Electron doping of NdNiO3 thin films using dual chamber CaH2 annealing

Amarasinghe, Dinesh K.; Yu, Haoming; Rodolakis, Fanny; Zhou, Hua; Cao, Hui; Ramanathan, Shriram

doi:10.1016/j.jssc.2022.123512

Electron doping of NdNiO₃ thin films using dual chamber CaH₂ annealing

Journal Article · Sat Aug 20 00:00:00 EDT 2022 · Journal of Solid State Chemistry

DOI:https://doi.org/10.1016/j.jssc.2022.123512· OSTI ID:1909347

^[1]; ^[1]; ^[2]; Zhou, Hua ^[2]; Cao, Hui ^[3]; Ramanathan, Shriram ^[1]

Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Hydrogen donor doping has been exploited as a strategy to manipulate the electronic structure and electrical properties of functional oxide systems. Especially, the development of synthetic methods to achieve electron doping of perovskite rare-earth nickelate thin films utilizing interstitial hydrogen is highly desirable considering the rich electronic phase diagram hosting several functional properties. Here, in this work, we present the hydrogenation of NdNiO₃ (NNO) thin films using CaH₂ annealing and the resulting giant modulation of electrical resistivity in hydrogenated NNO (H–NNO) thin films. Magnetron sputtering was employed to deposit epitaxial ~60 nm-thin NNO films on single crystal LaAlO₃ (LAO) substrates. The formation of the pristine perovskite NNO phase was realized after annealing the films at 500 °C for 24 h. CaH₂ annealing of NNO thin films for time durations ranging from 1 to 6 h was performed in a vacuumed ampule with two interconnected chambers at 280 °C. The two-chamber design enables a simple and clean approach for hydrogen doping without physical contact between the powder and sample of interest. X-ray diffraction and Raman spectroscopy revealed the formation of NNO in pristine samples, and the subsequent hydrogen incorporation upon CaH₂ annealing without forming any impurity phases. The conversion of the oxidation state of Ni towards +2 upon CaH₂ annealing was probed using X-ray photoelectron spectroscopy and X-ray absorption spectroscopy. Consequently, a substantial increase in the room-temperature resistivity was observed upon CaH₂ annealing indicating the formation of a strongly correlated electronic configuration of Ni in H–NNO due to electron doping. Overall, the findings of this study highlight the versatility of CaH₂ annealing as an electron doping method to tune the electrical properties of correlated oxides at low temperatures.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1909347

Alternate ID(s):: OSTI ID: 1883625

Journal Information:: Journal of Solid State Chemistry, Journal Name: Journal of Solid State Chemistry Vol. 315; ISSN 0022-4596

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CaH2 annealing
Electron doping
Hydrogenation
LaAlO3
Mott transition
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Electron doping of NdNiO3 thin films using dual chamber CaH2 annealing

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References (44)

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Electron doping of NdNiO₃ thin films using dual chamber CaH₂ annealing