Machine learning accelerated nonadiabatic dynamics simulations of materials with excitonic effects
The Journal of Chemical Physics,
Год журнала:
2025,
Номер
162(2)
Опубликована: Янв. 8, 2025
This
study
presents
an
efficient
methodology
for
simulating
nonadiabatic
dynamics
of
complex
materials
with
excitonic
effects
by
integrating
machine
learning
(ML)
models
simplified
Tamm–Dancoff
approximation
(sTDA)
calculations.
By
leveraging
ML
models,
we
accurately
predict
ground-state
wavefunctions
using
unconverged
Kohn–Sham
(KS)
Hamiltonians.
These
ML-predicted
KS
Hamiltonians
are
then
employed
sTDA-based
excited-state
calculations
(sTDA/ML).
The
results
demonstrate
that
energies,
time-derivative
couplings,
and
absorption
spectra
from
sTDA/ML
accurate
enough
compared
those
conventional
density
functional
theory
based
sTDA
(sTDA/DFT)
Furthermore,
sTDA/ML-based
molecular
simulations
on
two
different
systems,
namely
chloro-substituted
silicon
quantum
dot
monolayer
black
phosphorus,
achieve
more
than
100
times
speedup
the
linear
response
time-dependent
DFT
simulations.
work
highlights
potential
ML-accelerated
studying
complicated
photoinduced
large
offering
significant
computational
savings
without
compromising
accuracy.
Язык: Английский
Detailed Complementary Consistency: Wave Function Tells Particle How to Hop, Particle Tells Wave Function How to Collapse
The Journal of Physical Chemistry Letters,
Год журнала:
2024,
Номер
15(26), С. 6771 - 6781
Опубликована: Июнь 24, 2024
In
mixed
quantum-classical
dynamics,
the
quantum
subsystem
can
have
both
wave
function
and
particle-like
descriptions.
However,
they
may
yield
inconsistent
results
for
expectation
value
of
same
physical
quantity.
We
here
propose
a
novel
detailed
complementary
consistency
(DCC)
method
based
on
principle
internal
consistency.
Namely,
along
each
trajectory
tells
particle
how
to
hop,
while
collapse
active
states
in
ensemble.
As
benchmarked
diverse
array
representative
models
with
localized
nonadiabatic
couplings,
DCC
not
only
achieves
fully
consistent
(i.e.,
identical
populations
calculated
functions
states)
but
also
closely
reproduces
exact
results.
Due
high
performance,
our
new
has
great
potential
give
accurate
description
general
dynamics
after
further
development.
Язык: Английский
Coupled-trajectory surface hopping with sign consistency
The Journal of Chemical Physics,
Год журнала:
2025,
Номер
162(16)
Опубликована: Апрель 22, 2025
The
framework
of
exact
factorization
(XF)
has
inspired
a
series
trajectory-based
nonadiabatic
dynamics
methods
by
introducing
different
approximations.
Recently,
the
coupled-trajectory
surface
hopping
(CTSH)
method
been
proposed
to
combine
key
advantages
mixed
quantum–classical
based
on
XF
and
fewest
switches
hopping.
We
here
present
novel
variant
CTSH,
namely,
sign-consistent
CTSH
(SC-CTSH),
which
considers
proper
trajectory
clustering
reconstruct
nuclear
density
distribution
consistency
between
wave
function
active
states
introduce
decoherence.
Using
quantum
solutions
as
references,
high
performance
SC-CTSH
is
benchmarked
in
widely
studied
scattering
models
compared
with
other
related
XF-based
methods.
Due
incorporation
new
sign
algorithms,
obtains
more
accurate
momentum
decoherence
during
dynamics,
makes
combination
consistent
reliable.
This
study
further
highlights
significance
internal
states,
important
development
Язык: Английский
Detailed Complementary Consistency: Wave Function Tells Particle How to Hop, Particle Tells Wave Function How to Collapse
Опубликована: Апрель 5, 2024
In
mixed
quantum-classical
dynamics,
the
time
evolution
of
quantum
subsystem
can
involve
both
wave
function
and
particle-like
descriptions,
which
may
yield
inconsistent
results
for
expectation
value
same
physical
quantity.
this
study,
we
propose
a
novel
detailed
complementary
consistency
(DCC)
method,
achieves
fully
consistent
based
only
on
principle
internal
in
nonadiabatic
dynamics.
Namely,
tells
particle
how
to
hop
along
each
trajectory,
while
collapse
occupation
active
states.
As
benchmarked
diverse
array
representative
models,
DCC
not
gives
identical
populations
functions
states,
but
also
closely
systematically
reproduces
exact
Due
high
performance,
our
new
method
provides
promising
approach
toward
more
description
dynamics
with
much
better
reliability
efficiency
general
applications.
Язык: Английский
Multiconfigurational Surface Hopping: A Time-Dependent Variational Approach with Momentum-Jump Trajectories
Опубликована: Июнь 21, 2024
The
Ehrenfest
mean
field
dynamics
and
trajectory
surface
hopping
have
been
widely
used
in
nonadiabatic
simulations.
Based
on
the
time-dependent
variational
principle
(TDVP),
multiconfigurational
(MCE)
method
has
also
developed
can
be
regarded
as
a
extension
of
traditional
dynamics.
However,
it
is
not
straightforward
to
apply
TDVP
trajectories
because
there
exists
momentum
jump
during
hops.
To
solve
this
problem,
we
here
propose
(MCSH)
method,
where
continuous
momenta
are
obtained
by
linear
interpolation
interpolated
construct
basis
functions
for
post-processing
manner.
As
demonstrated
series
representative
spin-boson
models,
MCSH
achieves
high
accuracy
with
only
several
hundred
bases
uniformly
improve
performance
hopping.
In
principle,
combined
all
kinds
mixed
quantum-classical
trajectories,
thus
potential
properly
describe
general
Язык: Английский
Multiconfigurational Surface Hopping: a Time-Dependent Variational Approach with Momentum-Jump Trajectories
Journal of Chemical Theory and Computation,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 31, 2024
The
Ehrenfest
mean
field
dynamics
and
trajectory
surface
hopping
have
been
widely
used
in
nonadiabatic
simulations.
Based
on
the
time-dependent
variational
principle
(TDVP),
multiconfigurational
(MCE)
method
has
also
developed
can
be
regarded
as
a
extension
of
traditional
dynamics.
However,
it
is
not
straightforward
to
apply
TDVP
trajectories
because
there
exists
momentum
jump
during
hops.
To
solve
this
problem,
we
here
propose
(MCSH)
method,
where
continuous
momenta
are
obtained
by
linear
interpolation
interpolated
construct
basis
functions
for
postprocessing
manner.
As
demonstrated
series
representative
spin-boson
models,
MCSH
achieves
high
accuracy
with
only
several
hundred
bases
uniformly
improve
performance
hopping.
In
principle,
combined
all
kinds
mixed
quantum-classical
thus
potential
properly
describe
general
Язык: Английский