Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: April 10, 2023
As
promising
luminescent
materials
for
organic
light-emitting
diodes
(OLEDs),
thermally
activated
delayed
fluorescence
are
booming
vigorously
in
recent
years,
but
robust
blue
ones
still
remain
challenging.
Herein,
we
report
three
highly
efficient
and
deep-blue
comprised
of
a
weak
electron
acceptor
chromeno[3,2-c]carbazol-8(5H)-one
with
rigid
polycyclic
structure
donor
spiro[acridine-9,9'-xanthene].
They
hold
distinguished
merits
excellent
photoluminescence
quantum
yields
(99%),
ultrahigh
horizontal
transition
dipole
ratios
(93.6%),
fast
radiative
reverse
intersystem
crossing,
which
furnish
superb
electroluminescence
Commission
Internationale
de
I'Eclairage
coordinates
(CIEx,y)
(0.14,
0.18)
0.15)
record-beating
external
efficiencies
(ηexts)
43.4%
41.3%,
respectively.
Their
efficiency
roll-offs
successfully
reduced
by
suppressing
triplet-triplet
singlet-singlet
annihilations.
Moreover,
high-performance
green
hyperfluorescence
OLEDs
achieved
utilizing
these
as
sensitizers
multi-resonance
dopants,
providing
state-of-the-art
ηexts
32.5%
(CIEx,y
=
0.14,
0.10)
37.6%
0.32,
0.64),
respectively,
well
greatly
advanced
operational
lifetimes.
These
splendid
results
can
surely
inspire
the
development
devices.
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.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(29)
Published: May 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,
Journal Year:
2022,
Volume and Issue:
61(31)
Published: May 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,
Journal Year:
2022,
Volume and Issue:
61(24)
Published: April 1, 2022
Herein,
we
report
a
general
strategy
for
achieving
ultra-pure
green
emissions
by
suppressing
the
shoulder
peaks
in
emission
spectra
of
conventional
polycyclic
aromatic
hydrocarbons
(PAHs).
Through
precise
synthetic
fusion
multi-resonance
(MR)
fragments
with
PAH,
extended
π-conjugation
lengths,
increased
molecular
rigidity,
and
reduced
vibrational
frequency
could
be
simultaneously
realized.
The
proof-of-concept
emitters
exhibited
dominant
at
ca.
521
nm,
photoluminescence
quantum
yields
that
are
greater
than
99
%,
small
full-width-at-half-maximum
23
CIE
coordinates
(0.16,
0.77).
bottom-emitting
organic
light-emitting
diode
(OLED)
record-high
CIEy
value
0.74
high
maximum
external
efficiency
30.5
%.
top-emitting
OLED
not
only
achieved
BT.2020
color
(CIE:
0.17,
0.78)
first
time
but
also
showed
superior
performance
among
all
devices,
current
220
cd
A-
.
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.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(22), P. 12269 - 12273
Published: March 20, 2021
Abstract
Multiple‐resonance
(MR)
organic
emitters
bearing
small
full‐width
at
half‐maximum
(FWHMs)
are
of
general
interest
in
light‐emitting
diodes.
Indolo[3,2,1‐
jk
]carbazole
(ICz)
embedded
MR‐fluorophors
have
demonstrated
extremely
FWHMs,
yet
the
violet
region
with
low
electroluminescence
efficiency.
Herein,
a
strategic
implementation
ICz
subunits
into
MR
fluorophors
is
proposed
by
taking
advantage
synergetic
effect
para
‐positioned
nitrogen
atoms
to
enhance
electronic
coupling
decrease
emitting
energy
gap.
Deep
blue
peaking
441
and
447
nm
FWHMs
only
18
21
thereof
obtained,
respectively,
accompanied
≈90
%
photo‐luminance
quantum
yields.
With
assistance
thermally
activated
delayed
fluorescence
sensitizer
recycle
excitons,
corresponding
narrowband
electroluminescent
devices
show
unprecedent
high
maximum
external
efficiencies
32.0
34.7
CIE
y
0.10
0.085,
respectively.
Advanced Science,
Journal Year:
2021,
Volume and Issue:
8(16)
Published: June 16, 2021
Although
the
organic
light-emitting
diode
(OLED)
has
been
successfully
commercialized,
development
of
deep-blue
OLEDs
with
high
efficiency
and
long
lifetime
remains
a
challenge.
Here,
novel
hyperfluorescent
OLED
that
incorporates
Pt(II)
complex
(PtON7-dtb)
as
phosphorescent
sensitizer
hydrocarbon-based
multiple
resonance-based
fluorophore
an
emitter
(TBPDP
ν-DABNA)
in
device
emissive
layer
(EML),
is
proposed.
Such
EML
system
can
promote
efficient
energy
transfer
from
triplet
excited
states
to
singlet
fluorophore,
thus
significantly
improving
device.
As
result,
using
(ν-DABNA)
Commission
Internationale
de
L'Eclairage
chromaticity
coordinate
y
below
0.1
demonstrated,
which
attains
narrow
full
width
at
half
maximum
≈17
nm,
fourfold
increased
current
48.9
cd
A-1
,
19-fold
improved
half-lifetime
253.8
h
1000
m-2
compared
conventional
OLED.
The
findings
lead
better
understanding
performance.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(23)
Published: March 18, 2022
Abstract
Herein,
a
ternary
boron‐oxygen‐nitrogen
embedded
polycyclic
aromatic
hydrocarbon
with
multiple
resonance
thermally
activated
delayed
fluorescence
(MR‐TADF),
namely
DBNO,
is
developed
by
adopting
the
para
boron‐π‐boron
and
oxygen‐π‐oxygen
strategy.
The
designed
molecule
presents
vivid
green
emission
high
photoluminescence
quantum
yield
(96
%)
an
extremely
narrow
full
width
at
half
maximum
(FWHM)
of
19
nm/0.09
eV,
which
surpasses
all
previously
reported
TADF
emitters
to
date.
In
addition,
long
molecular
structure
along
transition
dipole
moment
direction
endows
it
horizontal
emitting
ratio
96
%.
organic
light‐emitting
diode
(OLED)
based
on
DBNO
reveals
narrowband
peak
504
nm
FWHM
24
nm/0.12
eV.
Particularly,
significantly
improved
device
performance
achieved
TADF‐sensitization
(hyperfluorescence)
mechanism,
presenting
27
external
efficiency
(EQE)
37.1