Role of Electron Correlation beyond the Active Space in Achieving Quantitative Predictions of Spin-Phonon Relaxation
Journal of Chemical Theory and Computation,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 12, 2025
Single-molecule
magnets
(SMMs)
are
promising
candidates
for
molecular-scale
data
storage
and
processing
due
to
their
strong
magnetic
anisotropy
long
spin
relaxation
times.
However,
as
the
temperature
rises,
interactions
between
electronic
states
lattice
vibrations
accelerate
relaxation,
significantly
limiting
practical
applications.
Recently,
ab
initio
simulations
have
made
it
possible
advance
our
understanding
of
phonon-induced
but
significant
deviations
from
experiments
often
been
observed.
The
description
molecules'
structure
has
mostly
based
on
complete
active
space
self-consistent
field
(CASSCF)
calculations,
impact
electron
correlation
beyond
remains
largely
unexplored.
In
this
study,
we
provide
first
systematic
investigation
spin-phonon
in
SMMs
with
post-CASSCF
multiconfigurational
methods,
specifically
CAS,
followed
by
second-order
perturbation
theory
multiconfiguration
pair-density
functional
theory.
Taking
Co(II)-
Dy(III)-based
case
studies,
analyze
how
influences
rates
across
a
range
temperatures
comparing
theoretical
predictions
experimental
observations.
Our
findings
demonstrate
that
treatments
make
achieve
quantitative
Co(II)-based
SMMs.
For
systems,
however,
accurate
require
consideration
additional
effects,
underscoring
urgent
necessity
further
advancing
study
effects
these
complex
systems.
Язык: Английский
Molecular spin relaxation of f-block metal complexes for quantum applications in a nutshell (Review article)
Low Temperature Physics,
Год журнала:
2025,
Номер
51(5), С. 517 - 532
Опубликована: Май 1, 2025
This
is
a
critical
report
on
the
most
recent
progress
towards
implementation
of
single-ion/molecule
magnets
(SIM/SMMs)
in
molecular
spin
qubits.
Short
flash-back
to
effect
lattice
distortions
doubly
degenerate
state
manganites,
mirrored
by
magnetic
bistability
SMMs,
followed
summary
suppression
quantum
decoherence
SIM/SMMs
units
slowing
spin-lattice
relaxation
and
avoiding
level
crossings.
Язык: Английский