Absence of hydrogen insertion into highly crystalline superconducting infinite layer nickelates

The discovery of superconductivity in the infinite layer nickelates introduced a materials system analogous to the cuprates for the study of unconventional superconductivity. The synthesis of infinite layer nickelates, (${\mathrm{RNiO}}_{2}$, R = lanthanide) often uses calcium hydride (${\mathrm{CaH}}_{2}$) to facilitate the deintercalation of apical site oxygen atoms from a precursor perovskite (${\mathrm{RNiO}}_{3}$) phase via topotactic reduction. However, it remains uncertain whether the use of ${\mathrm{CaH}}_{2}$ results in the insertion of hydrogen into the infinite layer structure, and if it does, what the implications are for superconductivity. To quantify the hydrogen composition of highly crystalline infinite layer nickelates, we synthesized ${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}$ thin films on LSAT substrates and conducted time-of-flight secondary ion mass spectroscopy measurements to generate hydrogen depth profiles. We compare the hydrogen density of nickelates prepared with and without a ${\mathrm{SrTiO}}_{3}$ capping layer. Additionally, we measure the hydrogen content in nickelate samples at various doping levels spanning the superconducting phase space, including the underdoped, optimally doped, and overdoped regime. We report no significant increase in hydrogen density between the perovskite and infinite layer phases in any of the measured samples. Furthermore, we put an upperbound on the hydrogen concentration of our nickelate samples to ${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}{\mathrm{H}}_{0.05}$. Our results imply that hydrogen is not responsible for the emergence of superconductivity in the infinite layer nickelates.

Authors

Institutions

Publication Details

Journal
Physical Review Materials
Published
2024-08-12
DOI
https://doi.org/10.1103/physrevmaterials.8.084804
Citations
11
Primary Topic
Magnetic and transport properties of perovskites and related materials
Type
article
Field-Weighted Citation Impact
1.30

Funders

Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Absence of hydrogen insertion into highly crystalline superconducting infinite layer nickelates

M. Gonzalez, Harold Y. Hwang, Jennifer Fowlie, Anton V. Ievlev et al.
11 citations
Physical Review Materials
Magnetic and transport properties of perovskites and related materials
1.30
article

Absence of hydrogen insertion into highly crystalline superconducting infinite layer nickelates

M. Gonzalez, Harold Y. Hwang, Jennifer Fowlie, Anton V. Ievlev, Yijun Yu, Kyuho Lee, Wookyung Kim
article en
11 citations

Abstract

The discovery of superconductivity in the infinite layer nickelates introduced a materials system analogous to the cuprates for the study of unconventional superconductivity. The synthesis of infinite layer nickelates, (${\mathrm{RNiO}}_{2}$, R = lanthanide) often uses calcium hydride (${\mathrm{CaH}}_{2}$) to facilitate the deintercalation of apical site oxygen atoms from a precursor perovskite (${\mathrm{RNiO}}_{3}$) phase via topotactic reduction. However, it remains uncertain whether the use of ${\mathrm{CaH}}_{2}$ results in the insertion of hydrogen into the infinite layer structure, and if it does, what the implications are for superconductivity. To quantify the hydrogen composition of highly crystalline infinite layer nickelates, we synthesized ${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}$ thin films on LSAT substrates and conducted time-of-flight secondary ion mass spectroscopy measurements to generate hydrogen depth profiles. We compare the hydrogen density of nickelates prepared with and without a ${\mathrm{SrTiO}}_{3}$ capping layer. Additionally, we measure the hydrogen content in nickelate samples at various doping levels spanning the superconducting phase space, including the underdoped, optimally doped, and overdoped regime. We report no significant increase in hydrogen density between the perovskite and infinite layer phases in any of the measured samples. Furthermore, we put an upperbound on the hydrogen concentration of our nickelate samples to ${\mathrm{Nd}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{NiO}}_{2}{\mathrm{H}}_{0.05}$. Our results imply that hydrogen is not responsible for the emergence of superconductivity in the infinite layer nickelates.

Physical Review MaterialsVol. 8(8)
Oak Ridge National Laboratory (US), SLAC National Accelerator Laboratory (US), Center for Nanophase Materials Sciences, Stanford University (US)
National Science Foundation, U.S. Department of Energy, Gordon and Betty Moore Foundation, UT-Battelle, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Openalex Percentile: Top 21%
Magnetic and transport properties of perovskites and related materials
1.30
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.