Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(41), С. 22826 - 22835
Опубликована: Окт. 5, 2023
A
twist
angle
at
a
van
der
Waals
junction
provides
handle
to
tune
its
optoelectronic
properties
for
variety
of
applications,
and
comprehensive
understanding
how
the
modulates
electronic
structure,
interlayer
coupling,
carrier
dynamics
is
needed.
We
employ
time-dependent
density
functional
theory
nonadiabatic
molecular
elucidate
angle-dependent
intervalley
transfer
recombination
in
bilayer
WS2.
Repulsion
between
S
atoms
twisted
configurations
weakens
increases
distance,
softens
layer
breathing
modes.
Twisting
has
minor
influence
on
K
valleys
while
it
lowers
Γ
raises
Q
because
their
wave
functions
are
delocalized
layers.
Consequently,
reduced
energy
gaps
accelerate
hole
structures.
Intervalley
electron
proceeds
nearly
an
order
magnitude
faster
than
transfer.
The
more
localized
values
larger
bandgaps
result
smaller
couplings
recombination,
making
3-4
times
slower
high-symmetry
B2g
breathing,
E2g
in-plane,
A1g
out-of-plane
modes
most
active
during
recombination.
extended
lifetimes
junctions
favorable
device
performance.
Light Science & Applications,
Год журнала:
2021,
Номер
10(1)
Опубликована: Апрель 2, 2021
Abstract
Van
der
Waals
(vdW)
heterostructures
based
on
transition
metal
dichalcogenides
(TMDs)
generally
possess
a
type-II
band
alignment
that
facilitates
the
formation
of
interlayer
excitons
between
constituent
monolayers.
Manipulation
in
TMD
vdW
holds
great
promise
for
development
excitonic
integrated
circuits
serve
as
counterpart
electronic
circuits,
which
allows
photons
and
to
transform
into
each
other
thus
bridges
optical
communication
signal
processing
at
circuit.
As
consequence,
numerous
studies
have
been
carried
out
obtain
deep
insight
physical
properties
excitons,
including
revealing
their
ultrafast
formation,
long
population
recombination
lifetimes,
intriguing
spin-valley
dynamics.
These
outstanding
ensure
with
good
transport
characteristics,
may
pave
way
potential
applications
efficient
devices
heterostructures.
At
present,
systematic
comprehensive
overview
exciton
relaxation,
transport,
is
still
lacking.
In
this
review,
we
give
description
discussion
these
frontier
topics
provide
valuable
guidance
researchers
field.
Wiley Interdisciplinary Reviews Computational Molecular Science,
Год журнала:
2019,
Номер
9(6)
Опубликована: Март 14, 2019
The
ultrafast
dynamics
of
photoexcited
charge
carriers
in
condensed
matter
systems
play
an
important
role
optoelectronics
and
solar
energy
conversion.
Yet
it
is
challenging
to
understand
such
multidimensional
at
the
atomic
scale.
Combining
real‐time
time‐dependent
density
functional
theory
with
fewest‐switches
surface
hopping
scheme,
we
develop
ab
initio
nonadiabatic
molecular
(NAMD)
code
Hefei‐NAMD
simulate
excited
carrier
systems.
Using
this
method,
have
investigated
interfacial
transfer
dynamics,
electron–hole
recombination
spin‐polarized
hole
different
are
studied
energy,
real
momentum
spaces.
In
addition,
coupling
phonons,
defects
adsorptions
investigated.
state‐of‐art
NAMD
studies
provide
unique
insights
This
article
categorized
under:
Structure
Mechanism
>
Computational
Materials
Science
Molecular
Statistical
Mechanics
Dynamics
Monte‐Carlo
Methods
Electronic
Theory
Ab
Initio
Software
Simulation
Low-cost
solution-based
synthesis
of
metal
halide
perovskites
(MHPs)
invariably
introduces
defects
in
the
system,
which
could
form
Shockley-Read-Hall
(SRH)
electron-hole
recombination
centers
detrimental
to
solar
conversion
efficiency.
Here,
we
investigate
nonradiative
processes
due
native
point
methylammonium
lead
(MAPbI3)
using
ab
initio
nonadiabatic
molecular
dynamics
within
surface-hopping
framework.
Regardless
whether
introduce
a
shallow
or
deep
band
state,
find
that
charge
MAPbI3
is
not
enhanced,
contrary
predictions
from
SRH
theory.
We
demonstrate
this
strong
tolerance
against
defects,
and
hence
breakdown
SRH,
arises
because
photogenerated
carriers
are
only
coupled
with
low-frequency
phonons
electron
hole
states
overlap
weakly.
Both
factors
appreciably
decrease
coupling.
argue
soft
nature
inorganic
lattice
small
bulk
modulus
key
for
defect
tolerance,
hence,
findings
general
other
MHPs.
Advanced Materials,
Год журнала:
2018,
Номер
30(39)
Опубликована: Июль 23, 2018
Abstract
2D
materials
and
heterostructures
have
attracted
significant
attention
for
a
variety
of
nanoelectronic
optoelectronic
applications.
At
the
atomically
thin
limit,
material
characteristics
functionalities
are
dominated
by
surface
chemistry
interface
coupling.
Therefore,
methods
comprehensively
characterizing
precisely
controlling
surfaces
interfaces
required
to
realize
full
technological
potential
materials.
Here,
properties
that
govern
performance
introduced.
Then
experimental
approaches
resolve
phenomena
down
atomic
scale,
as
well
strategies
allow
tuning
optimization
interfacial
interactions
in
van
der
Waals
heterostructures,
systematically
reviewed.
Finally,
future
outlook
delineates
remaining
challenges
opportunities
characterization
control
is
presented.
Applied Physics Reviews,
Год журнала:
2020,
Номер
7(3)
Опубликована: Сен. 1, 2020
Quantum
technology
has
grown
out
of
quantum
information
theory
and
now
provides
a
valuable
tool
that
researchers
from
numerous
fields
can
add
to
their
toolbox
research
methods.
To
date,
various
systems
have
been
exploited
promote
the
application
processing.
The
be
used
for
include
superconducting
circuits,
ultracold
atoms,
trapped
ions,
semiconductor
dots,
solid-state
spins
emitters.
In
this
review,
we
will
discuss
state-of-the-art
material
platforms
spin-based
technology,
with
focus
on
progress
in
emitters
several
leading
host
materials,
including
diamond,
silicon
carbide,
boron
nitride,
silicon,
two-dimensional
semiconductors,
other
materials.
We
highlight
how
first-principles
calculations
serve
as
an
exceptionally
robust
finding
novel
defect
qubits
single-photon
solids,
through
detailed
predictions
electronic,
magnetic,
optical
properties.
ACS Catalysis,
Год журнала:
2020,
Номер
10(3), С. 1976 - 1983
Опубликована: Янв. 8, 2020
Direct
Z-scheme
heterostructure
photocatalysts
possess
tremendous
potential
to
solar-driven
overall
water
splitting,
but
how
rationally
design
and
comprehensively
characterize
high-efficient
direct
heterostructures
remains
a
great
challenge.
Herein,
we
report
the
of
metal-free
C3B/C3N
through
constructing
p-n
heterojunction
as
photocatalyst
for
splitting
by
combining
first-principles
excited
state
dynamics
simulations.
Our
calculations
show
that
strong
interlayer
interaction
in
provides
large
built-in
electric
field
with
about
0.4
V/Å
interface
nonadiabatic
coupling
which
significantly
accelerates
recombination
carriers
weak
redox
capacity
(∼0.5
ps)
retards
lifetime
(∼4
ps).
Meanwhile,
B
atoms,
serving
Lewis
acid
sites,
are
good
catalytic
centers
trap
molecules.
The
hydrogen
reduction
reaction
complex
four-electronic
oxidation
can
happen
smoothly
on
C3B
C3N
surface,
respectively,
without
additional
overpotential
cocatalyst.
This
work
not
only
also
paves
way
rational
high-performance
photocatalysts.
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(4), С. 1215 - 1272
Опубликована: Янв. 1, 2023
Together
with
the
development
of
two-dimensional
(2D)
materials,
transition
metal
dichalcogenides
(TMDs)
have
become
one
most
popular
series
model
materials
for
fundamental
sciences
and
practical
applications.
Due
to
ever-growing
requirements
customization
multi-function,
dozens
modulated
structures
been
introduced
in
TMDs.
In
this
review,
we
present
a
systematic
comprehensive
overview
structure
modulation
TMDs,
including
point,
linear
out-of-plane
structures,
following
updating
conventional
classification
silicon
related
bulk
semiconductors.
particular,
focus
on
structural
characteristics
TMD
analyse
corresponding
root
causes.
We
also
summarize
recent
progress
modulating
methods,
mechanisms,
properties
applications
based
structures.
Finally,
demonstrate
challenges
prospects
TMDs
forecast
potential
directions
about
what
how
breakthroughs
can
be
achieved.
