Abstract
Thermally
activated
delayed
fluorescence
(TADF)
materials
with
extremely
small
singlet‐triplet
energy
offsets
have
opened
new
horizons
for
the
development
of
metal‐free
photosensitizers
photodynamic
therapy
(PDT)
in
recent
years.
However,
exploration
near‐infrared
(NIR)
TADF
emitters
efficient
two‐photon‐excited
(TPE)
PDT
is
still
a
formidable
challenge,
thus
it
has
not
been
reported
yet.
In
this
study,
purely
organic
(PSs)
based
on
nanoparticles
(NIR‐TADF
NPs)
are
designed
TPE‐PDT,
which
show
excellent
singlet
oxygen
generation
ability.
Thanks
to
intrinsic
two‐photon
excitation
and
NIR
emission
characteristics,
NIR‐TADF
NPs
demonstrate
promising
potential
both
single‐photon‐excited
(SPE)
TPE
imaging.
More
importantly,
anti‐tumor
efficiency
biosafety
TADF‐based
PSs
at
animal
level
confirmed
A549
tumor
xenograft
models
under
laser
irradiance,
will
facilitate
practical
biomedical
applications
materials.
This
work
only
provides
strategy
develop
PSs,
but
also
expands
applied
scope
nanotherapeutics
advances
their
possible
clinical
translation
cancer
therapy.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(14)
Опубликована: Фев. 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,
Год журнала:
2022,
Номер
61(23)
Опубликована: Март 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
SmartMat,
Год журнала:
2021,
Номер
2(3), С. 326 - 346
Опубликована: Авг. 27, 2021
Abstract
Red
and
near‐infrared
(NIR)
organic
light‐emitting
diodes
(OLED)
have
gained
remarkable
interest
due
to
their
numerous
applications.
However,
the
construction
of
highly
emissive
emitters
is
hampered
by
energy‐gap
law
aggregation‐caused
quenching
(ACQ)
effect.
Whereas,
aggregation‐induced
emission
(AIE)
materials
could
avoid
undesirable
ACQ
effect
emit
bright
light
in
aggregated
state,
which
one
class
most
promising
fabricate
high‐performance
OLED
with
a
high
external
quantum
efficiency
low
roll‐off.
This
review
summarizes
recent
advances
red
NIR
AIE
property,
including
traditional
fluorescence,
thermally
activated
delayed
hybridized
local
charge
transfer
compounds.
Meanwhile,
emphasis
attention
paid
molecular
design
principles,
as
well
structure‐photophysical
characteristics.
We
also
briefly
further
outlook
challenges
perspective
luminogens.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(41)
Опубликована: Авг. 19, 2022
Herein,
we
report
two
multiple-resonance
thermally
activated
delayed
fluorescence
emitters
(VTCzBN
and
TCz-VTCzBN)
based
on
indolo[3,2,1-jk]carbazole
unit
boron-nitrogen
skeletons,
whose
emissions
peaking
at
496
521
nm
with
full
width
half
maximum
of
34
29
nm,
respectively.
Meanwhile,
fast
rate
constants
reverse
intersystem
crossing
above
106
s-1
are
obtained
due
to
small
singlet-triplet
energy
gaps
large
spin-orbital
coupling
values.
Notably,
planar
molecular
structures
along
the
transition
dipole
moment
direction
endow
them
high
horizontal
emitting
ratios
up
94
%.
Consequently,
corresponding
organic
light-emitting
diodes
(OLEDs)
show
external
quantum
efficiencies
31.7
%
32.2
%,
Particularly,
OLED
TCz-VTCzBN
display
ultra-pure
green
emission
Commission
Internationale
de
l'Eclairage
coordinates
(0.22,
0.71),
consistent
standard
National
Television
System
Committee.
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(36)
Опубликована: Июль 15, 2022
The
realization
of
luminescent
materials
with
narrowband
and
circularly
polarized
luminescence
(CPL)
is
great
significance
for
the
development
future
optical
photonic
devices.
Herein,
through
a
steric-hindrance-assisted
dual-core
strategy,
two
pairs
chiral
multiple
resonance
thermally
activated
delayed
fluorescence
(MR-TADF)
(R/S-DOBN
R/S-DOBNT)
are
directly
constructed
by
bonding
organoboron
MR-TADF
monocores
(SOBN
SOBNT)
carbazole/3,6-di-tert-butyl-9H-carbazole
phenol
derivative
as
donors,
realizing
obvious
CPL
emissions.
Furthermore,
effect
in
prepared
R/S-DOBN
R/S-DOBNT
increases
transition
oscillator
strength
times
more
than
that
monocore
structure,
while
maintaining
ultrapure
blue
emissions
peaking
at
453
459
nm
narrower
full-width
half-maximum
21
reorganization
energy
reduction.
organic
light-emitting
diodes
based
on
enantiomers
exhibit
emission
Commission
Internationale
de
L'Eclairage
(CIE)
coordinates
(0.14,
0.10)
(0.13,
0.12),
high
maximum
external
quantum
efficiencies
23.9%
25.6%,
electroluminescence
dissymmetry
factors
(|gEL
|)
≈
10-3
.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(7)
Опубликована: Дек. 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,
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.
Abstract
During
the
last
few
years,
organoboron‐based
thermally
activated
delayed
fluorescence
(TADF)
materials
have
received
extensive
attention
in
optoelectronic
area,
owing
to
unique
electronegativity
of
boron
atom.
Herein,
many
research
progress
TADF
for
organic
devices
is
summarized.
This
review
comprehensively
documents
according
emission
colors
from
blue
red‐near‐infrared
(red‐NIR),
covering
molecular
design
strategies,
photophysical
properties,
and
performance
light‐emitting
diodes
(OLEDs).
The
current
future
challenges
this
fast‐growing
fields
are
reviewed
systematically,
providing
instructive
guidance
on
high‐performance
TADF‐OLEDs.