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The effects of plasma reactants on the plasma-assisted atomic layer deposition (ALD) of lithium phosphate were investigated in relation to the fabrication of high-quality lithium phosphorus oxynitride (LiPON) thin films for the potential use as a solid-state electrolyte (SSE) in both microbatteries and neuromorphic devices. Our ALD processes enable the incorporation of nitrogen into a lithium phosphate matrix, using lithium tert-butoxide and tris(dimethylamino)phosphine as the lithium and phosphorus precursors, respectively, in a deposition temperature window of 220-300 °C. With O2 plasma, polycrystalline lithium phosphate films, with a relatively well-arranged pyrophosphate, are deposited. Amorphous LiPON films, with a mixture of pyrophosphates and orthophosphate, are obtained when Ar or NH3 plasma is used. When the NH3 flow rate increases, the nitrogen composition increases up to ~13%, while residual carbon is kept to below a few percent. For a Li2.5PO1.9N0.8 film deposited at 300 °C with NH3 plasma, the ionic conductivity is measured as 1.65 ± 0.42 × 10-6 S/cm at 25 °C, with an activation energy of 0.66 eV. This conductivity is the highest value of any ALD LiPON film reported to date. Our ALD processes exhibit a high level of controllability of the molecular structures of the phosphorus oxynitride matrix, with high ionic conductivity, which makes them suitable for realizing high-performance Li SSE thin films.

権利情報:

• In Copyright
  

  This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.chemmater.4c00960

キーワード: atomic layer deposition, lithium phosphate, lithium phosphorus oxynitride, solid-state electrolyte, plasma reactant

刊行年月日: 2024-06-25

出版者: American Chemical Society (ACS)

掲載誌:

• Chemistry of Materials (ISSN: 08974756) vol. 36 issue. 12 p. 6193-6204

研究助成金:

• Ministry of Education, Culture, Sports, Science and Technology JPMXP1223NM5065
• Japan Society for the Promotion of Science 21H03412

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4556

公開URL: https://doi.org/10.1021/acs.chemmater.4c00960

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更新時刻: 2025-06-25 08:30:22 +0900

MDRでの公開時刻: 2025-06-25 08:22:56 +0900