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Selective epitaxial growth of Ca$$_{2}$$NH and CaNH thin films by reactive magnetron sputtering under hydrogen partial pressure control

Chon, S.*; Fukutani, Katsuyuki; 8 of others*

Calcium compounds with N and H are promising catalysts for NH$$_{3}$$ conversion, and their epitaxial thin films provide a platform to quantitatively understand the catalytic activities. Here we report the selective epitaxial growth of Ca$$_{2}$$NH and CaNH thin films by controlling the hydrogen partial pressure ($$P_{H_{2}}$$) during reactive magnetron sputtering. We find that the hydrogen charge states can be tuned by $$P_{H_{2}}$$: Ca$$_{2}$$NH containing H$$^{-}$$ is formed at $$P_{H_{2}}<0.04$$ Pa, while CaNH containing H$$^{+}$$ is formed at $$P_{H_{2}}>0.04$$ Pa. In situ plasma emission spectroscopy reveals that the intensity of the Ca atomic emission ($$sim$$422 nm) decreases as $$P_{H_{2}}$$ increases, suggesting that Ca reacts with H$$_{2}$$ and N$$_{2}$$ to form Ca$$_{2}$$NH at lower $$P_{H_{2}}$$, whereas at higher $$P_{H_{2}}$$, CaH$$_{x}$$ is first formed on the target surface and then sputtered to produce CaNH. This study provides a novel route to control the hydrogen charge states in Ca-N-H epitaxial thin films.

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Category:Chemistry, Physical

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