Cell Reports Physical Science,
Год журнала:
2023,
Номер
4(12), С. 101724 - 101724
Опубликована: Дек. 1, 2023
Since
superconductivity
was
first
reported
in
nickelate
thin
films,
many
studies
have
been
published
about
this
family
of
materials,
and
different
hypotheses
proposed
for
explaining
the
mechanisms
structural
dependence.
Here,
we
report
synthesis
anchored
infinite-layer
LaNi0.9Al0.1O2.1
its
hole-doped
derivatives
by
topotactic
reduction
from
La1−xSrxNi0.9Al0.1O3
rhombohedral
perovskites.
LaNiO2
constitute
a
new
high-temperature
superconductors,
with
same
structure
as
high-Tc
cuprates
but
based
on
nickel,
only
showing
films
now.
We
describe
strategy
to
stabilize
bulk:
presence
Al
at
octahedral
sites
helps
stabilize/anchor
structure.
The
reasons
bulk
being
non-superconductors
are
hotly
debated
literature.
An
important
question
is
whether
there
some
hydrogen
incorporated
into
during
process
LaNiO3
LaNiO2,
predicted
theoretically
not
experimentally.
Our
neutron
powder
diffraction
data
show
that,
indeed,
occupies
centers
Ni–O
squares,
spectroscopic
evidence
EELS
XAS
suggests
that
Ni
reduced
Ni+
oxidation
state,
consistent
crystallochemical
data.
We
report
on
superconductivity
in
Nd
1−
x
Eu
NiO
2
using
as
a
4f
dopant
of
the
parent
NdNiO
infinite-layer
compound.
use
an
all–in
situ
molecular
beam
epitaxy
reduction
process
to
achieve
superconducting
phase,
providing
alternate
method
ex
CaH
induce
nickelates.
The
samples
exhibit
step-terrace
structure
their
surfaces,
have
T
c
onset
21
K
at
=
0.25,
and
large
upper
critical
field
that
may
be
related
doping.
We
present
an
integrated
procedure
for
the
synthesis
of
infinite-layer
nickelates
using
molecular-beam
epitaxy
with
gas-phase
reduction
by
atomic
hydrogen.
first
discuss
challenges
in
growth
and
characterization
perovskite
NdNiO3/SrTiO3,
arising
from
post
crack
formation
stoichiometric
films.
then
detail
a
fully
reducing
NdNiO3
films
to
phase,
NdNiO2,
hydrogen;
resulting
display
excellent
structural
quality,
smooth
surfaces,
lower
residual
resistivities
than
reduced
other
methods.
utilize
situ
nature
this
technique
investigate
role
that
SrTiO3
capping
layers
play
process,
illustrating
their
importance
preventing
secondary
phases
at
exposed
nickelate
surface.
A
comparative
bulk-
surface-sensitive
study
indicates
polycrystalline
crust
on
film
surface
serves
limit
process.
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. 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.
Physical review. B./Physical review. B,
Год журнала:
2023,
Номер
108(17)
Опубликована: Ноя. 22, 2023
A
recent
experiment
[X.
Ding
et
al.,
Nature
(London)
615,
50
(2023)]
indicates
that
superconductivity
in
nickelates
is
restricted
to
a
narrow
window
of
hydrogen
concentration,
$0.22
Physical Review Materials,
Год журнала:
2024,
Номер
8(8)
Опубликована: Авг. 12, 2024
The
discovery
of
superconductivity
in
the
infinite
layer
nickelates
introduced
a
materials
system
analogous
to
cuprates
for
study
unconventional
superconductivity.
synthesis
nickelates,
(${\mathrm{RNiO}}_{2}$,
R
=
lanthanide)
often
uses
calcium
hydride
(${\mathrm{CaH}}_{2}$)
facilitate
deintercalation
apical
site
oxygen
atoms
from
precursor
perovskite
(${\mathrm{RNiO}}_{3}$)
phase
via
topotactic
reduction.
However,
it
remains
uncertain
whether
use
${\mathrm{CaH}}_{2}$
results
insertion
hydrogen
into
structure,
and
if
does,
what
implications
are
To
quantify
composition
highly
crystalline
we
synthesized
${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}$
thin
films
on
LSAT
substrates
conducted
time-of-flight
secondary
ion
mass
spectroscopy
measurements
generate
depth
profiles.
We
compare
density
prepared
with
without
${\mathrm{SrTiO}}_{3}$
capping
layer.
Additionally,
measure
content
nickelate
samples
at
various
doping
levels
spanning
superconducting
space,
including
underdoped,
optimally
doped,
overdoped
regime.
report
no
significant
increase
between
phases
any
measured
samples.
Furthermore,
put
an
upperbound
concentration
our
${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}{\mathrm{H}}_{0.05}$.
Our
imply
that
is
not
responsible
emergence
nickelates.
Crystals,
Год журнала:
2022,
Номер
12(5), С. 656 - 656
Опубликована: Май 4, 2022
Superconductivity
has
entered
the
nickel
age
marked
by
enormous
experimental
and
theoretical
efforts.
Notwithstanding,
synthesizing
nickelate
superconductors
remains
extremely
challenging,
not
least
due
to
incomplete
oxygen
reduction
topotactic
hydrogen.
Here,
we
present
density-functional
theory
calculations,
identify
a
phonon
mode
as
possible
indication
for
hydrogen
discuss
charge
redistribution
patterns
around
impurities.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(35), С. 23658 - 23669
Опубликована: Янв. 1, 2024
We
manipulated
the
ionic
defects
(protons
and
oxygen
vacancies)
in
perovskite
nickelates
through
thermochemical
dehydration.
quantified
correlation
between
physical
properties
of
vacancy
concentration.