National Science Review,
Journal Year:
2024,
Volume and Issue:
11(6)
Published: March 23, 2024
ABSTRACT
Multi-boron-embedded
multiple
resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
show
promise
for
achieving
both
high
color-purity
emission
and
exciton
utilization
efficiency.
However,
their
development
is
often
impeded
by
a
limited
synthetic
scope
excessive
molecular
weights,
which
challenge
material
acquisition
organic
light-emitting
diode
(OLED)
fabrication
vacuum
deposition.
Herein,
we
put
forward
B‒N
covalent
bond-involved
π-extension
strategy
via
post-functionalization
of
MR
frameworks,
leading
to
the
generation
high-order
B/N-based
motifs.
The
structurally
electronically
extended
π-system
not
only
enhances
rigidity
narrow
linewidth
but
also
promotes
reverse
intersystem
crossing
mitigate
efficiency
roll-off.
As
illustrated
examples,
ultra-narrowband
sky-blue
(full-width
at
half-maximum
as
small
8
nm
in
n-hexane)
have
been
developed
with
multi-dimensional
improvement
photophysical
properties
compared
precursor
emitters,
enables
narrowband
OLEDs
external
quantum
efficiencies
(EQEmax)
up
42.6%,
company
alleviated
decline
brightness,
representing
best
reported
single-host
OLEDs.
success
these
highlights
effectiveness
our
design
advanced
MR-TADF
confirms
extensive
potential
high-performance
optoelectronic
devices.
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.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(23), P. 12550 - 12560
Published: June 5, 2023
Multiple
resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
are
promising
candidates
for
narrowband
organic
light-emitting
diodes,
but
their
electroluminescent
performance
is
typically
hindered
by
the
slow
reverse
intersystem
crossing
rate
(kRISC).
Herein,
we
present
an
effective
strategy
to
introduce
a
multichannel
(RISC)
pathway
with
large
spin-orbit
coupling
orthogonally
linking
electron-donating
unit
MR
framework.
Through
delicate
manipulation
of
excited-state
energy
levels,
additional
intersegmental
charge
transfer
triplet
state
could
be
"silently"
induced
without
perturbing
character
lowest
excited
singlet
state.
The
proof-of-concept
emitter
CzBN3
not
only
affords
23-fold
increase
kRISC
compared
its
prototypical
skeleton
also
realizes
close-to-unity
photoluminescence
quantum
yield,
radiative
constant,
and
very
narrow
emission
spectrum.
These
merits
enable
high
maximum
external
efficiency
(EQEmax)
up
37.1%
alleviated
roll-off
in
sensitizer-free
device
(EQE1000
=
30.4%),
further
boost
(EQEmax/1000
42.3/34.1%)
realized
hyperfluorescent
device.
state-of-the-art
validates
superiority
our
molecular
design
strategy.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(7)
Published: Dec. 13, 2022
Abstract
Developing
solution‐processable
red
organic
light‐emitting
diodes
(OLEDs)
with
high
color
purity
and
efficiency
based
on
multiple
resonance
thermally
activated
delayed
fluorescence
(MR‐TADF)
is
a
formidable
challenge.
Herein,
by
introducing
auxiliary
electron
donor
acceptor
moieties
into
the
highest
occupied
molecular
orbital
(HOMO)
lowest
unoccupied
(LUMO)
distributed
positions
of
skeleton
simultaneously,
an
effective
strategy
to
obtain
MR‐TADF
emitters
was
represented.
The
proof‐of‐the‐concept
molecule
BN‐R
exhibits
narrowband
pure‐red
emission
at
624
nm,
luminous
94
%
narrow
bandwidth
46
nm.
Notably,
fabricated
OLED
state‐of‐the‐art
external
quantum
over
20
Commission
Internationale
de
I’Éclairage
coordinates
(0.663,
0.337)
long
operational
lifetime
(LT
50
)
1088
hours
initial
luminance
1000
cd
m
−2
.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
145(3), P. 1505 - 1511
Published: Dec. 22, 2022
Multiple-resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
have
emerged
as
an
important
component
of
organic
light-emitting
diodes
(OLEDs)
because
their
narrowband
emission
and
high
exciton
utilization
efficiency.
However,
the
chemical
space
MR-TADF
remains
mostly
unexplored
lack
suitable
synthetic
protocols.
Herein,
we
demonstrate
a
sequential
multiple
borylation
reaction
that
provides
new
synthetically
accessible
space.
ω-DABNA,
proof-of-concept
material,
exhibited
green
TADF
with
full
width
at
half-maximum
22
nm
small
singlet-triplet
energy
gap
13
meV.
The
OLED
employing
it
emitter
electroluminescence
512
nm,
Commission
International
de
l'Éclairage
coordinates
(0.13,
0.73)
external
quantum
efficiency
(EQE)
31.1%.
Moreover,
device
showed
minimum
roll-off,
EQE
29.4%
1000
cd
m-2.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(12)
Published: Jan. 8, 2023
Abstract
Multiple‐resonance
(MR)
thermal
activated
delayed
fluorescence
(TADF)
emitters
have
attracted
increasing
attention
in
organic
electroluminescence
devices,
owing
to
their
superior
quantum
efficiency
and
narrowband
emission
for
high
color
purity.
However,
MR‐TADF
materials
often
suffer
from
severe
aggregation‐caused
quenching
(ACQ)
roll‐off
problems
due
rigid
planar
structures
the
lack
of
sufficient
charge‐transfer
(CT)
characters
with
inefficient
reverse
intersystem
crossing
(RISC).
Herein,
by
attaching
electron‐rich
triphenylamine
(TPA)
twisted
spatial
conformation
MR
framework,
two
efficient
emitters,
namely
BNCz‐pTPA
BNCz‐mTPA
,
are
developed.
The
TPA
substituent
endows
new
aggregation‐induced
enhancement
(AIEE)
ACQ
suppression.
unprecedented
AIEE‐MR‐TADF
exhibit
CT
character
high‐lying
triplet
excited
states
faster
RISC,
while
locally‐excited
(LE)
first
singlet
state
is
retained
efficiency.
An
light‐emitting
diode
(OLED)
based
on
exhibits
a
maximum
external
27.3%
slow
roll‐off,
demonstrating
much
higher
performances
than
those
BNCz
‐based
OLED.
This
study
may
provide
simple
but
effective
approach
constructing
high‐performance
wide‐color‐gamut
OLED
displays.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(30)
Published: April 19, 2023
Polycyclic
heteroaromatics
with
multi-resonance
(MR)
characteristics
are
attractive
materials
for
narrowband
emitters
in
wide-color-gamut
organic
light-emitting
diodes.
However,
MR
pure-red
colors
still
rare
and
usually
exhibit
problematic
spectral
broadening
when
redshifting
emission.
Here,
a
emitter
is
reported
by
fusing
indolocarbazole
segments
into
boron/oxygen-embedded
skeleton,
realizing
BT.2020
red
electroluminescence
the
first
time
together
high
efficiency
an
ultralong
lifetime.
The
rigid
segment
possesses
strong
electron-donating
ability
due
to
its
para-positioned
nitrogen-π-nitrogen
backbone
also
enlarges
π-extension
of
skeleton
suppress
structural
displacement
during
radiation,
achieving
concurrently
redshifted
narrowed
emission
spectrum.
An
maximum
at
637
nm
full
width
half-maxima
merely
32
(0.097
eV)
recorded
toluene.
corresponding
device
simultaneously
exhibits
CIE
coordinates
(0.708,
0.292)
precisely
matching
point,
external
quantum
34.4%
low
roll-off
LT95
(time
95%
initial
luminance)
>10
000
h
1000
cd
m-2
.
These
performance
superior
even
those
state-of-the-art
perovskite
quantum-dot-based
devices
this
specific
color,
paving
way
toward
practical
applications.
Communications Chemistry,
Journal Year:
2022,
Volume and Issue:
5(1)
Published: Nov. 10, 2022
The
subclass
of
multi
resonant
thermally
activated
delayed
fluorescent
emitters
(MR-TADF)
containing
boron
atoms
has
garnered
significant
attention
in
the
field
organic
light
emitting
diode
(OLED)
research.
Among
boron-based
MR-TADF
emitters,
double
boron-embedded
(DB-MR-TADF)
show
excellent
electroluminescence
performances
with
high
photoluminescence
quantum
yields,
narrow
band
emission,
and
beneficially
small
singlet-triplet
energy
levels
all
full-color
gamut
regions.
This
article
reviews
recent
progress
DB-MR-TADF
particular
to
molecular
design
concepts,
synthetic
routes,
optoelectronic
properties,
OLED
performance,
giving
future
prospects
for
real-world
applications.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(50), P. 22976 - 22984
Published: Dec. 7, 2022
Multiresonance
thermal
activated
delayed
fluorescence
(MR-TADF)
materials
with
an
efficient
spin-flip
transition
between
singlet
and
triplet
excited
states
remain
demanding.
Herein,
we
report
MR-TADF
compound
(BN-Se)
simultaneously
possessing
(reverse)
intersystem
crossing
(ISC/RISC),
fast
radiative
decay,
close-to-unity
quantum
yield,
narrowband
emission
by
embedding
a
single
selenium
atom
into
common
4,4'-diazaborin
framework.
Benefitting
from
the
high
RISC
efficiency
accelerated
heavy-atom
effect,
organic
light-emitting
diodes
(OLEDs)
based
on
BN-Se
manifest
excellent
performance
external
of
up
to
32.6%
ultralow
roll-off
1.3%
at
1000
cd
m-2.
Furthermore,
ISC
small
inherent
energy
loss
also
render
superior
photosensitizer
realize
first
example
visible
(λex
>
450
nm)-to-UV
(λem
<
350
nm)
triplet-triplet
annihilation
upconversion,
(21.4%)
extremely
low
threshold
intensity
(1.3
mW
cm-2).
This
work
not
only
aids
in
designing
advanced
pure
molecules
exciton
dynamics
but
highlights
value
compounds
beyond
OLED
applications.
Advanced Photonics Research,
Journal Year:
2022,
Volume and Issue:
3(11)
Published: Sept. 4, 2022
Recently,
the
exploration
of
boron
(B)/heteroatom‐embedded
polycyclic
nanographites
featuring
multiresonance
thermally
activated
delayed
fluorescence
(MR‐TADF)
garners
astonishing
attention
to
promote
advancement
organic
light‐emitting
diodes
(OLEDs).
Contrary
traditional
donor–acceptor
(D–A)‐type
TADF
emitters,
MR‐TADF
emitters
manifest
narrowband
emission
with
full
width
at
half
maximum
(FWHM
≤
40
nm)
and
superior
photoluminescence
quantum
yield
(PLQY)
coupled
small
singlet–triplet
energy
splitting,
which
appeal
their
potential
as
promising
candidates
in
fabricating
efficient
OLEDs.
Growingly,
deliver
benchmark
device
performance
comparable
conventional
TADF/phosphorescent
emitters.
However,
they
are
suffering
from
major
drawbacks
such
difficult
realize
full‐color
slow
exciton
upconversion
dynamics,
aggregation‐caused
quenching,
severe
efficiency
roll‐off,
poor
operational
lifetime,
jeopardizes
practical
applicability.
Herein,
a
comprehensive
review
on
B‐based
reported
till
date
is
presented,
focusing
different
design
strategies
documented
for
circumventing
aforementioned
shortcomings.
This
divided
into
several
subgroups
based
color
materials
draw
electronics
community
toward
constructing
MR‐OLEDs.
Finally,
challenges
opportunities
discussed.