Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(27), P. 12247 - 12260
Published: June 29, 2022
The
electron-phonon
(e-ph)
interaction
in
lead
halide
perovskites
(LHPs)
plays
a
role
variety
of
physical
phenomena.
Unveiling
how
the
local
lattice
distortion
responds
to
charge
carriers
is
critical
step
toward
understanding
e-ph
LHPs.
Herein,
we
advance
fundamental
LHPs
from
perspective
stereochemical
activity
6s2
lone-pair
electrons
on
Pb2+
cation.
We
demonstrate
model
system
based
three
with
distinctive
activities
for
studying
structure-property
relationships.
By
tuning
A-cation
chemistry,
synthesized
single-crystal
CsPbBr3,
(MA0.13EA0.87)PbBr3
(MA+
=
methylammonium;
EA+
ethylammonium),
and
(MHy)PbBr3
(MHy+
methylhydrazinium),
which
exhibit
stereo-inactive,
dynamic
stereo-active,
static
stereo-active
lone
pairs,
respectively.
This
gives
rise
distortions
low-frequency
vibrational
modes.
find
that
leads
blue
shift
band
gap
as
temperature
increases
structure
pair
but
red
pair.
Furthermore,
analyses
temperature-dependent
low-energy
photoluminescence
tails
reveal
strength
increasing
activity,
leading
transition
large
polaron
small
polaron,
has
significant
influence
emission
spectra
carrier
dynamics.
Our
results
highlight
controlling
gap,
phonon,
polaronic
effect
provide
guidelines
optimizing
optoelectronic
properties,
especially
tin-based
germanium-based
perovskites,
where
pairs
are
more
prominent
than
their
counterparts.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(4), P. 2626 - 2662
Published: Jan. 1, 2021
This
review
provides
in-depth
insight
into
the
structure–luminescence–application
relationship
of
0D
all-inorganic/organic–inorganic
hybrid
metal
halide
luminescent
materials.
Advanced Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(40)
Published: July 10, 2021
Abstract
Luminescent
metal
halide
materials
with
flexible
crystallography/electronic
structures
and
tunable
emission
have
demonstrated
broad
application
prospects
in
the
visible
light
region.
However,
designing
near‐infrared
(NIR)
light‐emitting
halides
remains
a
challenge.
Here,
an
enlightening
prototype
is
proposed
to
explore
high‐efficiency
broadband
NIR
systems
by
incorporating
Sb
3+
into
Cs
2
ZnCl
4
matrix.
Combined
experimental
analysis
density
functional
theory
calculations
reveal
modified
self‐trapped
excitons
model
elaborate
emission.
The
high
photoluminescence
quantum
yield
of
69.9%
peaking
at
745
nm
large
full
width
half
maximum
175
nm,
along
excellent
air/thermal
stability,
show
unique
advantages
lead‐free
:Sb
as
source.
substitution
Cl
−
Br
further
enables
red‐shift
peak
from
823
nm.
diode
device
based
on
demonstrates
potential
non‐visible
source
night
vision.
This
study
puts
forward
effective
strategy
design
novel
eco‐friendly
emissive
provides
guidance
for
expanding
scope
luminescent
halides.
Chemistry of Materials,
Journal Year:
2020,
Volume and Issue:
32(24), P. 10255 - 10267
Published: Dec. 3, 2020
Bi3+
and
Sb3+
doping
(and
codoping
with
lanthanides)
in
Cs2SnCl6
vacancy
ordered
perovskites
Cs2MInCl6
(M
=
Na,
K,
Ag)
double
has
been
shown
to
open
up
new
opportunities
for
solid
state
lighting.
ns2
outer
electronic
configuration
can
tailor
both
optical
absorption
emission
properties
phosphor-converted
light
emitting
diode
(pc-LEDs)
applications.
Therefore,
the
s-electron
dopants
(Bi3+
Sb3+)
act
as
sensitizers
emitters.
This
is
because
dopant
s-electrons
contribute
near
band
edges
of
host,
unlike
cases
d-
f-electron
dopants.
Consequently,
also
a
sensitizer
lanthanide
luminescence
systems
like
Bi3+-Ln3+
codoped
Cs2AgInCl6,
where
Ln
Er,
Yb,
Tb.
In
this
perspective,
we
provide
insights
on
tailoring
by
electron
doping.
These
are
then
connected
rational
design
hosts,
dopants,
codopants,
their
potential
Finally,
discuss
challenges
future
research.
Advanced Optical Materials,
Journal Year:
2021,
Volume and Issue:
9(8)
Published: Feb. 18, 2021
Abstract
Emerging
lead‐free
metal
halides
with
low
toxicity
and
unparalleled
optoelectronic
properties
have
attracted
growing
research
interests,
also
demonstrating
extensive
application
potentials.
Among
these,
Sb
3+
‐based
all‐inorganic/organic–inorganic
hybrid
become
a
vital
group
due
to
the
special
energy
level
distribution
along
diverse
optical
properties.
However,
there
remains
gap
in
understanding
relationship
between
crystal
structure
radiation
process
of
involved
emission.
Herein,
existing
reports
about
luminescent
are
revisited
their
structure–luminescence–application
is
explored,
it
further
established
that
triplet
self‐trapped
excitons
(STEs)
emission
varies
different
crystallographic
environments
endows
tunable
performance.
This
work
aims
provide
constructive
strategies
exploitation
halides,
guides
structural
design
photoluminescence
tuning
doped
halide
materials.
Advanced Optical Materials,
Journal Year:
2021,
Volume and Issue:
9(17)
Published: May 31, 2021
Abstract
The
high‐profile
candidacy
of
low‐dimensional
metal‐halide
single
crystals
as
promising
light
emitters
originates
from
the
intriguing
emission
properties
(e.g.,
extremely
broad
luminescence
spectra,
large
Stokes
shift,
high
color
rendition),
which
have
enabled
recent
great
achievements
on
their
application
in
lighting,
artificial
illumination,
and
scintillators.
Among
family
crystals,
zero‐dimensional
(0D)
materials
been
featured
lowest
dimensionality,
a
consequence,
strongest
quantum
confinement,
softest
lattice,
electron–phonon
coupling
further
translated
into
near‐unity
photoluminescence
(PL)
efficiency
with
broadband
emission.
However,
far
it
is
known,
0D
structures
are
significantly
underexplored.
Herein,
an
overview
provided
advances
focus
comprehensive
understanding
insightful
perspectives
behind
photophysical
mechanism.
Additionally,
challenges
future
opportunities
currently
faced
by
bulk
metal
halides
discussed
order
to
provide
roadmap
for
development
novel
versatile
optical
suited
practical
applications.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(19)
Published: March 18, 2023
Abstract
The
excited‐state
tuning
of
luminescent
metal–organic
compounds
has
made
great
progress
in
the
fields
optical
imaging,
photocatalysis,
photodynamic
therapy,
light‐emitting
devices,
sensors,
and
so
on.
Although
with
high
luminescence
efficiency
can
be
realized
via
enhanced
molecular
rigidity
heavy‐atom
effect,
their
corresponding
lifetimes
are
still
limited
on
order
a
nanosecond
to
millisecond,
owing
inherent
competition
between
luminous
lifetime.
Therefore,
advanced
applications
(i.e.,
persistent
afterglow
information
security,
anti‐counterfeiting,
smart
materials,
among
others)
related
long
(LPL,
typically
lifetime
larger
than
millisecond)
seriously
hindered.
This
review
gives
timely
systematic
summary
for
realizing
room‐temperature
phosphorescence
(RTP)‐type
thermally
activated
delayed
fluorescence
(TADF)‐type
LPL
during
last
few
years.
Particularly,
based
perspectives
time,
space,
energy
dimensions,
fundamental
materials
design
coordination
assembly
systematically
described
first
time.
Moreover,
internal
external
factors
influencing
properties
terms
efficiency,
lifetime,
color
illustrated.
Last
but
not
least,
challenges
also
discussed
developing
from
compounds.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(18)
Published: March 2, 2022
0D
hybrid
metal
halides
(0D
HMHs)
are
considered
to
be
promising
luminescent
emitters.
HMHs
commonly
exhibit
self-trapped
exciton
(STE)
emissions
originating
from
the
inorganic
halide
anion
units.
Exploring
and
utilizing
emission
features
of
organic
cation
units
in
is
highly
desired
enrich
their
optical
properties
as
multifunctional
materials.
Here,
tunable
successfully
achieved
triphenylsulfonium
(Ph3
S+
)-based
HMHs.
Notably,
integrated
afterglow
STE
with
adjustable
intensities
obtained
S)2
Sn1-x
Tex
Cl6
(x
=
0-1)
via
delicate
combination
[SnCl6
]2-
[TeCl6
.
Moreover,
such
a
strategy
can
readily
extended
develop
other
HMH
materials
intriguing
properties.
As
demonstration,
Zn1-x
Mnx
Cl4
constructed
achieve
Mn2+
d-d
high
efficiency.
Consequently,
these
novel
colorful
applied
multiple
anti-counterfeiting
applications.
ACS Energy Letters,
Journal Year:
2021,
Volume and Issue:
6(6), P. 2283 - 2292
Published: May 27, 2021
We
synthesize
colloidal
nanocrystals
(NCs)
of
Rb3InCl6,
composed
isolated
metal
halide
octahedra
("0D"),
and
Cs2NaInCl6
Cs2KInCl6
double
perovskites,
where
all
share
corners
are
interconnected
("3D"),
with
the
aim
to
elucidate
compare
their
optical
features
once
doped
Sb3+
ions.
Our
computational
analyses
evidence
that
photoluminescence
quantum
yield
(PLQY)
these
systems
is
consistently
lower
than
corresponding
bulk
materials
due
presence
deep
surface
traps
from
under-coordinated
Also,
Sb-doped
"0D"
Rb3InCl6
NCs
exhibit
a
higher
PLQY
"3D"
NCs,
most
likely
because
excitons
responsible
for
PL
emission
migrate
faster
in
3D
0D
NCs.
also
observe
feature
large
Stokes
shift
(varying
system
system),
should
be
interest
applications
photon
management
scintillation
technologies.
Scintillation
properties
evaluated
via
radioluminescence
experiments,
re-absorption-free
waveguiding
performance
large-area
plastic
scintillators
assessed
using
Monte
Carlo
ray-tracing
simulations.