Absence of hydrogen insertion into highly crystalline superconducting infinite layer nickelates

M. Gonzalez, A. Ievlev, K. Lee, W. Kim, Y. Yu, J. Fowlie, H. Y. Hwang

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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, (RNiO2, R = lanthanide) often uses calcium hydride (CaH2) to facilitate the deintercalation of apical site oxygen atoms from a precursor perovskite (RNiO3) phase via topotactic reduction. However, it remains uncertain whether the use of CaH2 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 Nd1-xSrxNiO2 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 SrTiO3 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 Nd1-xSrxNiO2H0.05. Our results imply that hydrogen is not responsible for the emergence of superconductivity in the infinite layer nickelates.

Original languageEnglish
Article number084804
JournalPhysical Review Materials
Volume8
Issue number8
DOIs
StatePublished - Aug 2024

Funding

This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering (Contract No. DE-AC02-76SF00515) and the Gordon and Betty Moore Foundation's Emergent Phenomena in Quantum Systems Initiative (Grant No. GBMF9072, synthesis equipment). Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under Award No. ECCS-2026822. Part of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility and using instrumentation within ORNL's Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy.

FundersFunder number
Basic Energy Sciences
U.S. Department of Energy
Office of Science
Division of Materials Sciences and EngineeringDE-AC02-76SF00515
Gordon and Betty Moore FoundationGBMF9072
National Science FoundationECCS-2026822
UT-BattelleDE-AC05-00OR22725

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