shownthat
in the solubility
Figure 5. The of dye inshowed
studies the polymer was
that the low
LC, but high
polymer andindye
the
LC. chosen such that the solubility of dye in the polymer was low but high in the LC.
were
Figure 5. Graphical
Graphical representations
representations of of LC
LC droplets
droplets size
size of images observed by POM with with 50×
50×
magnification takenduring
magnification taken duringthe
theexperiment
experiment (a)(a) bipolar
bipolar andand radial
radial configuration
configuration ofdroplets
of LC LC droplets and
and (b–e)
stable stable
(b–e) bipolarbipolar
configuration with respect
configuration with torespect
their diverse
to their size of LC droplets
diverse size of with dye concentration.
LC droplets with dye
Reproduced with
concentration. permissionwith
Reproduced frompermission
ref. [97]. Copyright
from ref.2017,
[97]. ELSEVIER
Copyright Publications. SEMPublications.
2017, ELSEVIER images of (f)
pure PDLC,
SEM images(g)ofPDLC + 1%
(f) pure MR, (h)
PDLC, PDLC++3%
(g) PDLC 1%MRMR, and PDLC++3%
(h)(i)PDLC 5% MR
MR composites.
and (i) PDLCReproduced
+ 5% MR
with permission
composites. from ref.with
Reproduced [87]. permission
Copyright 2019, ELSEVIER
from ref. Publications.
[87]. Copyright 2019, ELSEVIER Publications.
6. Preparation
6. Preparation ofof Carbon
Carbon Nanofillers-doped
Nanofillers-doped PDLC PDLC Composite
Composite Film Film
Carbon nanofillers
Carbon nanofillers such
such as as nanographite,
nanographite, fullerenes
fullerenes andand carbon
carbon nanotubes
nanotubes (CNTs)
(CNTs) havehave been
been
paid more attention due to the advantages of their high electric, thermal and
paid more attention due to the advantages of their high electric, thermal and mechanical properties. mechanical properties.
Specifically, the
Specifically, the alignment
alignment of of CNTs
CNTs is is crucial
crucial for
for anisotropic
anisotropic mechanical
mechanical and and electric
electric properties: their
properties: their
properties are extraordinarily large along the tube axis and small along a
properties are extraordinarily large along the tube axis and small along a perpendicular direction.perpendicular direction.
Single wall
Single wall nanotubes
nanotubes (SWNTs)
(SWNTs) and and multiwall
multiwall nanotubes
nanotubes (MWNTs)
(MWNTs) are are two
two representative
representative types of
types of
CNTs successfully
CNTs successfully applied
applied as as dopants
dopants to to PDLCs
PDLCs to to improve
improve their
their E-O
E-O performance.
performance.
Jain et al. [99] of the Institute of Chemical Technology, Mumbai, India,
Jain et al. [99] of the Institute of Chemical Technology, Mumbai, India, prepared
prepared two two types of
types of
MWCNT-doped PDLCs (CPDLC), C00N and C36N using mixtures
MWCNT-doped PDLCs (CPDLC), C00N and C36N using mixtures of two different LCs (LC BL036of two different LCs (LC BL036 and
LC HPC850100-100),
and LC HPC850100-100), and NOA65. The LC The
and NOA65. dropletLCsize was not
droplet sizeinfluenced
was not by the doping
influenced byconcentration
the doping
because no UV light was absorbed by MWCNT. At the optimal doping concentration
concentration because no UV light was absorbed by MWCNT. At the optimal doping concentration (0.005%) CR and
thresholdCR
(0.005%) voltage of C36N, voltage
and threshold CPDLCof composite
C36N, CPDLC film was 990 and film
composite 1 V, respectively,
was 990 and and 1 V, that of C00N
respectively,
CPDLC composite film was 137 and 0.1 V, respectively. However, the composite
and that of C00N CPDLC composite film was 137 and 0.1 V, respectively. However, the composite film shrank because of
the formation of conductive channels between two electrodes of the composite
film shrank because of the formation of conductive channels between two electrodes of the composite film with the increment
of doping
film concentration.
with the increment ofFor the relaxation
doping behavior,
concentration. Forthe
thetwo composite
relaxation films both
behavior, showed
the two Debye-type
composite films
both showed Debye-type behavior having a zero value of the distribution parameter. Wu etofal.
behavior having a zero value of the distribution parameter. Wu et al. [100] from the University Science
[100]
and Technology, Beijing, China, focused on the improvement of E-O properties
from the University of Science and Technology, Beijing, China ,focused on the improvement of E-O of PDLC composed of
acrylate monomers,
properties of PDLCSLC1717,
composed and MWCNT
of acrylate modified
monomers,by a cyanobiphenyl
SLC1717, andfunctional
MWCNT group. The results
modified by a
indicated a reduction of driving voltage at an optimal MWCNT doping
cyanobiphenyl functional group. The results indicated a reduction of driving voltage at an optimal content of 0.01–0.03 mg,
which
MWCNT wasdoping
attributed to theofenhancement
content 0.01-0.03 mg, ofwhich
the electric
was field by reducing
attributed to the the resistivity of
enhancement ofthe
themedium
electric
field by reducing the resistivity of the medium and the increase of the capacitance of the cells induced
by the MWCNT. Moreover, the dispersion of MWCNT was further improved through modification,
Molecules 2020, 25, 5510 10 of 22
and the increase of the capacitance of the cells induced by the MWCNT. Moreover, the dispersion of
MWCNT was further improved through modification, and the corresponding anchoring effect on the
LC molecules was weakened, which improved the transmittance.
7. Applications
The efforts dedicated to fabrication methods and various outstanding properties make PDLCs
suitable for promising applications in energy saving smart windows, photovoltaics, optical elements,
light shutters, switching gratings, sensors, microlenses, lasers, smart food packaging, electrically
switchable high-fold-helix spiral phase plates and biocompatible materials, as well as biomedical
devices. In this section, we presented the information on the aforementioned applications in detail.
7.1. Traditional Applications

Since the beginning, the electrically switchable peculiarity of PDLCs from a light scattering state
to a transparent state has led to their excellent performance and extended application prospects in
energy-efficient smart windows. Although the fabrication of PDLC-based windows has not changed in
recent years, new formulations suitable for this purpose have been investigated thoroughly. Particularly,
the fundamental bottleneck was the optical modulation confined within a limited waveband, either
visible (400–800 nm) or near-infrared (NIR, 800–2500 nm) region. The shorter wavelength invisible
NIR (800 to 1500 nm) carries about 50% of entire solar energy and, therefore, the shielding performance
of a smart window in this range is crucial. To develop a highly efficient energy-saving smart window
Liang et al. [101] recently demonstrated the broadband optical modulation, the regulation of visible
light transmittance [102] and the shielding performance of NIR light from 800 nm to 2500 nm in PDLC
films. They combined a poly(vinylpyrrolidone) (PVP) tuning layer between tungsten bronze (Csx WO3 )
nanorods (NRs) and a polymeric syrup containing liquid crystals with a smectic A (SmA) to chiral
nematic (N*) phase transition, followed by forming an elaborately designed polymer structure within
the film [103]. In essence, the field of the PDLC for smart windows is still evolving [104–106] and there
is still huge room for improvement.
Transparent displays based on PDLCs have high visibility and require a black color as well
as complete blocking of the background. In Korea, Yoon et al. [107,108] of the National University,
Busan, prepared devices which consist of a dye-doped cholesteric liquid crystal (ChLC) layer and a
polymer dispersed liquid crystal (PDLC) film (E7 and NOA 65), for simultaneous control of haze and
transmittance. In the opaque state, this can not only provide a black color by using the dye-doped
ChLCs but also hides the objects behind the display panel by using the PDLC film. The proposed light
shutter shows a high haze value of 90.7% with a low specular transmittance of 1.20%.
7.2. HPDLC
Holographic PDLCs (HPDLCs) are another class of polymer-LC composite wherein prepolymer/
monomer/oligomer concentrations are quite high compared to PDLC. HPDLC structures (periodic dark
and bright fringes) are created in an LC cell filled with a mixture of LC, monomer and photoinitiator (PhI)
exposed under the interference pattern generated by two, or multiple, coherent laser beams with proper
wavelength and power. The interference pattern formed gives rise to nonuniform photopolymerization
and phase separation. High polymerization rate in the bright region (diffusion of the monomer from
dark to bright region) and low polymerization rate in dark region (diffusion of LC from bright to dark
region) creates a Bragg grating with alternate polymer-rich and LC-rich regions. A periodic refractive
index profile is formed in the cell, and thus light can be diffracted. Morphology and diffraction
properties of the grating depend upon writing set-up, materials, diffusion rate, curing conditions and
the phase separation process Typical morphology, the working principle and electro-optical properties
of HPDLCs are thoroughly elaborated in chapter 5 of the recently published book [109]. Promising
applications of HPDLCs include diffraction gratings (DGs), polymer slices (POLICRYPS), waveguides,
autostereoscopic image splitter, three-dimensional (3D) data storage and photonic crystals [110–117].
Molecules 2020, 25, 5510 11 of 22
Despite several attempts to overcome the need for a strong electric field when the diffraction
effects are not required, E-O efficiency of the HPDLCs was compromised. In the United States,
TJ. Buning et al. [118] of the Beam Engineering for Advanced Measurements Company, Florida
and Air Force Research Laboratory, Wright-Patterson Air Force Base, Dayton, Ohio, demonstrated
highly-efficient and fast DGs which were invisible (transparent) in the off state and exhibited
strong diffractive properties upon the application of a moderate E-field by employing photocurable
LC monomer and nematic LCs using holographic photopolymerization techniques. Similarly,
Manda et al. [119] of Chonbuk National University, Korea, obtained DGs which were optically
transparent in the visible wavelength regime by tuning the LC droplet size below the visible wavelength.
Efficient HPDLCs having low driving voltages and high diffraction efficiency were realized by using a
photoinhibitor, acrylamide and doping ZnS nanoparticles [120,121]. Also, a concurrent photoinitiation
and inhibition upon green light illumination was disclosed, which significantly improved the diffraction
efficiency of HPDLC gratings and afforded their utilization in storage of colored 3D images [122].
7.3. Novel Films

Although the displays based on PDLC films are simple and bright, there is huge room for
improvement. In this regard, optical diffusers play a critical role in preventing light sources
from being seen directly by viewers in the lighting system. Additionally, optical diffusers are a
key optical component in light-emitting diodes (LEDs), which can spread the point light source
uniformly without high intensity spots. In our group Zhou et al. [7,123–126] designed optical
diffusers with very high efficiency. Recently, an optical diffuser was prepared via a thiol ene click
reaction comprising of 1:1 of ene and thiol and exhibited high transmission (98.49%) and high
haze (91.77%). Similarly, display devices with narrow viewing angle (NVA) and wide viewing
angle (WVA) characteristics for privacy protection and information sharing were demonstrated [127].
Han et al. [128] from the University of Science and Technology, Beijing, China, fabricated a controllable
antipeeping device with a laminated structure of microlouver and PDLC films which reversibly
switched between a wider viewing angle range (VAR) for the WVA mode and a narrower viewing
angle range (VAR) for the NVA mode at 0 V and 8 V, respectively. In our recent studies novel
QDs films based on a liquid crystals/polymer composite were developed [8,129]. The fluorescence
enhancement of QDs-doped TiO2 /polymer, LCs/polymer and TiO2 /LCs/polymer composite systems
were comparatively studied. The photoluminescence enhancement of QDs was induced by the
synergistic effect of LCs/polymer composite and TiO2 nanoparticles (150 nm particle size) having
0.1 wt% loading content. The enhancement factor of QDs-doped TiO2 /LCs/polymer composite film
was approximately 6-fold relative to the QDs-doped polymer. The polymer dispersed vinyl-ether
liquid crystals (PDVLC), polymer dispersed crosslinked vinyl-ether liquid crystals (PDCVLC) and
fluorine-containing polymer-dispersed crosslinked vinyl-ether liquid crystals (F-PDCVLC) QDs films
were fabricated by dual-step polymerization as shown in Figure 6. The reported PDVLC film had
fluorescence enhancement and tuning, whereas the PDCVLC film not only maintained fluorescence
enhancement of the PDVLC film but also improved its water-resistant performance. Similarly,
hydrophobic PDLC films for ecofriendly optoelectronic applications were demonstrated by the
encapsulation of cholesteryl acetate LC by a chitosan polymer matrix [130].
Molecules 2020, 25, 5510 12 of 22
Figure 6.
Figure 6. Schematic
Schematicillustration
illustrationofofthe
thepreparation
preparation of of crosslinked
crosslinked V-LCs/polymer
V-LCs/polymer composite
composite films.
films. (a)
(a) The
The homogeneous
homogeneous polymeric
polymeric syrupsyrup containing
containing quantum quantum dots sandwiched
dots sandwiched between between two conductive
two conductive ITO glass
ITO glass coating
substrates substrates
withcoating
PVA. (b)with
ThePVA.PDVLC (b)film
ThewasPDVLC
formed film
by was formed
the first by thepolymerization
step radical first step radical of
polymerization of weak UV light to initiate microphase between V-LCs and
weak UV light to initiate microphase between V-LCs and polymer matrix. (c) Enlarged V-LCs domains polymer matrix. (c)
Enlarged
with V-LCs
randomly domains
oriented with
liquid randomly
crystal mixture.oriented
(d) V-LCs liquid
werecrystal mixture. aligned
homeotropically (d) V-LCs whenwerethe
homeotropically
electrical field wasaligned
applied. when
(e) Thethe electrical
second field was
step cationic applied. (e)
polymerization The second
of intense UV lightstep
wascationic
carried
polymerization
out to prepare the of intense
PDCVLC UVbylight
the was carried out to
polymerization of prepare the PDCVLC
V-LC monomers. by the polymerization
(f) Enlarged V-LCs domains of
V-LCthe
with monomers. (f) Enlarged
polymerization of V-LCV-LCs domains
monomers. withF-PDCVLC
(g) The the polymerization of V-LC monomers.
film was developed (g) The
by introducing the
F-PDCVLC
perfluoro film was
acrylate developed
monomers into by
the introducing
original syrup theand
perfluoro
repeating acrylate
the abovemonomers
dual-stepinto the original
polymerization.
syrup
(h) and repeating
Enlarged the above
polymer matrix with dual-step
the perfluoropolymerization. (h) Enlarged
acrylate monomers. Reproducedpolymer
with matrix withfrom
permission the
perfluoro
ref. acrylate monomers.
[8]. Copyright 2019, ELSEVIER Reproduced with permission from ref. [8]. Copyright 2019, ELSEVIER
Publications.
Publications.
7.4. Device Components
7.4. Device
PDLCsComponents
have been used as device components for OLED, Micro-LEDs, solar power collector, OFET,
and solar
PDLCs cells.
haveInbeen
UnitedusedStates, D.K.Yang
as device et al. [9]for
components of Kent
OLED, State University,solar
Micro-LEDs, Ohio, demonstrated
power collector,
PDLC
OFET, and solar cells. In United States, D.K.Yang et al. [9] of Kent State University, along
films in which LC droplets were unidirectionally aligned under an applied electric field Ohio,
the film normalPDLC
demonstrated direction.
films This PDLCLC
in which film was used
droplets to enhance
were the lightaligned
unidirectionally outcoupling
underefficiency
an applied of
OLEDs, because
electric field it could
along selectively
the film normalscatter light This
direction. emitted
PDLCfromfilm
the OLED
was usedinto to
directions
enhancewith the large
light
incident angles but not light with small incident angles, and thus reduced
outcoupling efficiency of OLEDs, because it could selectively scatter light emitted from the OLED light loss due to total
internal reflection.
into directions withSimilarly, Wu etangles
large incident al. [131]
butofnot
thelight
University of Central
with small Florida,
incident USA,
angles, anddemonstrated
thus reduced
volumetric light-shaping PDLC films for mini LED-backlit liquid crystal displays
light loss due to total internal reflection. Similarly, Wu et al. [131] of the University of Central (LCDs). PDLC films
Florida,
with a thickness 50-µm were prepared without surface alignment using
USA, demonstrated volumetric light-shaping PDLC films for mini LED-backlit liquid crystal displays a mixture containing LC
(ZLI
(LCDs). 1844PDLC= 49.92%)
filmsandwithprepolymer
a thickness (NOA 60 =were
50-μm 47.11%). With proper
prepared without material
surfaceengineering,
alignment usingpassivea
PDLC films with angle-selective scattering properties were shown which
mixture containing LC (ZLI 1844= 49.92%) and prepolymer (NOA 60=47.11%). With proper material respond to angles rather than
spatial locations.
engineering, passive PDLC films with angle-selective scattering properties were shown which
respondMonolithic
to anglesintegration
rather thanofspatial
CNT thin-film
locations.transistor driver circuits with PDLC pixels has been
studied [132]. The fabricated PDLC
Monolithic integration of CNT thin-film pixels possessed good
transistor contrast
driver and high-performance.
circuits with PDLC pixels has In Korea,
been
Song et al. [133] of the Kyungpook National University, Daegu, demonstrated
studied [132]. The fabricated PDLC pixels possessed good contrast and high-performance. In Korea, PDLC integrated-organic
field-effect
Song et al. transistors
[133] of the(PDLC-i-OFETs).
Kyungpook National The PLDC sensing
University, layersdemonstrated
Daegu, were prepared PDLCby embedding
integrated-
4,4 0 -pentyl-cyanobiphenyl (5CB) microdots in the poly (methyl methacrylate) (PMMA) matrix,
organic field-effect transistors (PDLC-i-OFETs). The PLDC sensing layers were prepared by
which
embedding were 4,4′-pentyl-cyanobiphenyl
integrated on the flexible OFETs with 200 µm-thick
(5CB) microdots in the poly poly (ethylene
(methyl naphthalate)
methacrylate) (PEN)
(PMMA)
substrates as shown in Figure 7. The PDLC layers were found to contain
matrix, which were integrated on the flexible OFETs with 200μm-thick poly (ethylene naphthalate)well-aligned LC micro-dots
embedded
(PEN) substrates in the PMMA
as shown layers. The fabricated
in Figure PDLC-i-OFET
7. The PDLC devices
layers were weretoable
found to sense
contain four different
well-aligned LC
micro-dots embedded in the PMMA layers. The fabricated PDLC-i-OFET devices were able to sense
four different stimulations such as weak air (gas) flow, strong physical force (touch), light and heat,
Molecules 2020, 25, 5510 13 of 22
as shown in Figure
stimulations such as7b. The air
weak concept of combining
(gas) flow, PDLC and
strong physical OFET
force could
(touch), contribute
light toas
and heat, the further
shown in
development
Figure 7b. Theof multifunctional
concept of combiningorganic
PDLC andsensory
OFET devices for various
could contribute to theapplications including
further development of
humanoid robots, artificial skin and wearable sensors.
multifunctional organic sensory devices for various applications including humanoid robots, artificial
skin and wearable sensors.
Figure 7. Structure and basic device performances of flexible PDLC-i-OFETs. (a) Illustration for the
device structure and materials used in this work (photographs demonstrate attachment of flexible
Figure 7. Structure and basic device performances of flexible PDLC-i-OFETs. (a) Illustration for the
PDLC-i-OFET array sensors on human hands), (b) Sensing performance by weak gas flow stimulations
device structure and materials used in this work (photographs demonstrate attachment of flexible
and mechanism change of 5CB alignment in the channel region of PDLC-i-OFET devices according to
PDLC-i-OFET array sensors on human hands), (b) Sensing performance by weak gas flow
applied voltages and nitrogen gas stimulations: illustrations for possible orientation of 5CB molecules
stimulations and mechanism change of 5CB alignment in the channel region of PDLC-i-OFET devices
in the LC micro-dots in the channel layers. Reproduced with permission from ref. [133] Copyright 2017,
according to applied voltages and nitrogen gas stimulations: illustrations for possible orientation of
Springer Nature Publications.
5CB molecules in the LC micro-dots in the channel layers. Reproduced with permission from ref. [133]
Copyright 2017, PDLCs-based
Conventional Springer Naturewindows
Publications.
require external electricity to operate, and these devices
cannot be combined with traditional solar cells for energy savings. To achieve nearly zero
Conventional PDLCs-based
energy-consuming windows require
windows, luminescent external electricity
solar concentrators (LSCs)towere
operate, and these
integrated withdevices
PDLC
cannot be combined with traditional solar cells for energy savings. To achieve nearly
devices [134–137]. The schematic illustration of LSC-coupled PDLC is shown in Figure 8a,b. zero energy-
consuming windows,
An important aspect of luminescent
the LSC devicesolar
is itsconcentrators (LSCs) were
capability to harvesting integrated
direct, withground-reflected
diffused and PDLC devices
[134–137]. The schematic illustration of LSC-coupled PDLC is shown in Figure 8a,b. An important
aspect of the LSC device is its capability to harvesting direct, diffused and ground-reflected light.
Molecules 2020, 25, 5510 14 of 22
Therefore, a measurable
light. Therefore, amount amount
a measurable of energyofcan be generated
energy even in nonideal
can be generated even inillumination conditions.
nonideal illumination
In Korea, Mateen
conditions. et al.Mateen
In Korea, of Dongguk
et al.University,
of Dongguk coupled an LSC
University, based on
coupled an luminophores (MACROLEX
LSC based on luminophores
Fluorescent
(MACROLEX Yellow 10GN and
Fluorescent MACROLEX
Yellow 10GN andFluorescent
MACROLEX Red G (Bayer, Germany))
Fluorescent Red G (Bayer,andGermany))
PDLC (E7 and and
NOA
PDLC65).(E7The
andPDLC
NOAwas 65). placed on thewas
The PDLC backside
placedofonthe LSC
the to reduce
backside the LSC
of the backside light losses
to reduce of LSC
the backside
because PDLC
light losses in offbecause
of LSC mode acted
PDLCasina offbackside scattering
mode acted as a reflector
backsideas shown inreflector
scattering Figure 8b–d. PDLC
as shown in
film not8b–d.
Figure only reflected
PDLC film thenot
untrapped light into
only reflected the the LSC partlight
untrapped but into
also the
redirected
LSC part thebut
light that
also was not
redirected
absorbed (i.e.,was
the light that outside the absorption
not absorbed range ofthe
(i.e., outside theabsorption
luminophores)
rangetowards the edges, andtowards
of the luminophores) thus to the
the
attached solar cells. The electricity produced by the LSC part was successfully employed
edges, and thus to the attached solar cells. The electricity produced by the LSC part was successfully for the
switching
employed operation of the PDLC
for the switching device.
operation of the PDLC device.
Figure 8. (a) Schematic representation and working principle of PDLC-coupled LSC [138] (b) Schematic
Figure 8. (a) Schematic representation and working principle of PDLC-coupled LSC [138] (b)
exploded representations of an active LSC window containing red-NIR phosphorescent octahedral
Schematic exploded representations of an active LSC window containing red-NIR phosphorescent
molybdenum nanoclusters composed of a PDLC matrix containing the phosphorescent inorganic emitter
octahedral molybdenum nanoclusters composed of a PDLC matrix containing the phosphorescent
surrounded by PV cells on its edges [138]. Figure 8a,b reproduced with permission from Ref. [138]
inorganic emitter surrounded by PV cells on its edges [138]. Figure 8a,b reproduced with permission
Copyright 2017, ACS Publications (c) PDLC backside emissions of an N-CQDs-based waveguide
from Ref. [138] Copyright 2017, ACS Publications (c) PDLC backside emissions of an N-CQDs-based
coupled with no PDLC and with PDLC. The driving voltage in the ON state was kept constant at 50 V
waveguide coupled with no PDLC and with PDLC. The driving voltage in the ON state was kept
(d) Backside emission power of PDLC-LSC devices in the OFF and ON mode. The driving voltage
constant at 50 V (d) Backside emission power of PDLC-LSC devices in the OFF and ON mode. The
in the ON mode was kept constant at 50 V in both devices. (e) Color possibilities of transmitted
driving voltage in the ON mode was kept constant at 50 V in both devices. (e) Color possibilities of
light through the ON and OFF states of a waveguide-coupled PDLC device plotted on a CIE 1931 XY
transmitted light through the ON and OFF states of a waveguide-coupled PDLC device plotted on a
chromaticity diagram. Figure 8c–e reproduced with permission from Ref. [134,136]. Copyright 2019,
CIE 1931 XY chromaticity diagram. Figure 8c–e reproduced with permission from Ref. [134,136].
ELSEVIER Publications.
Copyright 2019, ELSEVIER Publications.
7.5. Others
7.5. Others
The application of PDLC composites in biomedical devices has shown significant promise [139,140].
The
In Romania,application of[141–143]
Marin et al. PDLC composites in biomedical
from the Institute devices has
of Macromolecular shown prepared
Chemistry, significant promise
ecofriendly
[139,140].
PDLCs forIn Romania,
sensing Marin et
applications by al. [141–143]biocompatible
embedding from the Institute
LCs in of
theMacromolecular
polymer matrix of Chemistry,
polyvinyl
prepared ecofriendly
alcohol-boric PDLCs
acid (PVAB). Thefor sensing applications
composites films exhibited bywell-defined
embedding droplets
biocompatible LCs in the
of submicrometric
polymer matrix
size (250–650 of polyvinyl
nm). It was found alcohol-boric acid (PVAB).
that the composite filmsThe composites
possessed filmswettability
moderate exhibited well-defined
and showed
droplets of submicrometric
selective responsiveness for Lsize
or D(250–650 nm). Itacids
sugars, amino wasandfound
DNA. that the composite films possessed
moderate
PDLCswettability
were alsoand showed
shown to beselective
sensitiveresponsiveness
to ultrasoundfor L or D the
through sugars, amino acids
acousto-optic and DNA.
effect. In the
PDLCs were also shown to be sensitive to ultrasound through the acousto-optic
United Kingdom, Edwards et al. [144] of the University of Warwick, Coventry, prepared a PDLC effect. In the
United Kingdom,
sensor (E7: NOA68=Edwards
75:25)etand
al. [144] of the
studied theUniversity
acousto-opticof Warwick,
response Coventry,
of PDLCsprepared
coupled awithPDLCan
sensor (E7: NOA68= 75:25) and studied the acousto-optic response of PDLCs
ultrasound transducer over a broad frequency range (0.3–10 MHz). The displacements required to coupled with an
ultrasound transducer over
produce acousto-optic a broad
clearing of PDLCfrequency rangebetween
films were (0.3–10 around
MHz). The2 anddisplacements
50 nm. Theserequired
frequencyto
produce acousto-optic clearing of PDLC films were between around 2 and 50 nm. These frequency
dependent displacements could be used for ultrasound visualization in nondestructive testing.
Molecules 2020, 25, 5510 15 of 22
dependent displacements could be used for ultrasound visualization in nondestructive testing. Recently,
Firoozi et al. [145] reported a harmonic response in PDLCs to an applied square-wave voltage at low
frequencies (4.5–5.0 Hz) enabling their use in interferometers. Another important application of the
PDLCs is a polarization-dependent (Micro lenticular lens array) MLA device [146]. This device was
used to realize a 3D image when the polarized 2D image arrays encountered the microlens [147].
8. Conclusions
As detailed in this review, significant achievements have been made in the preparation, properties
and applications of polymer dispersed liquid crystal composite films between 2014 and 2020.
The electro-optical properties of the PDLC films were optimized by the structural variation of
monomers and liquid crystals, two-step polymerization as well as doping nanoparticles, dyes and
CNTs. Specifically, the two-step polymerization paved a new way to improve the electro-optical and
mechanical performance of PDLC composite films. Meanwhile, significant progress in applications
was also achieved such as diffuser films, antipeeping films, QDs films, device components of OLED,
OFET, sensors, photovoltaics, energy harvesting, actuators, biomedical applications, etc. Featuring
the advantages of simple preparation, cost-efficiency, large-area manufacturing and flexibility, PDLC
composite films promise to promote and expand the development of next-generation smart windows,
displays, wearable devices and sensors.
Funding: This work was supported by the National Key R&D Program of China (2019YFC1904702), the National
Natural Science Foundation of China (NSFC) (Grant No. 51272026), the joint fund of the ministry of education for
equipment pre research (6141A02033238).
Conflicts of Interest: The authors declare no conflict of interest.
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Molecules 2020, 25, 5510; doi:10.3390/molecules25235510 www.mdpi.com/journal/molecules

Figure 1.1. Operating

PDLCs can can bebe prepared

Here, we review the recent developments in preparation, experimental investigation and

3. Preparation of Modified PDLC Composite Film

5. Preparation of Dye-Doped PDLC Composite Film

7.1. Traditional Applications

7.3. Novel Films

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