ACS Applied Materials & Interfaces,
Journal Year:
2021,
Volume and Issue:
13(49), P. 58908 - 58915
Published: Dec. 3, 2021
Zero-dimensional
(0D)
organic
metal
halides
have
attracted
significant
attention
because
of
their
exceptional
structure
tunability
and
excellent
optical
characteristics.
However,
controllable
synthesis
a
desirable
configuration
halide
species
in
rational
way
remains
formidable
challenge,
how
the
unique
crystal
structures
affect
photophysical
properties
are
not
yet
well
understood.
Here,
reasonable
structural
modulation
strategy
is
proposed
to
realize
near-unity
photoluminescence
quantum
efficiency
(PLQE)
0D
antimony
halides.
By
carefully
controlling
reaction
conditions,
both
(C12H28N)2SbCl5
(C12H28N)SbCl4
with
different
configurations
can
be
prepared.
pyramid-shaped
[SbCl5]2-
exhibits
yellow
emission
PLQE
96.8%,
while
seesaw-shaped
[SbCl4]-
emissive
at
room
temperature.
Theoretical
calculations
indicate
that
these
two
crystals
attributed
symmetries
structures.
adopts
triclinic
P-1
symmetry,
possesses
monoclinic
P21/c
which
has
an
inversion
center,
thus
transitions
between
band-edge
states
give
minimal
dipole
intensity
similar
parity
character.
In
addition,
we
also
successfully
synthesized
nanocrystals
for
first
time,
particularly
appealing
solution
processibility
properties.
Furthermore,
flexible
composite
film
shows
bright
under
β-ray
excitation,
suggesting
strong
potential
detection.
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
33(5)
Published: Nov. 18, 2022
Abstract
Scintillators
with
high
light
yield,
low
detection
limit,
large
X‐ray
attenuation
efficiency
as
well
stable
and
nontoxic
compositions
are
of
great
importance
for
radiation
applications.
Here,
0D
(C
8
H
20
N)
2
Cu
Br
4
single
crystals
obtained
show
blue
emission
peaking
at
468
nm
a
near‐unity
photoluminescence
quantum
yield
99.7%,
Stokes
shift
148
(i.e.,
negligible
self‐absorption),
good
environmental
stability
along
strong
absorption
capability.
Moreover,
up
to
≈
91
300
photons/MeV
limit
52.1
nGy
air
s
−1
realized,
which
is
more
than
one
hundred
times
lower
the
dose
rate
5.5
µGy
required
medical
diagnostics.
ceramic
wafer
scintillation
screen
fabricated
by
cold
pressing
sintering
process,
clear
contrast
images
opaque
metal
box
electronic
component
spatial
resolution
9.54
lp
mm
realized.
This
study
not
only
designs
new
lead‐free
halide
scintillator,
but
also
develops
universal
strategy
preparation
large‐sized
scintillator
in
nondestructive
imaging.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(10)
Published: Jan. 10, 2022
Chiral
hybrid
organic-inorganic
metal
halides
(HOMHs)
with
intrinsic
noncentrosymmetry
have
shown
great
promise
for
applications
in
second-order
nonlinear
optics
(NLO).
However,
established
chiral
HOMHs
often
suffer
from
their
relatively
small
band
gaps,
which
lead
to
negative
impacts
on
transparent
window
and
laser-induced
damage
thresholds
(LDT).
Here,
we
synthesized
two
based
CuI
halides,
namely
(R-/S-MBA)CuBr2
,
feature
well-balanced
NLO
performances
a
highly
efficient
SHG
response,
outstanding
optical
transparency,
high
LDT.
The
effective
coefficient
of
(R-MBA)CuBr2
has
been
determined
be
≈24.7
pm
V-1
is
orders
magnitude
higher
than
that
CuII
counterparts.
This
work
shows
the
promising
potential
-based
photonic
wide
wavelength
regions.
Advanced Optical Materials,
Journal Year:
2022,
Volume and Issue:
10(12)
Published: April 21, 2022
Abstract
The
discovery
of
rare‐earth
free
luminescent
materials
with
blue‐light‐excitable
characteristic
is
great
importance
for
solid‐sate
lighting
applications.
Herein,
a
Cu(I)‐based
0D
hybrid
(
1,3‐dppH
2
)
Cu
4
I
8
∙H
O
synthesized
by
facile
solution
method,
and
it
shows
the
orange‐red
emission
peaking
at
625
nm
upon
460
excitation.
structure‐related
luminescence
mechanism
has
been
elaborated
experimental
theoretical
investigations.
Moreover,
intensity
remains
unchanged
even
after
continuous
water
treatment
60
days
due
to
improved
structural
stability
originating
from
intermolecular
π–π
interaction
between
organic
cations.
A
warm
white
light‐emitting
diode
(LED)
device
color
rendering
index
91.4%
fabricated
combining
440
LED
chip,
green‐emitting
Lu
3
Al
5
12
:Ce
3+
,
O.
This
work
provides
new
design
route
towards
cuprous
halide
will
initiate
more
exploration
their
intrinsic
mechanism.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(26)
Published: March 27, 2023
High-performance
X-ray
scintillators
with
low
detection
limits
and
high
light
yield
are
of
great
importance
a
challenge
for
low-dose
imaging
in
medical
diagnosis
industrial
detection.
In
this
work,
the
synthesis
new
2D
perovskite,
Cs2
CdBr2
Cl2
,
via
hydrothermal
reaction
is
reported.
By
doping
Mn2+
into
yellow
emission
located
at
593
nm
obtained,
photoluminescence
quantum
(PLQY)
:5%Mn2+
perovskite
reaches
highest
value
98.52%.
The
near-unity
PLQY
negligible
self-absorption
enable
excellent
scintillation
performance
64
950
photons
MeV-1
limit
17.82
nGyair
s-1
.
Moreover,
combining
poly(dimethylsiloxane)
to
fabricate
flexible
scintillator
screen
achieves
resolution
12.3
line
pairs
(lp)
mm-1
results
suggest
that
promising
candidate
high-resolution
imaging.
study
presents
approach
designing
high-performance
through
metal-ion
doping.
Chemical Science,
Journal Year:
2023,
Volume and Issue:
14(20), P. 5415 - 5424
Published: Jan. 1, 2023
Designing
and
synthesizing
cuprous
halide
phosphors
unifying
efficient
low-energy
emission
a
broad
excitation
band
is
still
great
challenge.
Herein,
by
rational
component
design,
three
novel
Cu(i)-based
metal
halides,
DPCu4X6
[DP
=
(C6H10N2)4(H2PO2)6;
X
Cl,
Br,
I],
were
synthesized
reacting
p-phenylenediamine
with
(CuX),
they
show
similar
structures,
consisting
of
isolated
[Cu4X6]2-
units
separated
organic
layers.
Photophysical
studies
uncover
that
the
highly
localized
excitons
rigid
environment
give
rise
to
yellow-orange
photoluminescence
in
all
compounds
spanning
from
240
450
nm.
The
bright
PL
(X
Br)
originates
self-trapped
due
strong
electron-phonon
coupling.
Intriguingly,
DPCu4I6
features
dual-band
emissive
characteristic,
attributed
synergistic
effect
halide/metal-to-ligand
charge-transfer
(X/MLCT)
triplet
cluster-centered
(3CC)
excited
states.
Benefiting
broadband
excitation,
high-performance
white-light
emitting
diode
(WLED)
high
color
rendering
index
85.1
was
achieved
using
single-component
phosphor.
This
work
not
only
unveils
role
halogens
photophysical
processes
but
also
provides
new
design
principles
for
WLEDs.
ACS Materials Letters,
Journal Year:
2024,
Volume and Issue:
6(4), P. 1542 - 1548
Published: March 19, 2024
Crystal-glass
phase
transformation
and
glass
recrystallization
in
zero-dimensional
(0D)
hybrid
metal
halides
make
them
thriving
X-ray
scintillators
with
the
advantages
of
large-area
fabrication
improved
performance.
Herein,
we
report
three
0D
copper(I)
composed
identical
organic
cations
versatile
self-assembly
copper-iodide
anions
find
that
volumes
inorganic
groups
are
related
to
their
lattice
energies,
which
conformationally
governed
thermodynamics
formation
through
destabilization.
A
subsequent
heating
counterparts
allows
bulk
glass-ceramic
via
recrystallization,
exhibiting
outstanding
scintillation
performances
(with
a
light
yield
64
000
ph
MeV–1
detection
limit
72.6
nGy
s–1)
high
stability
for
real-time
imaging
(spatial
resolution
above
20
lp
mm–1).
This
multiphase
strategy
luminescence
halide
opens
an
exploratory
way
structural
design
engineering
scintillator
screens
imaging.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
61(6)
Published: Nov. 16, 2021
As
low-dimensional
lead-free
hybrids
with
higher
stability
and
lower
toxicity
than
those
of
three-dimensional
lead
perovskites,
organic
antimony(III)
halides
show
great
application
potential
in
opt-electronic
field
owing
to
diverse
topologies
along
exceptional
optical
properties.
We
report
herein
an
hybrid
(MePPh3
)2
SbCl5
a
zero-dimensional
(0D)
structure,
which
exhibits
brilliant
orange
emission
peaked
at
593
nm
near-unity
photoluminescent
quantum
yield
(99.4
%).
The
characterization
photophysical
properties
demonstrates
that
the
broadband
microsecond
lifetime
(3.24
μs)
arises
from
self-trapped
(STE).
Electrically
driven
light-emitting
diodes
(OLEDs)
based
on
neat
doped
films
were
fabricated.
devices
significant
improvement
comparison
non-doped
OLEDs.
Owing
much
improved
surface
morphology
balanced
carrier
transport
layers
devices,
peak
luminance,
current
efficiency
(CE)
external
(EQE)
are
boosted
82
cd
m-2
3500
,
1.1
A-1
6.8
0.7
%
3.1
relative
respectively.
Advanced Optical Materials,
Journal Year:
2022,
Volume and Issue:
10(16)
Published: May 29, 2022
Abstract
Anti‐counterfeiting
has
become
a
serious
issue
around
the
global
world;
fluorescence‐based
tags
are
praised
for
low‐cost
and
facile
decryption
process.
However,
high‐level
anti‐counterfeiting
application
requires
incorporating
multifunctional
luminescent
materials
with
response
to
different
excitation
sources.
Herein,
dimeric
Cu(I)‐halide‐clusters‐assembled
single‐crystal
(AEP)
2
Cu
I
6
·2I·2H
O
(AEP
=
N
‐aminoethylpiperazinium)
concerning
high
down‐conversion
photoluminescence
quantum
yield
(PLQY)
value
of
near
unity
is
reported
(λ
ex
305
nm),
which
can
also
be
activated
by
near‐infrared
light
X‐ray.
The
ultrafast
spectroscopy
density
functional
theory
calculations
reveal
that
broad‐band
emission
originates
from
recombination
self‐trapped
excitons.
Remarkably,
PLQY
excellent
attenuation
capability
X‐ray
confers
an
outstanding
55
650
photons
MeV
−1
O,
5.25
times
higher
than
standard
bismuth
germaniumoxide
scintillator.
Such
multi‐light‐stimulus
endows
great
potential
in
anti‐counterfeiting,
solid‐state
lighting
devices,
digital
radiography.
Advanced Optical Materials,
Journal Year:
2022,
Volume and Issue:
10(20)
Published: July 15, 2022
Abstract
Metal
clusters
with
color‐tunable
radioluminescence
have
attracted
growing
attention
as
X‐ray
detection
materials.
However,
they
are
generally
less
scintillation‐efficient
due
to
the
coexistence
of
multiple
exciton
recombination
centers.
Herein,
two
new
zero‐dimensional
copper(I)‐based
(DIET)
3
Cu
X
(DIET
=
1,3‐Diethyl‐2‐thiourea,
Cl,
Br)
designed,
which
support
single
channel
photon
emission
(Cu
cluster
centered,
CC)
enhance
scintillation
performance.
Those
DIET
ligands
(L)
anchoring
copper(I)
ions
not
only
generate
direct
CuL
bonds,
but
also
form
a
disorder
[Cu
]
cluster,
results
in
intense
absorption.
Br
low
halogen
electronegativity
further
weakens
halogen‐to‐ligand
charge
transfer
(XLCT)
emission,
enabling
enhanced
quantum
efficiency
(≈69%)
and
performance
comparable
commercially
available
Lu
Al
5
O
12
:Ce.
Moreover,
flexible
thin
film
counterpart
demonstrates
legible
imaging
high
spatial
resolution
11.71
lp
mm
−1
.
This
study
provides
feasible
design
principle
discover
metal
cluster‐based
scintillators
expand
their
radiation
applications.