Precise controls and fundamental understandings of oxidation reactions to for ultrathin oxides at Ge surfaces for future nano-devices

• Project/Area Number: 26420289
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Multi-year Fund
• Section: 一般
• Research Field: Electronic materials/Electric materials
• Research Institution: Japan Atomic Energy Agency
• Principal Investigator: Yoshigoe Akitaka 国立研究開発法人日本原子力研究開発機構, 原子力科学研究部門 物質科学研究センター, 研究主幹 (00283490)
• Co-Investigator(Kenkyū-buntansha): 寺岡 有殿 国立研究開発法人量子科学技術研究開発機構, 関西光科学研究所 放射光科学研究センター, 上席研究員(定常) (10343922)
• Project Period (FY): 2014-04-01 – 2017-03-31
• Project Status: Completed (Fiscal Year 2016)
• Budget Amount: ¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000); Fiscal Year 2016: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000); Fiscal Year 2015: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000); Fiscal Year 2014: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
• Keywords: Ge / 酸化 / 放射光 / 分子線 / 酸化物 / 表面化学 / 表面反応 / 反応ダイナミクス / 半導体 / 酸化反応プロセス / 光電子分光 / ゲルマニウム / シリコン / キネティクス / ダイナミクス / 吸着 / 半導体表面 / Ge単結晶表面 / 酸化反応 / 超音速分子線 / その場観察 / 表面

Outline of Final Research Achievements

Ge is an attracting material for future nano-devices becasue of its high carrier mobility compared to Si. This study aimed to find out the reaction parameters to control Ge oxide formation and discover anomalous oxidation reactions for IV -group elements based on the precise measurements of synchrotron radiation photoelectron spectroscopy combined with supersonic molecular beams. As expected prior to this study, it was found that supersonic oxygen molecular beams induces to form the different oxidation states, which can not be realized only using thermal equilibrium gas. The valency of oxidation states and its oxygen translational energy dependence are considerably different from that of Si oxidation. We also succeeded to observe a molecularly adsorbed oxygen, which has been considered to be absent over three decades. We believe that our experimental results are important and useful to control nanoscale oxidation recations at surfaces for not only Ge but also Si.

Research Products

• [Journal Article] Initial oxidation behavior of Ni3Al(210) surface induced by supersonic oxygen molecular beam at room temperature (2017)
  • Author(s): Y. Xu, J. Sakurai, Y. Teraoka, A. Yoshigoe, M. Demura, T. Hirano
  • Journal Title: Applied Surface Science Volume: 391 Pages: 18-23
  • DOI: 10.1016/j.apsusc.2016.01.259
  • Peer Reviewed
• [Journal Article] Comprehensive study on initial thermal oxidation of GaN(0001) surface and subsequent oxide growth in dry oxygen ambient (2017)
  • Author(s): T. Yamada, J. Ito, R. Asahara, K. Watanabe, M. Nozaki, S. Nakazawa, Y. Anda, M. Ishida, T. Ueda, A. Yoshigoe, T. Hosoi, T. Shimura, H. Watanabe
  • Journal Title: J. Appl. Phys. Volume: 121 Issue: 3
  • DOI: 10.1063/1.4974458
  • Peer Reviewed
• [Journal Article] Detection of molecular oxygen adsorbate during room-temperature oxidation of Si(100)2×1 surface: In situ synchrotron radiation photoemission study (2016)
  • Author(s): A. Yoshigoe, Y. Yamada, R. Taga, S. Ogawa, Y. Takakuwa
  • Journal Title: Japanese Journal of Applied Physics Volume: 55 Issue: 10 Pages: 100307-100307
  • DOI: 10.7567/jjap.55.100307
  • NAID: 210000147114
  • Peer Reviewed
• [Journal Article] Effect of nitrogen incorporation into Al-based gate insulators in AlON/AlGaN/GaN metal-oxide-semiconductor structures (2016)
  • Author(s): R. Asahara, M. Nozaki, T. Yamada, J. Ito, S. Nakazawa, M. Ishida, T. Ueda, A. Yoshigoe, T. Hosoi, T. Shimura, H. Watanabe
  • Journal Title: Applied Physics Express Volume: 9 Issue: 10 Pages: 101002-101002
  • DOI: 10.7567/apex.9.101002
  • NAID: 210000138056
  • Peer Reviewed
• [Journal Article] Synchrotron radiation X-ray photoelectron spectroscopy of Ti/Al ohmic contacts to n-type GaN: Key role of Al capping layers in interface scavenging reactions (2016)
  • Author(s): M. Nozaki, J. Ito, R. Asahara, S. Nakazawa, M. Ishida, T. Ueda, A. Yoshigoe, T. Hosoi, T. Shimura, H. Watanabe
  • Journal Title: Applied Physics Express Volume: 9 Issue: 10 Pages: 105801-105801
  • DOI: 10.7567/apex.9.105801
  • NAID: 210000138073
  • Peer Reviewed
• [Journal Article] Valence-band electronic structure evolution of graphene oxide upon thermal annealing for optoelectronics (2016)
  • Author(s): H. Yamaguchi, S. Ogawa, D. Watanabe, H. Hozumi, Y. Gao, G. Eda, C. Mattevi, T. Fujita, A. Yoshigoe, S. Ishizuka, L. Adamska, T. Yamada, A. M. Dattelbaum, G. Gupta, S. K. Doorn, K. A. Velizhanin, Y. Teraoka, M. Chen, H. Htoon, M. Chhowalla, A. D. Mohite, Y. Takakuwa
  • Journal Title: Phys. Status Solidi A Volume: 213 Issue: 9 Pages: 2380-2386
  • DOI: 10.1002/pssa.201532855
  • Peer Reviewed
• [Journal Article] Surface temperature dependence of oxidation of Cu3Au(111) by an energetic oxygen molecule (2016)
  • Author(s): Y. Tsuda, A. Yoshigoe, Y. Teraoka, M. Okada
  • Journal Title: Materials Research Express Volume: 3 Issue: 3 Pages: 035014-035014
  • DOI: 10.1088/2053-1591/3/3/035014
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Investigation of segregation during oxidation of Ni-Cu alloy by in situ photoelectron spectroscopy (2016)
  • Author(s): T. Doi, Y. Nishiyama, A. Yoshigoe, Y. Teraoka
  • Journal Title: Surface and Interface Analysis Volume: 48 Issue: 7 Pages: 685-688
  • DOI: 10.1002/sia.6001
  • Peer Reviewed
• [Journal Article] Experimental and Theoretical Studies on Oxidation of Cu-Au Alloy Surfaces -Effect of Bulk Au Concentration- (2016)
  • Author(s): M. Okada, Y. Tsuda, K. Oka, K. Kojima, W. A. Dino, A.Yoshigoe, H. Kasai
  • Journal Title: Scientific Reports Volume: 6 Issue: 1
  • DOI: 10.1038/srep31101
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Enhancement of SiO2/Si(001) interfacial oxidation induced by thermal strain during rapid thermal oxidation (2016)
  • Author(s): S. Ogawa, J. Tang, A. Yoshigoe, S. Ishidzuka, Y. Takakuwa
  • Journal Title: The Journal of Chemical Physics Volume: 145 Issue: 11 Pages: 114701-114701
  • DOI: 10.1063/1.4962671
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Characterization of Polycrystalline Tungsten Surfaces Irradiated with Nitrogen Ions by X-ray Photoelectron Spectroscopy (2016)
  • Author(s): Y. Kamiura, K. Umezawa, Y. Teraoka, A. Yoshigoe
  • Journal Title: MATERIALS TRANSACTIONS Volume: 57 Issue: 9 Pages: 1609-1614
  • DOI: 10.2320/matertrans.M2016107
  • NAID: 130005289914
  • ISSN: 1345-9678, 1347-5320
  • Peer Reviewed
• [Journal Article] Comprehensive Study and Design of Scaled Metal/High-k/Ge Gate Stacks with Ultrathin Aluminum Oxide Interlayers (2015)
  • Author(s): Ryohei Asahara, Iori Hideshima, Hiroshi Oka, Yuya Minoura, Shingo Ogawa, Akitaka, Yoshigoe, Yuden Teraoka, Takuji Hosoi, Takayoshi Shimura, and Heiji Watanabe
  • Journal Title: Applied Physics Letters Volume: 106 Issue: 23 Pages: 233503-233503
  • DOI: 10.1063/1.4922447
  • Peer Reviewed / Open Access
• [Journal Article] In Situ SR-XPS Observation of Ni-Assisted Low-Temperature Formation of Epitaxial Graphene on 3X-SiC/Si (2015)
  • Author(s): Mika Hasegawa, Kenta Sugawara, Ryota Suto, Shota Sambonsuge, Yuden Teraoka, Akitaka Yoshigoe, Sergey Filimonov, Hirokazu Fukidome, and Maki Suemitsu
  • Journal Title: Nanoscale Research Letter Volume: 10 Issue: 1 Pages: 421-426
  • DOI: 10.1186/s11671-015-1131-9
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Spontaneous activation behavior of Ni3Sn, an intermetallic catalyst, for hydrogen production via methanol decomposition (2015)
  • Author(s): Meiqiang Fan, Ya X, Junya Sakurai, Masahiko Demura, Toshiyuki Hirano, Yuden Teraoka, Akitaka Yoshigoe
  • Journal Title: doi:10.1016/j.ijhydene.2015.05.197 Volume: 4 Issue: 37 Pages: 12663-12673
  • DOI: 10.1016/j.ijhydene.2015.05.197
• [Journal Article] In situ synchrotron radiation photoemission study of ultrathin surface oxides of Ge(111)-c(2 ' 8) induced by supersonic O2 beams (2015)
  • Author(s): Ryuta Okada, Akitaka Yoshigoe, Yuden Teraoka, Yoichi Yamada, and Masahiro Sasaki
  • Journal Title: Appl. Phys. Express Volume: 8 Issue: 2 Pages: 025701-025701
  • DOI: 10.7567/apex.8.025701
  • NAID: 210000137404
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] In-situ synchrotron radiation photoelectron spectroscopy study on oxidation of Ge(100)-2×1 surface by means of supersonic oxygen molecular beam (2014)
  • Author(s): A. Yoshigoe, Y. Teraoka, R. Okada, Y. Yamada, M. Sasaki
  • Journal Title: J. Chem.Phys. Volume: 141 Issue: 17 Pages: 174708-174708
  • DOI: 10.1063/1.4900633
  • Peer Reviewed
• [Journal Article] Synchrotron radiation photoelectron spectroscopy study on oxide evolution during oxidation of a Si(111)-7x7 surface at 300K: Comparison of thermal equilibrium gas and supersonic molecular beams for oxygen adsorption (2014)
  • Author(s): Akitaka Yoshigoe and Yuden Teraoka
  • Journal Title: The Journal of Physical Chemistry C Volume: 118 Issue: 18 Pages: 9436-9442
  • DOI: 10.1021/jp410821r
  • Peer Reviewed
• [Journal Article] Self-accelerating oxidation on Si(111)7×7 surfaces studied by real-time photoelectron spectroscopy (2014)
  • Author(s): J. Tang, K. Nishimoto, S. Ogawa, A. Yoshigoe, S. Ishidzuka, D. Watanabe, Y. Teraoka, and Y. Takakuwa
  • Journal Title: Surface and Interface Analysis Volume: 46 Issue: 12-13 Pages: 1147-1150
  • DOI: 10.1002/sia.5615
  • Peer Reviewed
• [Presentation] 超音速分子ビームによる表面化学反応の放射光光電子分光観察 (2017)
  • Author(s): 吉越章隆
  • Organizer: 第64回応用物理学会春季学術講演会
  • Place of Presentation: パシフィコ横浜（神奈川県、横浜市）
  • Year and Date: 2017-03-14
  • Invited
• [Presentation] 超熱エネルギー酸素分子によるCu3Pt(111)表面の酸化過程 (2017)
  • Author(s): 津田泰孝、牧野隆正、塚田千恵、吉越章隆、福山哲也、岡田美智雄
  • Organizer: 第64回応用物理学会春季学術講演会
  • Place of Presentation: パシフィコ横浜（神奈川県、横浜市）
  • Year and Date: 2017-03-14
• [Presentation] AlGaN表面の熱酸化過程の放射光光電子分光分析 (2017)
  • Author(s): 渡邉 健太, 山田 高寛, 野崎 幹人, 中澤 敏, 志, 施 泓安, 按田 義治, 上田 哲三, 吉越 章隆, 細井 卓治, 志村 考功, 渡部 平司
  • Organizer: 第64回応用物理学会春季学術講演会
  • Place of Presentation: パシフィコ横浜（神奈川県、横浜市）
  • Year and Date: 2017-03-14
• [Presentation] Surface Chemistry Experimental Station at Soft X-ray Beamline (BL23SU) in SPring-8 (2017)
  • Author(s): Akitaka Yoshigoe
  • Organizer: Symposium on Surface Science & Nanotechnology, 25th Anniversary of SSSJ Kansai
  • Place of Presentation: 京都国際会議場（京都府、京都市）
  • Year and Date: 2017-01-24
  • Int'l Joint Research
• [Presentation] In situ synchrotron radiation photoemission study on molecular oxygen adsorbate during room-temperature oxidation of Si(100)2×1 surface (2017)
  • Author(s): Akitaka Yoshigoe
  • Organizer: Symposium on Surface and Nano Science 2017
  • Place of Presentation: 富良野プリンスホテル（北海道、富良野市）
  • Year and Date: 2017-01-11
  • Int'l Joint Research
• [Presentation] Si(100)表面室温酸化中の「分子状吸着酸素」の発見 －放射光が30年来の謎を解く－ (2016)
  • Author(s): 吉越章隆, 多賀稜, 小川修一, 高桑雄二
  • Organizer: 第16回東北大学 多元物質科学研究所 研究発表会
  • Place of Presentation: 東北大（宮城県、仙台市）
  • Year and Date: 2016-12-07
• [Presentation] 超音速分子線を用いたCu(111)表面におけるエチレン分子の反応 (2016)
  • Author(s): 牧野隆正，津田泰孝，塚田千恵，吉越章隆，岡田美智雄
  • Organizer: 2016真空・表面科学合同講演会
  • Place of Presentation: 名古屋国際会議場（愛知県、名古屋市）
  • Year and Date: 2016-11-29
• [Presentation] Cu3Pd(111)合金表面の初期酸化過程 (2016)
  • Author(s): 津田泰孝、牧野隆正、塚田千恵、吉越章隆、福山哲也、岡田美智雄
  • Organizer: 2016年<第77回>応用物理学会秋季学術講演会
  • Place of Presentation: 朱鷺メッセ（新潟県、新潟市）
  • Year and Date: 2016-09-13
• [Presentation] シリコン酸化膜上のグラフェン薄膜の熱的安定性の解析 (2016)
  • Author(s): 小川新，大野真也，吉越章隆
  • Organizer: 2016年<第77回>応用物理学会秋季学術講演会
  • Place of Presentation: 朱鷺メッセ（新潟県、新潟市）
  • Year and Date: 2016-09-13
• [Presentation] 放射光XPS によるSi(100)2×1 へのCH3Cl 吸着反応の研究 (2016)
  • Author(s): 塚田 千恵，吉田 光，岡田 美智雄，吉越 章隆，矢板 毅
  • Organizer: 2016年<第77回>応用物理学会秋季学術講演会
  • Place of Presentation: 朱鷺メッセ（新潟県、新潟市）
  • Year and Date: 2016-09-13
• [Presentation] 熱酸化処理によるSiO2/GaN界面でのGaOx形成とMOS界面特性向上 (2016)
  • Author(s): 山田高寛，渡邉健太，野崎幹人，吉越章隆，細井卓治，志村考功，渡部平司
  • Organizer: 2016年<第77回>応用物理学会秋季学術講演会
  • Place of Presentation: 朱鷺メッセ（新潟県、新潟市）
  • Year and Date: 2016-09-13
• [Presentation] Ge(100)2×1 表面の大気酸化物の放射光光電子分光分析 (2015)
  • Author(s): 吉越章隆, 岡田隆太, 寺岡有殿, 山田洋一, 佐々木正洋
  • Organizer: 2015年真空・表面科学合同講演会、第35回表面科学学術講演会、第56回真空に関する連合講演会
  • Place of Presentation: つくば国際会議場（茨城県、つくば市）
  • Year and Date: 2015-12-01
• [Presentation] Ge(100)2×1 およびGe(111）c(2×8)表面の室温酸化物の放射光光電子分光研究 (2015)
  • Author(s): 吉越章隆, 岡田隆太, 寺岡有殿, 山田洋一, 佐々木正洋
  • Organizer: 2015年真空・表面科学合同講演会、第35回表面科学学術講演会、第56回真空に関する連合講演会
  • Place of Presentation: つくば国際会議場（茨城県、つくば市）
  • Year and Date: 2015-12-01
• [Presentation] 低速電子回折と電子分光法によるHf 蒸着Si(110)-16×2 シングルドメイン表面の研究 (2015)
  • Author(s): 垣内拓大, 桂木拓磨, 中納佑二, 吉越章隆, 長岡伸一, 間瀬一彦
  • Organizer: 2015年真空・表面科学合同講演会、第35回表面科学学術講演会、第56回真空に関する連合講演会
  • Place of Presentation: つくば国際会議場（茨城県、つくば市）
  • Year and Date: 2015-12-01
• [Presentation] 超音速分子線を用いて酸化したSi(113)表面の電子状態解析 (2015)
  • Author(s): 田中一馬, 大野真也, 小玉開, 吉越章隆， 寺岡有殿, 田中正俊
  • Organizer: 2015年真空・表面科学合同講演会、第35回表面科学学術講演会、第56回真空に関する連合講演会
  • Place of Presentation: つくば国際会議場（茨城県、つくば市）
  • Year and Date: 2015-12-01
• [Presentation] Rapid Temperature Oxidation at SiO2/Si(001) Interface Studied by Real-time X-ray photoelectron spectroscopy: Rapid Cooling Versus Rapid Heating (2015)
  • Author(s): Jiayi Tang, Shuichi Ogawa, Akitaka Yoshigoe, Shinji Ishidzuka, Yuji Takakuwa
  • Organizer: 2015 International Workshop on DIELECTRIC THIN FILMS FOR FUTURE ELECTRON DEVICES: SCIENCE AND TECHNOLOGY (2015 IWDTF)
  • Place of Presentation: 未来館（東京都、江東区）
  • Year and Date: 2015-11-02
• [Presentation] Synchrotron radiation photoemission study of oxides at Ge(100) surface after atmospheric exposure (2015)
  • Author(s): Akitaka Yoshigoe, Ryuta Okada, Yuden Teraoka, Yoichi Ymada, and Masahiro Sasaki
  • Organizer: 10th International Symposium on Atomic Level Characterizations for New Materials and Devices ’15 (ALC’15)
  • Place of Presentation: くにびきメッセ（島根県、松江市）
  • Year and Date: 2015-10-25
• [Presentation] Strain-induced Reaction Kinetics of O2 Molecule at SiO2/Si Interfaces studied by Real-time X-ray Photoelectron Spectroscopy (2015)
  • Author(s): Jiayi Tang, Shuichi Ogawa, Akitaka Yoshigoe, Shinji Ishidzuka, Yuji Takakuwa
  • Organizer: 0th International Symposium on Atomic Level Characterizations for New Materials and Devices ’15 (ALC’15)
  • Place of Presentation: くにびきメッセ（島根県、松江市）
  • Year and Date: 2015-10-25
• [Presentation] Strain-induced oxide decomposition at SiO2/Si(001) and SiO2/Si(111) interfaces studied by X-ray photoelectron spectroscopy and scanning tunnelling microscopy (2015)
  • Author(s): Jiay Tang, Shuichi Ogawa, Akitaka Yoshigoe, Yuden Teraoka, Yuji Takakuwa
  • Organizer: European Conference on Surface Science-31
  • Place of Presentation: Barcelona(Spain)
  • Year and Date: 2015-08-31
• [Presentation] 放射光リアルタイム光電子分光を用いたシリコン表面反応ダイナミクスの研究 (2015)
  • Author(s): 吉越章隆
  • Organizer: The 9th Hydrogen Materials Unit Seminar
  • Place of Presentation: NIMS(茨城県、つくば市)
  • Year and Date: 2015-07-31
  • Invited
• [Presentation] Synchrotron radiation photoelectron spectroscopy study of room-temperature oxidation of Ge(100)2×1 surface using pure O2 gas (2015)
  • Author(s): A. Yoshigoe, R. Okada, Y. Teraoka, Y. Yamada, M. Sasaki
  • Organizer: Symposium on Surface and Nano Science 2015 (SSNS'15)
  • Place of Presentation: 新富良野プリンスホテル（北海道富良野市）
  • Year and Date: 2015-01-14 – 2015-01-18
• [Presentation] Synchrotron radiation photoelectron spectroscopy study on surface oxidation of Ge(100) and Ge(111) at room temperture (2014)
  • Author(s): Akitaka Yoshigoe, R. Okada, Y. Teraoka, Y. Yamada, M. Sasak
  • Organizer: Pacific Rim Symposium on Surfaces, Coatings & Interfaces (PacSurf 2014)
  • Place of Presentation: Kohala Coast, Hawaii, USA
  • Year and Date: 2014-12-07 – 2014-12-11
• [Presentation] Sub-monolayer oxides on Ge(100) surface fabricated with pure O2 gas (2014)
  • Author(s): Akitaka Yoshigoe, Ryuta Okada, Yuden Teraoka, Yoichi Yamada and Masahiro Sasaki
  • Organizer: The 2nd International Symposium on the Functionality of organized Nanostructures (FON'14)
  • Place of Presentation: 日本科学未来館（東京都江東区）
  • Year and Date: 2014-11-27 – 2014-11-28
• [Presentation] Synchrotron Radiation Photoelectron Spectroscopy Study on Surface Oxides at Ge(100)-2×1 Surface (2014)
  • Author(s): Akitaka Yoshigoe, Ryuta Okada, Yuden Teraoka, Yutaro Iwai, Yoichi Yamada, Masahiro Sasak
  • Organizer: The 7th International Symposium on Surface Science (ISSS-7)
  • Place of Presentation: 松江くにびきメッセ（島根県松江市）
  • Year and Date: 2014-11-02 – 2014-11-06
• [Presentation] Si(100)-2×1表面の分子状吸着状態の放射光リアルタイム光電子分光による時分割観察 (2014)
  • Author(s): 吉越章隆、岡田隆太、寺岡有殿、岩井優太郎、山田洋一、佐々木正洋
  • Organizer: 2014年第75回応用物理学会秋季学術講演会
  • Place of Presentation: 北海道大学、札幌キャンパス(札幌市)
  • Year and Date: 2014-09-17 – 2014-09-20
• [Presentation] Ge(111)-c(2×8)表面の酸化発展のO2並進エネルギー依存性 (2014)
  • Author(s): 岡田隆太、吉越章隆、寺岡有殿、岩井優太郎、山田洋一、佐々木正洋
  • Organizer: 2014年第75回応用物理学会秋季学術講演会
  • Place of Presentation: 北海道大学、札幌キャンパス（札幌市）
  • Year and Date: 2014-09-17 – 2014-09-20
• [Presentation] Temperature Dependence of Oxidation Reacation Paths on Si(111)7×7 Studied by Real-time Photoelectron Spectroscopy and Theoretical Calculations (2014)
  • Author(s): Jiayi Tang, Shuichi Ogawa, Akitaka Yoshigoe, Kiwamu Nishimoto, Shinnji Ishidzuka, Yuden Teraoka, and Yuji Takakuwa
  • Organizer: 30th European Conference on Surface Science
  • Place of Presentation: Antalya, Turkey
  • Year and Date: 2014-08-31 – 2014-09-05