Extensive hydrogen incorporation is not necessary for superconductivity in topotactically reduced nickelates

Purnima P. Balakrishnan (), Dan Ferenc Segedin, Lin Er Chow, P. Quarterman, Shin Muramoto, Mythili Surendran, Ranjan K. Patel, Harrison LaBollita, Grace A. Pan, Qi Song, Yang Zhang, Ismail El Baggari, Koushik Jagadish, Yu-Tsun Shao, Berit H. Goodge, Lena F. Kourkoutis, Srimanta Middey, Antia S. Botana, Jayakanth Ravichandran (), A. Ariando (), Julia A. Mundy () and Alexander J. Grutter ()
Additional contact information
Purnima P. Balakrishnan: National Institute of Standards and Technology
Dan Ferenc Segedin: Harvard University
Lin Er Chow: National University of Singapore
P. Quarterman: National Institute of Standards and Technology
Shin Muramoto: National Institute of Standards and Technology
Mythili Surendran: University of Southern California
Ranjan K. Patel: Indian Institute of Science
Harrison LaBollita: Arizona State University
Grace A. Pan: Harvard University
Qi Song: Harvard University
Yang Zhang: Harvard University
Ismail El Baggari: Harvard University
Koushik Jagadish: University of Southern California
Yu-Tsun Shao: University of Southern California
Berit H. Goodge: Cornell University
Lena F. Kourkoutis: Cornell University
Srimanta Middey: Indian Institute of Science
Antia S. Botana: Arizona State University
Jayakanth Ravichandran: University of Southern California
A. Ariando: National University of Singapore
Julia A. Mundy: Harvard University
Alexander J. Grutter: National Institute of Standards and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH2. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La1−xXxNiO2 / SrTiO3 (X = Ca and Sr) and Nd6Ni5O12 / NdGaO3 films, along with non-superconducting NdNiO2 / SrTiO3 and (Nd,Sr)NiO2 / SrTiO3. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that extensive hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates.

Date: 2024
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DOI: 10.1038/s41467-024-51479-3

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