Advanced Materials,
Год журнала:
2023,
Номер
36(1)
Опубликована: Ноя. 14, 2023
Abstract
Helicenes
exhibit
substantial
potential
as
circularly
polarized
luminescence
(CPL)
active
molecules.
However,
their
application
in
organic
light‐emitting
diodes
(CP‐OLEDs)
is
typically
hindered
by
the
challenge
of
integrating
both
high
color
purity
and
efficient
triplet‐harvesting
capability,
particularly
blue
spectral
region.
Herein,
a
series
hetero[6]helicene‐based
emitters
that
strategically
engineered
through
helical
extension
deep‐blue
double‐boron‐based
multiple
resonance
thermally
activated
delayed
fluorescence
(MR‐TADF)
motif,
introduced.
Importantly,
does
not
cause
apparent
structural
deformation
or
perturb
frontier
molecular
orbitals;
thus,
preserving
emission
MR‐TADF
characteristics
parent
molecule.
This
approach
also
leads
to
reduced
reorganization
energy,
resulting
with
narrower
linewidth
higher
photoluminescence
quantum
yield.
Further,
motif
enhances
racemization
barrier
improved
CPL
performance
dissymmetry
factor
values
up
1.5
×
10
−3
.
Exploiting
these
merits,
devices
incorporating
chiral
dopants
demonstrate
within
Broadcast
Service
Television
2020
color‐gamut
range,
record
external
efficiencies
(EQEs)
29.3%,
have
distinctive
electroluminescence
(CPEL)
signals.
Overall,
authors’
findings
underscore
promising
strategy
for
designing
narrowband
chiroptical
materials
advancing
high‐definition
displays.
Advanced Optical Materials,
Год журнала:
2022,
Номер
10(22)
Опубликована: Сен. 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.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(29)
Опубликована: Май 10, 2022
Multi-resonance
TADF
(MR-TADF)
emitters
are
promising
for
high-resolution
OLEDs,
but
the
concurrent
optimization
of
excited-state
dynamics
and
color
purity
remains
a
tough
challenge.
Herein,
three
deep-blue
MR-TADF
compounds
(BN1-BN3)
featuring
gradually
enlarged
ring-fused
structures
increased
rigidity
accessed
by
lithium-free
borylation
in
high
yields
from
same
precursor,
with
all
possessing
CIEy
coordinates
below
0.08.
Structure-property
investigations
demonstrate
strategic
improvement
oscillator
strength
(fosc
)
acceleration
reverse
intersystem
crossing
(RISC)
process
extending
π-skeleton,
where
BN3
realizes
maximum
external
quantum
efficiency
(EQE)
37.6
%
reduced
roll-off,
thus
showing
best
reported
OLEDs.
The
internal
regulation
these
validate
general
effectiveness
to
achieve
advanced
narrowband
higher-order
boron/nitrogen-based
MR
motifs.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(31)
Опубликована: Май 27, 2022
Narrowband
emissive
organoboron
emitters
featuring
the
multi-resonance
(MR)
effect
have
now
become
a
critical
material
component
for
constructing
high-performance
organic
light-emitting
diodes
(OLEDs)
with
pure
emission
colors.
These
MR
are
capable
of
exhibiting
high-efficiency
narrowband
thermally
activated
delayed
fluorescence
(TADF)
by
allowing
triplet-to-singlet
reverse
intersystem
crossing
(RISC).
However,
RISC
involving
spin-flip
exciton
upconversion
is
generally
rate-limiting
step
in
overall
TADF;
hence,
deeper
understanding
and
precise
control
dynamics
ongoing
crucial
challenges.
Here,
we
introduce
first
emitter
(CzBSe)
doped
selenium
atom,
demonstrating
record-high
rate
exceeding
108
s-1
,
which
even
higher
than
its
radiation
rate.
Furthermore,
process
CzBSe
can
be
accelerated
factors
≈20000
≈800,
compared
to
those
oxygen-
sulfur-doped
homologs
(CzBO
CzBS),
respectively.
Unlike
CzBO
CzBS,
photophysical
no
longer
RISC,
but
process;
this
behavior
completely
different
from
conventional
time-delaying
TADF
limited
slow
RISC.
Benefitting
ultrafast
spin
conversion
ability,
OLEDs
incorporating
achieved
maximum
external
electroluminescence
quantum
efficiency
as
high
23.9
%,
accompanied
MR-induced
blue
significantly
alleviated
roll-off
features.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(40)
Опубликована: Авг. 18, 2022
Multi-resonance
boron-nitrogen-containing
thermally
activated
delayed
fluorescence
(MR-TADF)
emitters
have
experienced
great
success
in
assembling
narrowband
organic
light-emitting
diodes
(OLEDs).
However,
the
slow
reverse
intersystem
crossing
rate
(kRISC
)
of
MR-emitters
(103
-105
s-1
that
will
lead
to
severe
device
efficiency
roll-off
has
received
extensive
attention
and
remains
a
challenging
issue.
Herein,
we
put
forward
"space-confined
donor-acceptor
(SCDA)"
strategy
accelerate
RISC
process.
The
introduction
SCDA
units
onto
MR-skeleton
induces
intermediate
triplet
states,
which
leads
multichannel
process
thus
increases
kRISC
.
As
illustrated
examples,
efficient
been
developed
with
sub-microsecond
lifetime
high
2.13×106
,
enables
assemble
high-performance
OLEDs
maximum
external
quantum
(EQEmax
as
32.5
%
an
alleviated
(EQE1000
:
22.9
%).
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(23), С. 12550 - 12560
Опубликована: Июнь 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,
Год журнала:
2022,
Номер
61(30)
Опубликована: Май 10, 2022
Highly
efficient
circularly
polarized
luminescence
(CPL)
emitters
with
narrowband
emission
remain
a
formidable
challenge
for
OLEDs
(CP-OLEDs).
Here,
promising
strategy
developing
chiral
concurrently
featuring
multi-resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
and
electroluminescence
(CPEL)
is
demonstrated
by
the
integration
of
molecular
rigidity,
central
chirality
MR
effect.
A
pair
green
denoted
as
(R)-BN-MeIAc
(S)-BN-MeIAc
designed.
Benefited
rigid
quasi-planar
MR-framework,
enantiomers
not
only
display
mirror-image
CPL
spectra,
but
also
exhibit
TADF
properties
high
photoluminescence
quantum
yield
96
%,
narrow
FWHM
30
nm,
horizontal
dipole
orientation
90
%
in
doped
film.
Consequently,
enantiomer-based
CP-OLEDs
achieved
excellent
external
efficiencies
37.2
very
low
efficiency
roll-off,
representing
highest
device
all
reported
CP-OLEDs.
Advanced Materials,
Год журнала:
2022,
Номер
34(32)
Опубликована: Июнь 21, 2022
Multiple
resonance
(MR)-effect-induced
thermally
activated
delayed
fluorescence
(TADF)
materials
have
garnered
significant
attention
because
they
can
achieve
both
high
color
purity
and
external
quantum
efficiency
(EQE).
However,
the
reported
green-emitting
MR-TADF
exhibit
broader
emission
compared
to
those
of
blue-emitting
ones
suffer
from
severe
roll-off
due
insufficient
rate
constants
reverse
intersystem
crossing
process
(kRISC
).
Herein,
a
pure
green
material
(ν-DABNA-CN-Me)
with
kRISC
105
s-1
is
reported.
The
key
success
introduction
cyano
groups
into
(ν-DABNA),
which
causes
remarkable
bathochromic
shift
without
loss
purity.
organic
light-emitting
diode
employing
it
as
an
emitter
exhibits
at
504
nm
small
full-width
half-maximum
23
nm,
corresponding
Commission
Internationale
d'Éclairage
coordinates
(0.13,
0.65).
device
achieves
maximum
EQE
31.9%
successfully
suppresses
luminance.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
145(3), С. 1505 - 1511
Опубликована: Дек. 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.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(47)
Опубликована: Сен. 28, 2022
Multiple
resonance
(MR)
type
thermally
activated
delayed
fluorescence
(TADF)
material
is
currently
a
research
hotspot
in
organic
light-emitting
diodes
(OLEDs)
due
to
their
high
color
purity
and
exciton
utilization.
However,
there
are
only
handful
of
MR-TADF
emitters
with
emissions
beyond
the
blue-to-green
region.
The
very
limited
emission
colors
for
mainly
caused
by
fact
that
so
far
molecular
modifications
do
not
offer
much
change
colors.
Here,
we
report
new
approach
modifying
prototypical
MR
core
DABNA
fusing
carbazoles
framework.
carbazole-fused
molecule
(TCZ-F-DABNA)
basically
maintains
MR-dominated
features
while
red-shifting
emission.
Its
OLED
achieves
an
external
quantum
efficiency
39.2
%
peak
at
588
nm,
which
record-high
OLEDs
peaks
560
nm.
This
work
provides
significantly
tunning
emitters.