Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(47), С. 32816 - 32825
Опубликована: Ноя. 12, 2024
Solar-driven
conversion
of
CH4
into
value-added
methyl
chlorides
and
H2
with
abundant
chloride
ions
offers
a
sustainable
reforming
strategy
but
suffers
from
inefficient
Cl–
activation
severe
e––h+
recombination
in
traditional
photocatalysts.
Herein,
we
demonstrate
that
BiOCl
moiré
superlattices
11.1°
twist
angle
are
highly
efficient
for
photocatalytic
CH3Cl
NaCl.
These
superlattices,
featuring
misalignment-induced
tensile
strains,
destabilize
surface
Bi–Cl
bonds,
facilitating
hole-mediated
MvK-analogous
process
to
activate
lattice
Cl
reactive
•Cl
chlorination.
Meanwhile,
their
twisted
stacking
configurations
reinforce
interlayer
electronic
coupling
thus
accelerate
out-of-plane
carrier
transfer.
Along
anchoring
single-atom
Pt
sites
evolution,
the
resulting
Pt1/BiOCl
deliver
yield
53.4
μmol
g–1
h–1
an
impressive
selectivity
96%
under
visible
light.
This
study
highlights
potential
engineering
two-dimensional
photocatalysts
regulate
structural
strains
dynamics
decentralized
CH4.
Nanotechnology,
Год журнала:
2025,
Номер
36(18), С. 185202 - 185202
Опубликована: Март 28, 2025
Abstract
The
optical
response
manipulation
of
two-dimensional
materials
is
crucial
for
designing
and
optimizing
high-performance
optoelectronic
devices.
Previously,
modulation
in
semiconductors
primarily
relied
on
adjusting
carrier
density
through
excitation
or
charge
injection
using
the
energy
band-filling
effect.
Recently,
twist
angle
has
been
found
to
tune
properties
van
der
Waals
structure,
but
its
impact
transient
remains
unexplored.
Herein,
we
demonstrate
that
can
effectively
regulate
behaviors
by
tracing
evolution
responses
twisted
bilayer
WS
2
from
0°
60°.
Both
Raman
PL
spectra
consistently
show
bilayers
are
highly
dependent
angle.
Exciton
behavior
phonon
modes
exhibit
similarity
at
angles
near
60°,
significantly
change
as
approaches
30°.
Moreover,
was
carefully
investigated
a
femtosecond
pump-probe
technique.
results
reveal
significant
decrease
thermalization/relaxation
time
exciton
formation/recombination
with
∼31.0°,
compared
∼2.9°
∼58.9°,
which
be
attributed
accumulation
intralayer
carriers
due
weakened
interlayer
coupling.
These
modulate
2D
materials.
Our
study
elucidates
dynamic
provides
new
insights
future
photonic
The Journal of Physical Chemistry Letters,
Год журнала:
2025,
Номер
unknown, С. 5272 - 5280
Опубликована: Май 19, 2025
The
moiré
potential
in
van
der
Waals
(vdW)
superlattices
is
well-established
to
significantly
influence
electronic
structures
and
optical
excitations.
When
Janus
monolayers
are
employed
construct
twisted
bilayers,
an
additional
degree
of
freedom─the
out-of-plane
field─is
introduced
alongside
the
potential,
leading
modifications
both
properties.
While
these
two
effects
have
been
individually
investigated
prior
studies
on
excitons,
behavior
excitons
under
simultaneous
presence
remained
unexplored.
In
this
study,
we
investigate,
for
first
time,
interplay
between
In2SSe.
Our
results
demonstrate
that
band
excitonic
properties
can
be
modulated
through
variations
stacking
sequences
intrinsic
dipole
orientations.
This
work
provides
a
framework
precise
control
emission
energy,
exciton
characteristics,
spatial
distribution
excitons.
We
predict
coexistence
field-induced
interlayer
potential-driven
bilayer
These
findings
not
only
elucidate
interaction
fields
potentials
but
also
introduce
novel,
multifaceted
strategy
manipulation.
The Journal of Physical Chemistry Letters,
Год журнала:
2023,
Номер
14(47), С. 10685 - 10692
Опубликована: Ноя. 21, 2023
Perovskite
solar
cells
have
witnessed
a
surge
in
interest
as
promising
technology
for
low-cost,
high-efficiency
photovoltaics
with
certified
power
conversion
efficiencies
beyond
25%.
However,
their
commercial
development
is
hindered
by
poor
stability
and
nonradiative
losses
that
restrict
approach
to
the
theoretical
efficiency
limit.
Using
ab
initio
nonadiabatic
molecular
dynamics,
we
demonstrate
charge
recombination
suppressed
when
iodide
formamidinium
lead
(FAPbI3)
partially
replaced
pseudohalide
anions
(SCN-,
BF4-,
PF6-).
The
replacement
breaks
symmetry
of
system
creates
local
structural
distortion
dynamic
disorder,
decreasing
electron-hole
overlap
electron-vibrational
coupling.
carrier
lifetime
found
increase
increased
longest
PF6-.
This
work
fundamentally
relevant
design
high-performance
perovskite
materials
optoelectronic
applications.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(2), С. 2902 - 2911
Опубликована: Янв. 3, 2024
Monolayer
transition
metal
dichalcogenides
have
strong
intracovalent
bonding.
When
stacked
in
multilayers,
however,
weak
van
der
Waals
interactions
dominate
interlayer
mechanical
coupling
and,
thus,
influence
their
lattice
vibrations.
This
study
presents
the
frequency
evolution
of
phonons
twisted
WS2
bilayers,
highly
subject
to
twist
angle.
The
angle
between
layers
is
controlled
modulate
spacing
layers,
which,
turn,
affects
that
probed
by
Raman
spectroscopy.
shifts
high-frequency
E2g1
(Γ)
and
A1g
phonon
modes
separations
are
dependent
on
angle,
reflecting
correlation
In
this
work,
we
fabricated
large-area,
bilayer
with
a
clean
interface
angles.
Polarized
spectroscopy
identified
new
modes,
which
were
not
previously
reported,
depending
appearance
breathing
spectra
provides
evidence
structures.
We
confirm
can
alter
exciton
trion
dynamics
bilayers
as
indicated
photoluminescence
peak
shift.
These
large-area
samples
practical
applications
optoelectronic
device
fabrication
twistronics.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(47), С. 32816 - 32825
Опубликована: Ноя. 12, 2024
Solar-driven
conversion
of
CH4
into
value-added
methyl
chlorides
and
H2
with
abundant
chloride
ions
offers
a
sustainable
reforming
strategy
but
suffers
from
inefficient
Cl–
activation
severe
e––h+
recombination
in
traditional
photocatalysts.
Herein,
we
demonstrate
that
BiOCl
moiré
superlattices
11.1°
twist
angle
are
highly
efficient
for
photocatalytic
CH3Cl
NaCl.
These
superlattices,
featuring
misalignment-induced
tensile
strains,
destabilize
surface
Bi–Cl
bonds,
facilitating
hole-mediated
MvK-analogous
process
to
activate
lattice
Cl
reactive
•Cl
chlorination.
Meanwhile,
their
twisted
stacking
configurations
reinforce
interlayer
electronic
coupling
thus
accelerate
out-of-plane
carrier
transfer.
Along
anchoring
single-atom
Pt
sites
evolution,
the
resulting
Pt1/BiOCl
deliver
yield
53.4
μmol
g–1
h–1
an
impressive
selectivity
96%
under
visible
light.
This
study
highlights
potential
engineering
two-dimensional
photocatalysts
regulate
structural
strains
dynamics
decentralized
CH4.