Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(6)
Published: Dec. 14, 2022
Chiral
boron/nitrogen
doped
multiple
resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
are
promising
for
highly
efficient
and
color-pure
circularly
polarized
organic
light-emitting
diodes
(CP-OLEDs).
Herein,
we
report
two
pairs
of
MR-TADF
materials
(Czp-tBuCzB,
Czp-POAB)
based
on
planar
chiral
paracyclophane
with
photoluminescence
quantum
yields
up
to
98
%.
The
enantiomers
showed
symmetric
spectra
dissymmetry
factors
|gPL
|
1.6×10-3
in
films.
Meanwhile,
the
sky-blue
CP-OLEDs
(R/S)-Czp-tBuCzB
an
external
efficiency
32.1
%
narrowest
full-width
at
half-maximum
24
nm
among
reported
CP-OLEDs,
while
devices
(R/S)-Czp-POAB
displayed
first
nearly
pure
green
CP
electroluminescence
|gEL
10-3
level.
These
results
demonstrate
incorporation
chirality
into
emitter
is
a
reliable
strategy
constructing
CP-OLEDs.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
34(3)
Published: Nov. 12, 2021
Multiresonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
manifest
great
potential
for
organic
light-emitting
diodes
(OLEDs)
due
to
their
high
exciton-utilization
efficiency
and
narrowband
emission.
Nonetheless,
tendency
toward
self-quenching
caused
by
strong
interchromophore
interactions
would
induce
doping
sensitivity
deteriorate
the
device
performances,
effective
strategy
construct
quenching-resistant
without
sacrifycing
color
purity
is
still
be
developed.
By
segregating
planar
MR-TADF
skeleton
using
two
bulky
carbazolyl
units,
herein
a
highly
emissive
molecule
with
enhanced
quenching
resistance
reported.
The
steric
effect
largely
removes
formation
of
detrimental
excimers/aggregates,
boosts
performance
corresponding
devices
maximum
external
quantum
(EQEmax
)
up
40.0%
full
width
at
half
(FWHM)
25
nm,
representative
only
example
single
OLED
that
can
concurrently
achieve
narrow
bandwidth
EL
surpassing
40%
date.
Even
ratio
30
wt%,
EQEmax
retained
33.3%
nearly
unchanged
emission
spectrum.
This
work
provides
viable
approach
realize
doping-insensitive
extreme
high-end
displays.
Advanced Optical Materials,
Journal Year:
2022,
Volume and Issue:
10(22)
Published: Sept. 23, 2022
Abstract
Organic
thermally
activated
delayed
fluorescence
(TADF)
materials
have
attracted
significant
research
interest
in
the
field
of
organic
electronics
because
their
inherent
advantage
100%
exciton
utilization
capability
light‐emitting
diodes
(OLEDs)
without
use
noble
metals.
However,
despite
high
internal
electroluminescence
quantum
efficiencies
approaching
unity,
broad
emission
spectra
with
sizable
full
width
at
half
maxima
(FWHM;
60–100
nm)
present
a
critical
issue
that
must
be
solved
for
application
ultrahigh‐definition
OLED
displays.
Recently,
new
paradigm
TADF
featuring
multiple
resonance
(MR)
effect
based
on
heteroatom‐doped
polycyclic
aromatic
frameworks,
referred
to
as
MR‐TADF
materials,
has
emerged
and
garnered
considerable
owing
remarkable
features
efficient
narrowband
emissions
extremely
small
FWHMs
(≤30
nm).
Currently,
occupy
prominent
position
cutting‐edge
from
both
chemical
physical
perspectives.
This
review
article
focuses
recent
progress
emissive
systems
perspective
molecular
design,
photophysical
properties,
performance
OLEDs.
The
current
status
future
prospects
this
advanced
material
technology
are
discussed
comprehensively.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
34(9)
Published: Dec. 8, 2021
To
achieve
an
ultimate
wide
color
gamut
for
ultrahigh-definition
displays,
there
is
great
demand
the
development
of
organic
light-emitting
diodes
(OLEDs)
enabling
monochromatic,
ultrapure
blue
electroluminescence
(EL).
Herein,
high-efficiency
and
OLEDs
based
on
polycyclo-heteraborin
multi-resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
materials,
BOBO-Z,
BOBS-Z,
BSBS-Z,
are
reported.
The
key
to
design
present
luminophores
exquisite
combination
interplay
multiple
boron,
nitrogen,
oxygen,
sulfur
heteroatoms
embedded
in
a
fused
polycyclic
π-system.
Comprehensive
photophysical
computational
investigations
this
family
MR-TADF
materials
reveal
that
systematic
implementation
chalcogen
(oxygen
sulfur)
atoms
can
finely
modulate
emission
while
maintaining
narrow
bandwidth,
as
well
spin-flipping
rates
between
excited
singlet
triplet
states.
Consequently,
BSBS-Z
demonstrate
narrowband
EL
emission,
with
peaks
at
445-463
nm
full
width
half
maxima
18-23
nm,
leading
Commission
Internationale
de
l'Éclairage-y
coordinates
range
0.04-0.08.
Particularly,
incorporating
sulfur-doped
BOBS-Z
notably
high
maximum
external
quantum
efficiencies
26.9%
26.8%,
respectively,
small
efficiency
roll-offs
achieved
concurrently.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(44)
Published: Sept. 13, 2021
Abstract
Thermally
activated
delayed
fluorescence
(TADF)
emitters
featuring
preferential
horizontal
emitting
dipole
orientation
(EDO)
are
in
urgent
demand
for
enhanced
optical
outcoupling
efficiency
organic
light‐emitting
diodes
(OLEDs).
However,
simultaneously
manipulating
EDO
and
optoelectronic
properties
remains
a
formidable
challenge.
Here,
an
extended
linear
D–A–D
structure
with
both
enlarged
donor
(D)
acceptor
(A)
π‐systems
is
established,
not
only
elaborately
parallel
molecular
along
its
long
axis
by
multi‐driving‐forces
high
ratio
(
Θ
//
),
but
also
delocalizing
distribution
of
frontier
energy
levels
optimized
electronic
properties.
The
proof‐of‐the‐concept
emitter
affords
92%,
photoluminescence
quantum
yield
95%,
fast
reverse
intersystem
crossing
rate
1.16
×
10
6
s
‐1
.
corresponding
OLED
achieves
champion
maximum
external
39.1%
among
all
green
TADF
devices
without
any
light‐extraction
techniques,
together
power
112.0
lm
W
alleviated
roll‐off.
These
findings
may
inspire
even
better
full‐color
that
push
the
device
toward
theoretical
limits.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(43), P. 23142 - 23147
Published: Aug. 18, 2021
Abstract
Establishing
a
simple
and
versatile
design
strategy
to
finely
modulate
emission
colors
while
retaining
high
luminescence
efficiency
color
purity
remains
an
appealing
yet
challenging
task
for
the
development
of
multi‐resonance‐induced
thermally
activated
delayed
fluorescence
(MR‐TADF)
materials.
Herein,
we
demonstrate
that
strategic
introduction
electron‐withdrawing
imine
electron‐donating
amine
moieties
into
boron‐embedded
1,3‐bis(carbazol‐9‐yl)benzene
skeleton
enables
systematic
hypsochromic
bathochromic
shifts
narrowband
emissions,
respectively.
By
this
method,
effective
electroluminescence
tuning
was
accomplished
over
wide
visible
range
from
deep‐blue
yellow
(461–571
nm),
using
same
MR
molecular
system,
without
compromising
very
narrow
spectral
features.
Deep‐blue
organic
light‐emitting
diodes
with
maximum
external
quantum
efficiencies
as
19.0–29.2
%
superb
could
be
produced
family
color‐tunable
MR‐TADF
emitters.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(37), P. 20280 - 20285
Published: July 16, 2021
Abstract
Developing
organic
luminophores
with
unique
capability
of
strong
narrowband
emission
is
both
crucial
and
challenging
for
the
further
advancement
light‐emitting
diodes
(OLEDs).
Herein,
a
nanographitic
fused‐nonacyclic
π‐system
(
BSBS‐N1
),
which
was
strategically
embedded
multiple
boron,
nitrogen,
sulfur
atoms,
developed
as
new
multi‐resonance
thermally
activated
delayed
fluorescence
(MR‐TADF)
emitter.
Narrowband
sky‐blue
peak
at
478
nm,
full
width
half
maximum
24
photoluminescence
quantum
yield
89
%
obtained
.
Additionally,
spin‐orbit
coupling
enhanced
by
incorporating
two
thereby
facilitating
spin‐flipping
process
between
excited
triplet
singlet
states.
OLEDs
based
on
MR‐TADF
emitter
achieved
high
external
electroluminescence
efficiency
21.0
%,
improved
roll‐off.
Advanced Science,
Journal Year:
2021,
Volume and Issue:
8(24)
Published: Oct. 27, 2021
Abstract
The
development
of
simple,
efficient,
and
biocompatible
organic
luminescent
molecules
is
great
significance
to
the
clinical
transformation
biomaterials.
In
recent
years,
purely
thermally
activated
delayed
fluorescence
(TADF)
materials
with
an
extremely
small
single‐triplet
energy
gap
(Δ
E
ST
)
have
been
considered
as
most
promising
new‐generation
electroluminescence
emitters,
which
enormous
breakthrough
in
optoelectronics.
By
merits
unique
photophysical
properties,
high
structure
flexibility,
reduced
health
risks,
such
metal‐free
TADF
luminophores
attracted
tremendous
attention
biomedical
fields,
including
conventional
imaging,
time‐resolved
imaging
sensing,
photodynamic
therapy.
However,
there
currently
no
systematic
summary
for
applications,
presented
this
review.
Besides
a
brief
introduction
major
developments
material,
typical
mechanisms
fundamental
principles
on
design
strategies
nanomaterials
are
subsequently
described.
Importantly,
specific
emphasis
placed
discussion
various
applications.
Finally,
authors
make
forecast
remaining
challenges
future
developments.
This
review
provides
insightful
perspectives
clear
prospects
towards
rapid
biomedicine,
will
be
highly
valuable
exploit
new
materials.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(17)
Published: March 2, 2022
Emerging
multi-resonance
(MR)
thermally
activated
delayed
fluorescence
(TADF)
emitters
can
combine
100%
exciton
harvesting
and
high
color
purity
for
their
organic
light-emitting
diodes
(OLED).
However,
the
highly
planar
configurations
of
MR
molecules
lead
to
intermolecular-interaction-induced
quenching.
A
feasible
way
is
integrating
host
segments
into
molecules,
namely
a
"self-host"
strategy,
but
without
involving
additional
charge
transfer
and/or
vibrational
components
excited
states.
Herein,
an
ambipolar
self-host
featured
emitter,
tCBNDADPO,
demonstrated,
whose
segment
(DADPO)
significantly
comprehensively
improves
TADF
properties,
especially
greatly
accelerated
singlet
radiative
rate
constant
2.11
×
108
s-1
exponentially
reduced
nonradiative
constants.
Consequently,
at
same
time
as
preserving
narrowband
blue
emission
with
FWHM
≈28
nm
doping
concentration
30%,
tCBNDADPO
reveals
state-of-the-art
photoluminescence
electroluminescence
quantum
efficiencies
99%
respectively.
The
corresponding
internal
efficiency
supported
by
ultrasimple
trilayer
heavily
doped
device
demonstrates
feasibility
strategy
constructing
practically
applicable
materials.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(14)
Published: Feb. 1, 2022
Multiple
resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
show
great
potentials
for
high
color
purity
organic
light-emitting
diodes
(OLEDs).
However,
the
simultaneous
realization
of
photoluminescence
quantum
yield
(PLQY)
and
reverse
intersystem
crossing
rate
(kRISC
)
is
still
a
formidable
challenge.
Herein,
novel
asymmetric
MR-TADF
emitter
(2Cz-PTZ-BN)
designed
that
fully
inherits
PLQY
large
kRISC
values
properly
selected
parent
molecules.
The
resonating
extended
π-skeleton
with
peripheral
protection
can
achieve
96
%
fast
above
1.0×105
s-1
,
boost
performance
corresponding
pure
green
devices
an
outstanding
external
efficiency
(EQE)
up
to
32.8
without
utilizing
any
sensitizing
hosts.
Remarkably,
device
sufficiently
maintains
EQE
exceeding
23
at
luminance
1000
cd
m-2
representing
highest
value
reported
materials
same
luminescence.