Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c0261710169J
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Funding
- JSPS Kakenhi [JP19H04689, JP17H05216, JP19H02596, JP18H05514, JP18H05518, JP22H04506, JP18H03876]
- JST-PRESTO [JPMJPR17N6]
- JST-CREST Grant [JPMJCR1523]
- Institute for Materials Research, Tohoku University [18K0095, 19K0060]
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Selective epitaxial growth of Ca2NH and CaNH thin films is achieved by controlling hydrogen partial pressure (PH2). This study provides a novel approach to control hydrogen charge states in Ca-N-H epitaxial thin films.
Calcium compounds with N and H are promising catalysts for NH3 conversion, and their epitaxial thin films provide a platform to quantitatively understand the catalytic activities. Here we report the selective epitaxial growth of Ca2NH and CaNH thin films by controlling the hydrogen partial pressure (PH2) during reactive magnetron sputtering. We find that the hydrogen charge states can be tuned by PH2: Ca2NH containing H- is formed at PH2 < 0.04 Pa, while CaNH containing H+ is formed at PH2 > 0.04 Pa. In situ plasma emission spectroscopy reveals that the intensity of the Ca atomic emission (similar to 422 nm) decreases as PH2 increases, suggesting that Ca reacts with H2 and N2 to form Ca2NH at lower PH2, whereas at higher PH2, CaHx 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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