利用報告書 / User's Report

【公開日：2023.07.28】【最終更新日：2023.05.16】

課題データ / Project Data

課題番号 / Project Issue Number

22BA0005

利用課題名 / Title

次世代高機能性薄膜の評価

利用した実施機関 / Support Institute

筑波大学

機関外・機関内の利用 / External or Internal Use

内部利用（ARIM事業参画者以外）/Internal Use (by non ARIM members)

技術領域 / Technology Area

【横断技術領域 / Cross-Technology Area】（主 / Main）計測・分析/Advanced Characterization（副 / Sub）加工・デバイスプロセス/Nanofabrication

【重要技術領域 / Important Technology Area】（主 / Main）革新的なエネルギー変換を可能とするマテリアル/Materials enabling innovative energy conversion（副 / Sub）-

キーワード / Keywords

電子顕微鏡/Electron microscopy,スパッタリング/Sputtering,リソグラフィ/Lithography,膜加工・エッチング/Film processing and Etching,二次電池/ Secondary battery,太陽電池/ Solar cell,熱電材料/ Thermoelectric material,電極材料/ Electrode material


利用者と利用形態 / User and Support Type

利用者名（課題申請者）/ User Name (Project Applicant)

都甲 薫

所属名 / Affiliation

筑波大学

共同利用者氏名 / Names of Collaborators in Other Institutes Than Hub and Spoke Institutes

石山隆光,鈴木大成,野沢公暉,前田真太郎,居倉功汰,西田竹志

ARIM実施機関支援担当者 / Names of Collaborators in The Hub and Spoke Institutes
利用形態 / Support Type

（主 / Main）機器利用/Equipment Utilization（副 / Sub）,技術代行/Technology Substitution


利用した主な設備 / Equipment Used in This Project

BA-020：顕微ラマン
BA-009：パターン投影リソグラフィシステム
BA-003：FIB-SEM
BA-007：ウェハーダイシングマシン
BA-008：電界放出型走査電子顕微鏡


報告書データ / Report

概要（目的・用途・実施内容）/ Abstract (Aim, Use Applications and Contents)

高機能性薄膜（Si、Ge、C、GaAs等）は、次世代のディスプレイや太陽電池、熱電素子、二次電池等の材料として有望である。ガラスやプラスチック等の汎用基板上に合成された各材料について、その特性を評価することを目的とする。

実験 / Experimental

 Ta箔上に非晶質C層とNi層を各25–500 nm堆積後、600  ℃の熱処理を施し、層交換を誘起した。MLGを金属Liと対向させ、電解液1M LiPF6 in EC/DEC（1:1 v/v）を用いた二極式セルを作製し、充放電試験を行った。

結果と考察 / Results and Discussion

Ni除去後の試料表面のラマンスペクトルから、MLGに起因した3つのピークが得られた（Fig. 1(a)）。100 nmの試料の断面TEM像より、MLGは基板に垂直に配向していた（Fig. 1(b),(c)）。各試料の充放電特性を測定した結果、膜厚が大きいほどプラトー領域が増大した（Fig. 2(a),(b)）。一方、0.1 V以上で見られる非プラトーな容量は膜厚による大きな変化が見られず、界面に生成された金属酸化物に起因することが推察された。

図・表・数式 / Figures, Tables and Equations


Fig. 1 (a) Raman spectra obtained from the front side of the annealed samples. (b) Cross-sectional TEM image and (c) high-resolution lattice image of the 100-nm-thick sample.



Fig. 2 Galvanostatic charge/discharge cycles for the (a) 25- and  (b) 500-nm-thick samples at a current rate of 1C.


その他・特記事項（参考文献・謝辞等） / Remarks(References and Acknowledgements)

　本研究にご協力いただいたARIMスタッフの皆さまに御礼申し上げます。


成果発表・成果利用 / Publication and Patents

論文・プロシーディング（DOIのあるもの） / DOI (Publication and Proceedings)
  1. Takamitsu Ishiyama, Machine learning of fake micrographs for automated analysis of crystal growth process, Science and Technology of Advanced Materials: Methods, 2, 213-221(2022).
    DOI: 10.1080/27660400.2022.2082235
  2. H. Murata, Si1–xGex anode synthesis on plastic films for flexible rechargeable batteries, Scientific Reports, 12, (2022).
    DOI: 10.1038/s41598-022-18072-4
  3. Toshifumi Imajo, Acceptor defects in polycrystalline Ge layers evaluated using linear regression analysis, Scientific Reports, 12, (2022).
    DOI: 10.1038/s41598-022-19221-5
  4. Koki Nozawa, Metal-Catalyzed Nanostructured Silicon Films as Potential Anodes for Flexible Rechargeable Batteries, ACS Applied Nano Materials, 5, 17264-17270(2022).
    DOI: 10.1021/acsanm.2c04476
  5. Shintaro Maeda, High Thermoelectric Performance in Polycrystalline GeSiSn Ternary Alloy Thin Films, ACS Applied Materials & Interfaces, 14, 54848-54854(2022).
    DOI: 10.1021/acsami.2c14785
  6. Taisei Suzuki, Thickness Dependency of Battery Anode Properties in Multilayer Graphene, ACS Applied Materials & Interfaces, 14, 54670-54675(2022).
    DOI: 10.1021/acsami.2c14152
  7. Koki Nozawa, n-Type Polycrystalline Germanium Layers Formed by Impurity-Doped Solid-Phase Growth, ACS Applied Electronic Materials, 5, 1444-1450(2023).
    DOI: 10.1021/acsaelm.2c01381
口頭発表、ポスター発表および、その他の論文 / Oral Presentations etc.
  1. Shintaro Maeda, Tomoki Ozawa, Takashi Suemasu and Kaoru Toko, Group IV Semiconductor Alloy Thin Films for Environmentally Friendly Thermoelectric Generators, 2022 International Conference on Solid State Devices and Materials（SSDM2022), C-1-01, Online, Sept. 27 (2022).
  2. Koki Nozawa, Takeshi Nishida, Takashi Suemasu and Kaoru Toko, Impact on N-type Impurities on Solid-phase Crystallization of Amorphous Ge, 2022 International Conference on Solid State Devices and Materials（SSDM2022), B-3-03, Online, Sept. 27 (2022).
  3. Takeshi Nishida, Takashi Suemasu and Kaoru Toko, Large-grained GaAs Films Synthesized on Insulating Substrates for Flexible Solar Cells, The 22nd International Vacuum Congress（IVC-22), Mon-B1-5, Hokkaido, Sept. 12 (2022).
  4. Takamitsu Ishiyama, Toshifumi Imajo, Takashi Suemasu and Kaoru Toko, Polycrystalline Ge layer on plastic film leading to high carrier mobility, The 22nd International Vacuum Congress（IVC-22), Tue-E1-3, Hokkaido, Sept. 13 (2022).
  5. Taisei Suzuki, Takashi Suemasu and Kaoru Toko, Lithium-ion Battery Anode Operation of Multilayer Graphene Formed by Low-temperature Layer Exchange, The 22nd International Vacuum Congress（IVC-22), Tue-G2-7, Hokkaido, Sept. 13 (2022).
  6. Koki Nozawa, Hiromasa Murata, Takashi Suemasu and Kaoru Toko, Compositional Effects on Anode Properties of SiGe Formed by Al-Induced Layer-Exchange, The 22nd International Vacuum Congress（IVC-22), Tue-E1-4, Hokkaido, Sept. 13 (2022).
  7. Shintaro Maeda, Takamitsu Ishiyama, Toshifumi Imajo, Takashi Suemasu and Kaoru Toko, Grain size control of in solid-phase crystallization of Ge thin films using nucleation layer, The 22nd International Vacuum Congress（IVC-22), Tue-PO1B-6, Hokkaido, Sept. 13 (2022).
  8. Takeshi Nishida, Takashi Suemasu and Kaoru Toko, First Elucidation of the Correlation between Grain Size and Photoresponsivity in Polycrystalline GaAs Films, The 5th International Union of Materials Research Societies　International Conference of Young Researchers on Advanced Material（IURMS-ICYRAM 2022), E-O4-003, online, Japan, Aug. 4 (2022).
  9. Takamitsu Ishiyama, Takuto Mizoguchi, Toshifumi Imajo, Takashi Suemasu and Kaoru Toko, Demonstration of photoresponsivity in polycrystalline Ge-based thin films, The 5th International Union of Materials Research Societies　International Conference of Young Researchers on Advanced Material（IURMS-ICYRAM 2022), E-O4-002, online, Japan, Aug. 4 (2022).
  10. Koki Nozawa, Hiromasa Murata, Takashi Suemasu and Kaoru Toko, Low-temperature Synthesis of Si1-xGex Layers for Flexible Battery Anodes, The 5th International Union of Materials Research Societies　International Conference of Young Researchers on Advanced Material（IURMS-ICYRAM 2022), E-O3-010, online, Japan, Aug. 3 (2022).
  11. Shintaro Maeda, Takamitsu Ishiyama, Toshifumi Imajo, Takashi Suemasu and Kaoru Toko, Nucleation control in the solid-phase crystallization of amorphous Ge layer leading to high hole mobility, The 5th International Union of Materials Research Societies　International Conference of Young Researchers on Advanced Material（IURMS-ICYRAM 2022), E-O3-005, online, Japan, Aug. 3 (2022).
  12. Takeshi Nishida, Takashi Suemasu and Kaoru Toko, Large-grained GaAs Films Synthesized on Insulating Substrates for Flexible Solar Cells, The 6th Asia-Pacific Conference on Semiconducting Silicides and Related Materials , P-II-5, online, July 31, 2022.
  13. Taisei Suzuki, Takashi Suemasu and Kaoru Toko, Effects of Layer Exchange Conditions o, f Multilayer Graphene on Anode Properties in Li-ion Batteries, The 6th Asia-Pacific Conference on Semiconducting Silicides and Related Materials , Sun-a-O3, online, July 31, 2022.
  14. Takamitsu Ishiyama, Takashi Suemasu and Kaoru Toko, Automated and fast analysis of solid-phase growth properties using deep machine learning, The 6th Asia-Pacific Conference on Semiconducting Silicides and Related Materials , Sun-a-O2, online, July 31, 2022.
  15. Koki Nozawa, Takeshi Nishida, Takashi Suemasu and Kaoru Toko, Solid-phase Crystallization of P-doped Amorphous Ge on Insulator Leading to the Highest Electron Mobility, The 6th Asia-Pacific Conference on Semiconducting Silicides and Related Materials , Sun-a-O1, online, July 31, 2022.
  16. Shintaro Maeda, Tomoki Ozawa, Takashi Suemasu and Kaoru Toko, Thermoelectric Properties in Group IV Ternary Alloy Thin Films Formed by Advanced Solid-phase Crystallization, The 6th Asia-Pacific Conference on Semiconducting Silicides and Related Materials , Sat-p-O5, online, July 30, 2022.
  17. 野沢 公暉, 加登 裕也, 石山 隆光, 末益 崇, 都甲 薫, 機械学習を用いた多元III-V族化合物半導体のリチウムイオン二次電池負極特性実証, SATテクノロジーショーケース2023, P-6, つくば国際会議場, Jan. 26 (2023).
  18. 野沢公暉, 末益崇, 都甲薫, V族元素添加によるGeSn薄膜の低温成長, 第5回結晶工学×ISYSE合同研究会, P-03, 大阪大学, Nov. 18 (2022).
  19. 前田真太郎, 末益崇, 都甲薫, IV 族三元混晶の薄膜合成と高熱電性能実証, 薄膜材料デバイス研究会 第19回研究集会, 17p-O06, 京都, Nov. 17 (2022).
  20. 西田 竹志, 末益 崇, 都甲 薫, 層交換Geシード技術を活用した疑似単結晶GaAs薄膜の絶縁基板上合成, 第51回結晶成長国内会議, 01p-P17, 広島, Nov. 1 (2022).
特許 / Patents

特許出願件数 / Number of Patent Applications：2件
特許登録件数 / Number of Registered Patents：0件

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