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2019 Fiscal Year Annual Research Report

Development of real space charge density mapping method using atomic-resolution DPC STEM and its application to material interfaces

Research Project

Project/Area Number 17H01316
Research InstitutionThe University of Tokyo

Principal Investigator

柴田 直哉  東京大学, 大学院工学系研究科(工学部), 教授 (10376501)

Co-Investigator(Kenkyū-buntansha) 石川 亮  東京大学, 大学院工学系研究科(工学部), 助教 (20734156)
Project Period (FY) 2017-04-01 – 2020-03-31
Keywords走査型透過電子顕微鏡 / 材料界面 / 電荷密度 / 微分位相コントラスト法
Outline of Annual Research Achievements

本研究では、申請者らが近年開発した原子分解能DPC STEM法をベースとして、材料局所領域の電荷密度分布を原子レベルで実空間マッピングするための新たな電子顕微鏡法を開発する。更に、この手法を無機材料界面構造解析に応用することで、異種結晶間の界面形成メカニズムを原子・電子スケールから本質的に明らかにすることを最終的な目標としている。

本年度は、実際の試料膜厚を想定した動力学的回折効果を加味した原子電場・電荷密度分布の理論計算解析を行い、その効果が像解釈に及ぼす影響の検証を系統的に行った。ここで得られた知見を基に、CTF理論とマルチスライス計算に基づいた反復的計算を行うことにより動力学的回折効果を除去する手法の開発を行った。その結果、10nm程度の試料厚の結晶では動力学回折効果の影響を除去でき、定量的な電場・電荷密度分布解析が可能であることを示した。また、原子分解能DPC STEMからの局所電磁場情報を電荷密度分布に変換するオペレーションソフトを実装し、電荷密度分布のライブイメージングを可能にした。この像観察により、像非点やフォーカスなど光軸条件の更なる精密調整が可能になるという副次的なメリットも生まれた。また、GaN系半導体モデルヘテロ界面において本手法を応用し、界面における電荷移動に伴う電場分布観察に成功した。更に、これまでの研究結果を総括し、原子レベルでの電場分布及び電荷密度分布直接観察手法としてDPC STEM法を確立し、界面解析への有効性を示すことにも成功した。

Research Progress Status

令和元年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和元年度が最終年度であるため、記入しない。

  • Research Products

    (52 results)

All 2020 2019 Other

All Int'l Joint Research (1 results) Journal Article (26 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 26 results,  Open Access: 3 results) Presentation (24 results) (of which Int'l Joint Research: 14 results,  Invited: 21 results) Remarks (1 results)

  • [Int'l Joint Research] Monash University(オーストラリア)

    • Country Name
      AUSTRALIA
    • Counterpart Institution
      Monash University
  • [Journal Article] Grain boundary Li-ion conductivity in (Li0.33La0.56)TiO3 polycrystal2020

    • Author(s)
      Shun Sasano, Ryo Ishikawa, Kazuaki Kawahara, Teiichi Kimura, Yumi H. Ikuhara, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Applied Physics Letters

      Volume: 116 Pages: 43901

    • DOI

      10.1063/1.5141396

    • Peer Reviewed
  • [Journal Article] Direct Measurement of Electronic Band Structures at Oxide Grain Boundaries.2020

    • Author(s)
      Jiake Wei, Takafumi Ogawa, Bin Feng, Tatsuya Yokoi, Ryo Ishikawa, Akihide Kuwabara, Katsuyuki Matsunaga, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Nano letters

      Volume: 20 Pages: 2530-2536

    • DOI

      10.1021/acs.nanolett.9b05298

    • Peer Reviewed
  • [Journal Article] Coexistence of two different atomic structures in the Σ13 pyramidal twin boundary in α-Al2O32019

    • Author(s)
      Naoya Shibata
    • Journal Title

      Journal of the Ceramic Society of Japan

      Volume: 127 Pages: 708-714

    • DOI

      Rr10.2109/jcersj2.19118

    • Peer Reviewed
  • [Journal Article] Oxysulfide photocatalyst for visible-light-driven overall water splitting2019

    • Author(s)
      Qian Wang, Mamiko Nakabayashi, Takashi Hisatomi, Song Sun, Seiji Akiyama, Zheng Wang, Zhenhua Pan, Xiong Xiao, Tomoaki Watanabe, Taro Yamada, Naoya Shibata, Tsuyoshi Takata, Kazunari Domen
    • Journal Title

      Nature Materials

      Volume: 18 Pages: 827-832

    • DOI

      10.1038/s41563-019-0399-z

    • Peer Reviewed
  • [Journal Article] Atomic Scale Origin of Enhanced Ionic Conductivity at Crystal Defects.2019

    • Author(s)
      Bin Feng, Ryo Ishikawa, Akihito Kumamoto, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Nano letters

      Volume: 19 Pages: 2162-2186

    • DOI

      10.1021/acs.nanolett.9b00506

    • Peer Reviewed
  • [Journal Article] Efficient hydrogen evolution on (CuInS2)x(ZnS)1-x solid solution-based photocathodes under simulated sunlight.2019

    • Author(s)
      Jiao Zhao, Tsutomu Minegishi, Hiroyuki Kaneko, Guijun Ma, Miao Zhong, Mamiko Nakabayashi, Takashi Hisatomi, Masao Katayama, Naoya Shibata, Taro Yamada, Kazunari Domen
    • Journal Title

      Chemical communications (Cambridge, England)

      Volume: 55 Pages: 470-473

    • DOI

      10.1039/c8cc08623k

    • Peer Reviewed
  • [Journal Article] Direct observation of atomic-scale fracture path within ceramic grain boundary core.2019

    • Author(s)
      Shun Kondo, Akihito Ishihara, Eita Tochigi, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Nature communications

      Volume: 10 Pages: 2112

    • DOI

      10.1038/s41467-019-10183-3

    • Peer Reviewed / Open Access
  • [Journal Article] Transition-Metal Distribution in Brownmillerite Ca2FeCoO5.2019

    • Author(s)
      Kei Nakayama, Ryo Ishikawa, Akihide Kuwabara, Shunsuke Kobayashi, Teruki Motohashi, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Inorganic chemistry

      Volume: 58 Pages: 10209

    • DOI

      10.1021/acs.inorgchem.9b01356

    • Peer Reviewed
  • [Journal Article] High contrast STEM imaging for light elements by an annular segmented detector.2019

    • Author(s)
      Kousuke Ooe, Takehito Seki, Yuichi Ikuhara, Naoya Shibata
    • Journal Title

      Ultramicroscopy

      Volume: 202 Pages: 148-155

    • DOI

      10.1016/j.ultramic.2019.04.011

    • Peer Reviewed
  • [Journal Article] Redox-Inactive CO2 Determines Atmospheric Stability of Electrical Properties of ZnO Nanowire Devices through a Room-Temperature Surface Reaction.2019

    • Author(s)
      Kentaro Nakamura, Tsunaki Takahashi, Takuro Hosomi, Takehito Seki, Masaki Kanai, Guozhu Zhang, Kazuki Nagashima, Naoya Shibata, Takeshi Yanagida
    • Journal Title

      ACS applied materials & interfaces

      Volume: 11 Pages: 40260-40266

    • DOI

      10.1021/acsami.9b13231

    • Peer Reviewed
  • [Journal Article] Atomic-Resolution Stem Imaging for Beam-Sensitive Li-Ion Battery Materials2019

    • Author(s)
      K. Nakayama, R. Ishikawa, S. Kobayashi, N. Shibata, Y. Ikuhara
    • Journal Title

      AMTC Letters

      Volume: 6 Pages: 18-19

    • DOI

      -

    • Peer Reviewed
  • [Journal Article] Upscaling of Temperature-Sensitive Particle Photocatalyst Electrodes: Fully Ambient and Scalable Roll-Press Fabrication of Ta3N5 Photoelectrodes on Metal Substrate2019

    • Author(s)
      Xiong Xiao, Motoki Iwase, Ge Yin, Mamiko Nakabayashi, Tomohiro Higashi, Naoya Shibata, Kazunari Domen, Tomoaki Watanabe
    • Journal Title

      ACS Sustainable Chemistry and Engineering

      Volume: 7 Pages: 19407-19414

    • DOI

      10.1021/acssuschemeng.9b03987

    • Peer Reviewed
  • [Journal Article] Metal selenide photocatalysts for visible-light-driven Z-scheme pure water splitting2019

    • Author(s)
      Shanshan Chen, Guijun Ma, Qian Wang, Song Sun, Takashi Hisatomi, Tomohiro Higashi, Zheng Wang, Mamiko Nakabayashi, Naoya Shibata, Zhenhua Pan, Toshio Hayashi, Tsutomu Minegishi, Tsuyoshi Takata, Kazunari Domen
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 7 Pages: 7415-7422

    • DOI

      10.1039/C9TA00768G

    • Peer Reviewed
  • [Journal Article] Defect-Rich NiCeOx Electrocatalyst with Ultrahigh Stability and Low Overpotential for Water Oxidation2019

    • Author(s)
      Jun Yu, Qi Cao, Yanbo Li, Xia Long, Shihe Yang, J. Kenji Clark, Mamiko Nakabayashi, Naoya Shibata, Jean Jacques Delaunay
    • Journal Title

      ACS Catalysis

      Volume: 9 Pages: 1605-1611

    • DOI

      10.1021/acscatal.9b00191

    • Peer Reviewed
  • [Journal Article] The effects of annealing barium niobium oxynitride in argon on photoelectrochemical water oxidation activity2019

    • Author(s)
      Jeongsuk Seo, Mamiko Nakabayashi, Takashi Hisatomi, Naoya Shibata, Tsutomu Minegishi, Masao Katayama, Kazunari Domen
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 7 Pages: 493-502

    • DOI

      10.1039/c8ta09950b

    • Peer Reviewed
  • [Journal Article] Atomic resolution electron microscopy in a magnetic field free environment2019

    • Author(s)
      N. Shibata, Y. Kohno, A. Nakamura, S. Morishita, T. Seki, A. Kumamoto, H. Sawada, T. Matsumoto, S. D. Findlay, Y. Ikuhara
    • Journal Title

      Nature Communications

      Volume: 10 Pages: 2308

    • DOI

      10.1038/s41467-019-10281-2

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Fast Li-ion conduction at grain boundaries in (La,Li)NbO3 polycrystals2019

    • Author(s)
      Kazuaki Kawahara, Ryo Ishikawa, Kei Nakayama, Takuma Higashi, Teiichi Kimura, Yumi H. Ikuhara, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Journal of Power Sources

      Volume: 441 Pages: 227187

    • DOI

      10.1016/j.jpowsour.2019.227187

    • Peer Reviewed
  • [Journal Article] Sunlight-Driven Production of Methylcyclohexane from Water and Toluene Using ZnSe : Cu(In,Ga)Se2-Based Photocathode2019

    • Author(s)
      Yosuke Kageshima, Yosuke Goto, Hiroyuki Kaneko, Mamiko Nakabayashi, Naoya Shibata, Kazunari Domen, Tsutomu Minegishi
    • Journal Title

      ChemCatChem

      Volume: 11 Pages: 4266-4271

    • DOI

      10.1002/cctc.201900739

    • Peer Reviewed
  • [Journal Article] Solar-Driven Water Splitting over a BaTaO2N Photoanode Enhanced by Annealing in Argon2019

    • Author(s)
      Jeongsuk Seo, Mamiko Nakabayashi, Takashi Hisatomi, Naoya Shibata, Tsutomu Minegishi, Kazunari Domen
    • Journal Title

      ACS Applied Energy Materials

      Volume: 2 Pages: 5777-5784

    • DOI

      10.1021/acsaem.9b00908

    • Peer Reviewed
  • [Journal Article] One-dimensional Anisotropic Electronic States in Needle-shaped La 5 Ti 2 CuS 5 O 7 Single Crystals Grown in Molten Salt in Bridgman Furnace2019

    • Author(s)
      Motoki Iwase, Mamiko Nakabayashi, Naoya Shibata, Hiroyuki Matsuzaki, Hisayoshi Kobayashi, Taro Yamada, Kazunari Domen, Tomoaki Watanabe
    • Journal Title

      Crystal Growth and Design

      Volume: 19 Pages: 2419-2427

    • DOI

      10.1021/acs.cgd.9b00091

    • Peer Reviewed
  • [Journal Article] Coexistence of two different atomic structures in the Σ13 pyramidal twin boundary in α-Al2O32019

    • Author(s)
      Saki Ishihara, Eita Tochigi, Ryo Ishikawa, Naoya Shibata, Yuichi Ikuhara
    • Journal Title

      Philosophical Magazine Letters

      Volume: 99 Pages: 435-443

    • DOI

      10.1080/09500839.2019.1698780

    • Peer Reviewed
  • [Journal Article] 先進原子分解能電子顕微鏡による材料局所構造解析2019

    • Author(s)
      柴田直哉
    • Journal Title

      日本原子力学会誌

      Volume: 61 Pages: 24-27

    • DOI

      10.3327/jaesjb.61.10_724

    • Peer Reviewed
  • [Journal Article] DPC STEMの原理と応用2019

    • Author(s)
      柴田直哉
    • Journal Title

      顕微鏡

      Volume: 54 Pages: 77-84

    • DOI

      10.11410/kenbikyo.54.2_77

    • Peer Reviewed
  • [Journal Article] DPC STEMによる局所電磁場の直接観察2019

    • Author(s)
      柴田直哉
    • Journal Title

      まてりあ

      Volume: 58 Pages: 433ー439

    • DOI

      10.2320/materia.58.433

    • Peer Reviewed
  • [Journal Article] グラフェン欠陥の原子電場構造解析2019

    • Author(s)
      石川亮 柴田直哉 幾原雄一
    • Journal Title

      日本結晶学会誌

      Volume: 61 Pages: 231-236

    • DOI

      10.5940/jcrsj.61.231

    • Peer Reviewed / Open Access
  • [Journal Article] Anisotropic Atomic Electric Fields of Si Dopants in Monolayer Graphene2019

    • Author(s)
      R. Ishikawa S.D. Findlay T. Seki G. Sanchez-Santolino Y. Kohno Y. Ikuhara N. Shibata
    • Journal Title

      AMTC Letters

      Volume: 6 Pages: 22-23

    • DOI

      -

    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 先進DPC STEM法による材料局所構造解析2020

    • Author(s)
      柴田 直哉
    • Organizer
      ASTEC2020
    • Invited
  • [Presentation] Atomic-scale chemical analysis at ceramic interfaces by advanced scanning transmission electron microscopy2019

    • Author(s)
      N. Shibata
    • Organizer
      MRS spring meeting 2019
    • Int'l Joint Research / Invited
  • [Presentation] Seeing inside atoms Beyond atomic resolution electron microscopy2019

    • Author(s)
      N. Shibata
    • Organizer
      INCP 2019
    • Int'l Joint Research / Invited
  • [Presentation] Advanced atomic-resolution STEM for real-space electromagnetic field imaging2019

    • Author(s)
      N. Shibata
    • Organizer
      KSM annual meeting
    • Int'l Joint Research / Invited
  • [Presentation] Advanced DPC STEM for materials research2019

    • Author(s)
      N. Shibata
    • Organizer
      AMTC6
    • Int'l Joint Research / Invited
  • [Presentation] Towards sub-atomic resolution electron microscopy2019

    • Author(s)
      N. Shibata
    • Organizer
      German-Japan Joint Seminar on Advanced Electron Microscopy and Its Application
    • Int'l Joint Research / Invited
  • [Presentation] Magnetic-field-free atomic resolution STEM2019

    • Author(s)
      N. Shibata
    • Organizer
      NEXTEM, Pre-meeting congress, Microscopy & Microanalysis 2019
    • Int'l Joint Research / Invited
  • [Presentation] Differential phase contrast scanning transmission electron microscopy at atomic resolution2019

    • Author(s)
      N. Shibata
    • Organizer
      Microscopy & Microanalysis 2019
    • Int'l Joint Research / Invited
  • [Presentation] Advanced electron microscopy for atomic-scale electromagnetic field imaging2019

    • Author(s)
      N. Shibata
    • Organizer
      ALC 19
    • Int'l Joint Research / Invited
  • [Presentation] Development of magnetic field free atomic-resolution STEM2019

    • Author(s)
      N. Shibata
    • Organizer
      PACRIM 13
    • Int'l Joint Research / Invited
  • [Presentation] Development and application of electromagnetic field imaging STEM2019

    • Author(s)
      N. Shibata
    • Organizer
      PACRIM 13
    • Int'l Joint Research / Invited
  • [Presentation] Atomic-resolution electromagnetic field imaging by DPC STEM2019

    • Author(s)
      N. Shibata
    • Organizer
      FEMMS2019
    • Int'l Joint Research / Invited
  • [Presentation] Advanced atomic resolution STEM for electromagnetic field imaging2019

    • Author(s)
      N. Shibata
    • Organizer
      ICAE 2019
    • Int'l Joint Research / Invited
  • [Presentation] 最先端STEMによる材料局所構造解析2019

    • Author(s)
      柴田 直哉
    • Organizer
      日立金属セミナー
    • Invited
  • [Presentation] 原子分解能磁場フリー電子顕微鏡(MARS)の開発と応用2019

    • Author(s)
      柴田 直哉
    • Organizer
      日本顕微鏡学会第75回学術講演会
    • Invited
  • [Presentation] 電子顕微鏡の挑戦 -原子分解能の先へ-2019

    • Author(s)
      柴田 直哉
    • Organizer
      日立ハイテクノロジーズセミナー
    • Invited
  • [Presentation] DPC STEM法による材料局所電磁場解析2019

    • Author(s)
      柴田 直哉
    • Organizer
      日本金属学会2019年秋期大会
    • Invited
  • [Presentation] 先進原子分解能STEMの開発と材料局所構造解析2019

    • Author(s)
      柴田 直哉
    • Organizer
      日本セラミックス協会関西支部第22回若手フォーラム
    • Invited
  • [Presentation] DPC STEM法の基礎と応用2019

    • Author(s)
      柴田 直哉
    • Organizer
      第12回日本電子TEMユーザーズミーティング
    • Invited
  • [Presentation] 原子分解能電磁場計測電子顕微鏡法の開発と応用2019

    • Author(s)
      柴田 直哉
    • Organizer
      第61回日本顕微鏡学会九州支部総会・学術講演会
    • Invited
  • [Presentation] 原子分解能電子顕微鏡によるセラミックス材料の構造解析2019

    • Author(s)
      石川 亮
    • Organizer
      2019年度エンジニアリングセラミックス若手セミナー
    • Invited
  • [Presentation] グラフェン欠陥における電場構造解析2019

    • Author(s)
      石川 亮 Findlay Scott 関 岳人 Sanchez-Santolino Gabriel 河野 祐二 幾原 雄一 柴田 直哉
    • Organizer
      日本金属学会165回講演大会
  • [Presentation] Anisotropic Atomic Electric Fields of Si Dopants in Monolayer Graphene2019

    • Author(s)
      R. Ishikawa S.D. Findlay T. Seki G. Sanchez-Santolino Y. Kohno Y. Ikuhara N. Shibata
    • Organizer
      AMTC6
    • Int'l Joint Research
  • [Presentation] Direct Electric field imaging of atomistic defects in graphene2019

    • Author(s)
      R. Ishikawa S.D. Findlay T. Seki G. Sanchez-Santolino Y. Kohno Y. Ikuhara N. Shibata
    • Organizer
      FEMMS2019
    • Int'l Joint Research
  • [Remarks] 電子顕微鏡材料学研究室

    • URL

      http://www.saaf.t.u-tokyo.ac.jp/

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Published: 2021-01-27  

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