Formulation and Implementation of Frequency-Dependent Linear Response Properties with Relativistic Coupled Cluster Theory for GPU-Accelerated Computer Architectures
Journal of Chemical Theory and Computation,
Journal Year:
2024,
Volume and Issue:
20(2), P. 677 - 694
Published: Jan. 9, 2024
We
present
the
development
and
implementation
of
relativistic
coupled
cluster
linear
response
theory
(CC-LR),
which
allows
determination
molecular
properties
arising
from
time-dependent
or
time-independent
electric,
magnetic,
mixed
electric-magnetic
perturbations
(within
a
common
gauge
origin
for
magnetic
properties)
as
well
taking
into
account
finite
lifetime
excited
states
in
framework
damped
theory.
showcase
our
implementation,
is
capable
to
offload
computationally
intensive
tensor
contractions
characteristic
onto
graphical
processing
units,
calculation
(a)
frequency-(in)dependent
dipole-dipole
polarizabilities
IIB
atoms
selected
diatomic
molecules,
with
particular
emphasis
on
valence
absorption
cross
sections
I
Language: Английский
Benchmarking third-order cluster perturbation theory for electronically excited states
The Journal of Chemical Physics,
Journal Year:
2025,
Volume and Issue:
162(9)
Published: March 5, 2025
In
this
study,
we
investigate
the
reliability
of
cluster
perturbation
(CP)
theory
applied
to
calculation
electronically
excited
states
through
a
comprehensive
benchmark.
CP
theory,
perturbative
corrections
are
added
properties
parent
excitation
space,
which
converge
toward
target
space.
For
CPS(D-n)
model,
order
n
coupled
singles
(CCS)
energies
and
doubles
(CCSD)
energies.
Through
comparative
analysis
energy
calculations
across
diverse
set
molecules
wavefunction
methods,
present
evaluation
accuracy
third-order
CPS(D)
CPS(D-3),
in
calculating
Our
findings
demonstrate
that
CPS(D-3)
is
reliable
alternative
established
particularly
CCSD,
while
systematically
overestimating
compared
high-level
methods
such
as
CC3.
These
results
highlight
strengths
limitations
well
promising
directions
for
its
future
development.
Language: Английский
Cluster perturbation theory. XII. Parallel implementation of variational excitation energy series for the coupled cluster singles and doubles model
The Journal of Chemical Physics,
Journal Year:
2025,
Volume and Issue:
162(21)
Published: June 3, 2025
An
efficient
implementation
of
the
variational
cluster
perturbation
excitation
energy
series
through
fifth
order
is
described.
The
has
coupled
singles
energies
as
zeroth
and
targets
doubles
(CCSD)
energies.
utilizes
resolution
identity
approximation
for
two-electron
integrals.
uses
2n
+
1/2n
2
rules
to
eliminate
all
parameters
higher
than
second
order.
computational
efficiency
illustrated
by
performing
calculations
on
a
single
node
systems
with
up
1000
basis
functions
comparing
CCSD
calculations.
Using
hybrid
parallel
open
multiprocessing/message-passing
interface
graphics
processing
unit
offloading,
fifth-order
1750
can
be
calculated
in
8
h
using
20
nodes
Frontier
supercomputer
at
Oak
Ridge
National
Laboratory.
A
benchmark
131
diverse
set
molecules
presented.
For
fourth
models,
few
prominent
outliers
are
present.
We
demonstrate
how
these
cases
may
identified
simple
diagnostic,
remaining
values
being
indistinguishable
from
practice.
Language: Английский
Tensor Hypercontraction of Cluster Perturbation Theory: Quartic Scaling Perturbation Series for the Coupled Cluster Singles and Doubles Ground-State Energies
Journal of Chemical Theory and Computation,
Journal Year:
2024,
Volume and Issue:
20(5), P. 1932 - 1943
Published: Feb. 21, 2024
Even
though
cluster
perturbation
theory
has
been
shown
to
be
a
robust
noniterative
alternative
coupled
theory,
it
is
still
plagued
by
high
order
polynomial
computational
scaling
and
the
storage
of
higher
tensors.
We
present
proof-of-concept
strategy
for
implementing
ground-state
energy
series
singles
doubles
with
N4
using
tensor
hypercontraction
(THC).
The
reduction
in
two
orders
achieved
decomposing
electron
repulsion
integrals,
amplitudes
multipliers,
as
well
selected
double
intermediates
THC
format.
Using
outlined
strategy,
we
showcase
that
pilot
implementations
retain
numerical
accuracy
within
1
kcal/mol
relative
corresponding
conventional
density
fitting
implementations,
empirically
verify
scaling.
Language: Английский
Cluster Perturbation Theory for Core Excited States and Core Ionization Potentials Using Core-Valence Separation
The Journal of Physical Chemistry A,
Journal Year:
2024,
Volume and Issue:
128(46), P. 10087 - 10098
Published: Nov. 13, 2024
The
development
of
accurate
and
fast
computational
procedures
for
the
Language: Английский
Coupled cluster theory on modern heterogeneous supercomputers
Frontiers in Chemistry,
Journal Year:
2023,
Volume and Issue:
11
Published: June 14, 2023
This
study
examines
the
computational
challenges
in
elucidating
intricate
chemical
systems,
particularly
through
Language: Английский
Corrigendum: Coupled cluster theory on modern heterogeneous supercomputers
Frontiers in Chemistry,
Journal Year:
2023,
Volume and Issue:
11
Published: Aug. 15, 2023
[This
corrects
the
article
DOI:
10.3389/fchem.2023.1154526.].
Language: Английский
Special Topic on High Performance Computing in Chemical Physics
The Journal of Chemical Physics,
Journal Year:
2023,
Volume and Issue:
159(21)
Published: Dec. 1, 2023
Computational
modeling
and
simulation
have
become
indispensable
scientific
tools
in
virtually
all
areas
of
chemical,
biomolecular,
materials
systems
research.
Computation
can
provide
unique
detailed
atomic
level
information
that
is
difficult
or
impossible
to
obtain
through
analytical
theories
experimental
investigations.
In
addition,
recent
advances
micro-electronics
resulted
computer
architectures
with
unprecedented
computational
capabilities,
from
the
largest
supercomputers
common
desktop
computers.
Combined
development
new
domain
science
methodologies
novel
programming
models
techniques,
this
has
resources
capable
providing
results
at
better
than
chemical
accuracy
for
increasingly
realistic
environments.
Language: Английский