The
recent
discovery
of
superconductivity
in
hole-doped
infinite-layer
nickelates
has
triggered
a
great
interest
the
synthesis
novel
nickelate
phases,
which
have
primarily
been
examined
thin
film
samples.
Here,
we
report
high-pressure
optical
floating
zone
(OFZ)
growth
various
perovskite
and
perovskite-derived
rare-earth
single-crystals,
investigate
effects
hole-,
electron-,
self-doping.
For
hole-doping
with
Ca
Sr,
observe
phase
separations
during
process
when
substitution
level
8%
is
exceeded.
A
similar
trend
emerges
for
electron-doping
Ce
Zr.
Employing
lower
doping
levels
allows
us
to
grow
sizeable
crystals
phase,
exhibit
significantly
different
electronic
magnetic
properties
than
undoped
parent
compounds,
such
as
decreased
resistivity
suppressed
response.
Our
insights
into
doping-dependent
formation
resulting
synthesized
reveal
limitations
opportunities
exploration
manipulation
states
nickelates.
Physical review. B./Physical review. B,
Год журнала:
2024,
Номер
109(2)
Опубликована: Янв. 19, 2024
We
conducted
a
comparative
study
of
the
rare-earth
infinite-layer
nickelate
films,
$R{\mathrm{NiO}}_{2}$
($R$
=
La,
Pr,
and
Nd),
using
resonant
inelastic
x-ray
scattering
(RIXS).
found
that
gross
features
orbital
configurations
are
essentially
same,
with
minor
variations
in
detailed
hybridization.
For
low-energy
excitations,
we
unambiguously
confirm
presence
damped
magnetic
excitations
all
three
compounds.
By
fitting
to
linear
spin-wave
theory,
comparable
spin
exchange
coupling
strengths
damping
coefficients
extracted,
indicating
universal
structure
nickelates.
Interestingly,
while
signatures
charge
order
observed
${\mathrm{LaNiO}}_{2}$
quasielastic
region
RIXS
spectrum,
it
is
absent
${\mathrm{NdNiO}}_{2}$
${\mathrm{PrNiO}}_{2}$.
This
prompts
further
investigation
into
universality
origins
within
Physical Review Materials,
Год журнала:
2023,
Номер
7(1)
Опубликована: Янв. 30, 2023
Infinite-layer
(IL)
nickelates
are
an
emerging
family
of
superconductors
whose
similarities
and
differences
to
cuprate
under
intense
debate.
To
date,
the
IL
phase
can
only
be
reached
via
topotactic
oxygen
reduction
perovskite
phase,
using
H$_2$
gas
or
reducing
agents
such
as
CaH$_2$.
While
method
has
been
widely
employed
on
thin
film
polycrystalline
powder
samples,
La$_{1-x}$Ca$_x$NiO$_3$
single-crystals
with
lateral
dimensions
up
150
$\mu$m
was
achieved
recently,
indirect
contact
Here
we
report
transformation
much
larger
LaNiO$_3$
crystals
more
than
one
millimeter,
direct
We
characterize
crystalline,
magnetic,
electronic
properties
obtained
LaNiO$_{2}$
by
single-crystal
x-ray
diffraction
(XRD),
magnetometry,
electrical
transport,
photoelectron
spectroscopy
(XPS)
measurements.
The
amount
incorporated
hydrogen
due
process
is
determined
a
extraction
method.
In
addition,
investigate
evolution
lattice
parameters
hydrostatic
pressure
12
GPa,
high-resolution
synchrotron
XRD.
Furthermore,
provide
comparison
several
physical
their
counterparts.
Physical Review Letters,
Год журнала:
2024,
Номер
133(6)
Опубликована: Авг. 8, 2024
Topotactic
reduction
utilizing
metal
hydrides
as
reagents
has
emerged
an
effective
approach
to
achieve
exceptionally
low
oxidization
states
of
ions
and
unconventional
coordination
networks.
This
method
opens
avenues
the
development
entirely
new
functional
materials,
with
one
notable
example
being
infinite-layer
nickelate
superconductors.
However,
effect
on
atomic
reconstruction
electronic
structures-crucial
for
superconductivity-remains
largely
unresolved.
We
designed
two
sets
control
Nd_{0.8}Sr_{0.2}NiO_{2}
thin
films
used
secondary
ion
mass
spectroscopy
highlight
absence
reduction-induced
hydrogen
intercalation.
X-ray
absorption
revealed
a
significant
linear
dichroism
dominant
Ni
3d_{x2-y2}
orbitals
superconducting
samples,
indicating
single-band
nature
nickelates.
Consistent
T_{c},
3d
asymmetry
manifests
domelike
dependence
duration.
Our
results
unveil
critical
role
in
modulating
Ni-3d
orbital
polarization
its
impact
properties.
Annual Review of Condensed Matter Physics,
Год журнала:
2023,
Номер
15(1), С. 305 - 324
Опубликована: Дек. 6, 2023
The
superconducting
nickelates
were
first
proposed
as
potential
analogs
to
the
cuprate
unconventional
superconductors
in
1999,
but
it
took
twenty
years
before
superconductivity
was
successfully
stabilized
epitaxial
thin
films.
Since
then,
a
flurry
of
both
experimental
and
theoretical
efforts
have
sought
understand
similarities
differences
between
two
systems
how
they
manifest
macroscopic
normal
state
properties.
Although
cuprates
indeed
share
many
commonalities
within
their
respective
phase
diagrams,
several
notable
also
emerged,
especially
regarding
parent
compounds,
electronic
hybridization,
fermiology.
Here,
we
provide
survey
rapidly
developing
landscape
layered
nickelate
superconductors,
including
recent
progress
probe
not
just
other
ordered
phases
these
compounds.
We
study
the
magnetic
and
spectral
properties
of
a
single-band
Hubbard
model
for
infinite-layer
nickelate
compound
LaNiO$_2$.
As
spatial
correlations
turn
out
to
be
key
ingredient
understanding
its
physics,
we
use
two
complementary
extensions
dynamical
mean-field
theory
take
them
into
account:
cellular
vertex
approximation.
Additionally
systematic
analysis
doping
dependence
non-Curie-Weiss
behavior
uniform
susceptibility,
provide
insight
relation
formation
pseudogap
regime
by
calculation
one-particle
function
correlation
length.
The
latter
is
order
few
lattice
spacings
when
opens,
indicating
strong-coupling
in
analogy
cuprates.
Physical review. B./Physical review. B,
Год журнала:
2024,
Номер
109(23)
Опубликована: Июнь 12, 2024
Many
mechanisms
for
unconventional
superconductivity
have
been
proposed,
but
actually
proving
which
one
is
in
charge
challenging.
Quite
astonishingly,
dynamical
vertex
approximation
predict
the
superconducting
phase
diagram
of
novel
nickelate
superconductors,
with
microscopic
origin
being
antiferromagnetic
spin
fluctuations.
The
authors
compare
fluctuations
behind
these
calculations
to
experiment.
again
good
agreement
gives
an
overall
coherent
and
complete
picture,
thus
a
high
level
confidence
that
nickelates
indeed
mediated
by
Infinite-layer
(IL)
nickelates
are
an
emerging
class
of
superconductors,
where
the
Ni$^{1+}$
valence
state
in
a
square
planar
NiO$_2$
coordination
can
only
be
reached
via
topotactic
reduction
perovskite
phase.
However,
this
soft
chemistry
with
hydrogenous
reagents
is
still
at
stage
rapid
development,
and
there
number
open
issues,
especially
considering
possibility
hydrogen
incorporation.
Here
we
study
time
dependence
transformation
LaNiO$_3$
to
LaNiO$_2$
for
powder
samples
x-ray
diffraction
gas
extraction
techniques.
While
content
increases
time,
neutron
shows
no
negative
scattering
crystal
lattice.
The
extra
appears
confined
grain
boundaries
or
secondary-phase
precipitates.
average
structure,
possibly
also
physical
properties,
primary
phase
therefore
not
noticeably
affected
by
residues
created
transformation.
Physical review. B./Physical review. B,
Год журнала:
2022,
Номер
106(3)
Опубликована: Июль 7, 2022
Since
the
discovery
of
superconductivity
in
infinite-layer
nickelates
RNiO$_2$
(R=La,
Pr,
Nd),
great
research
efforts
have
been
paid
to
unveil
its
underlying
superconducting
mechanism.
However,
physical
origin
intriguing
hole-doped
phase
diagram,
characterized
by
a
dome
sandwiched
between
two
weak
insulators,
is
still
unclear.
Here,
we
present
microscopic
theory
for
electronic
structure
from
fundamental
model-based
perspective.
We
found
that
appearance
insulator
lightly
and
heavily
regime
dominated
Mottness
Hundness,
respectively,
exhibiting
unique
orbital-selective
doping
originated
competition
Hund
interaction
crystal
field
splitting.
Moreover,
can
also
be
created
"mixed"
transition
Mott-insulator
Hund-induced
insulator,
exactly
reproducing
experimentally
observed
diagram.
Our
findings
not
only
demonstrate
orbital-dependent
strong-correlation
physics
Ni
3$d$
states,
but
provide
unified
understanding
diagram
nickelates,
which
are
distinct
well-established
paradigms
cuprates
iron
pnictides.
Physical review. B./Physical review. B,
Год журнала:
2023,
Номер
107(16)
Опубликована: Апрель 10, 2023
Despite
enormous
experimental
and
theoretical
efforts,
obtaining
generally
accepted
conclusions
regarding
the
intrinsic
magnetic
electronic
properties
of
superconducting
nickelates
remains
exceptionally
challenging.
Experiments
show
a
significant
degree
uncertainty,
indicating
hidden
factors
in
synthesized
films,
which
call
for
further
investigations.
One
those
is
possibility
intercalating
hydrogen
during
chemical
reduction
process
from
$\mathrm{Nd}(\mathrm{La}){\mathrm{NiO}}_{3}$
to
$\mathrm{Nd}(\mathrm{La}){\mathrm{NiO}}_{2}$
using
${\mathrm{CaH}}_{2}$.
While
has
been
detected
samples,
not
much
known
about
its
distribution
through
crystal
influence
on
environment.
Here,
we
tendency
toward
formation
one-dimensional
chains
infinite-layers
${\mathrm{LaNiO}}_{2}$
superconductors
density-functional
theory
supplemented
by
dynamical
mean-field
theory.
The
such
induces
coexistence
different
oxidation
states
Ni
competing
phases,
possibly
explains
recently
observed
charge
order
nickelate
superconductors.
Furthermore,
it
contributes
difficulty
synthesizing
homogeneous
determining
their
ground
states.
smoking
gun
detect
excess
flat
phonon
modes,
are
infrared
active
quite
insensitive
exact
arrangement
H
atoms.