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2018 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走査透過型電子顕微鏡法 / 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、原子分解能DPC STEMの定量観察により、原子電場を定量的に可視化し、その情報から原子スケールの電荷密度分布の直接観察が可能かどうか、実験及び理論計算を用いて検証した。その前段階として、ノイズを加味した解析を行い、ノイズを取り入れた像理論を構築し、原子分解能DPC STEM法と他の手法を比較し、その優位性の検証に成功した。モデル試料としてGaN結晶を用いて、その原子電場像から電荷密度分布像を形成した。その結果、原子中心の正電荷を持つ原子核と負電荷をもつ電子雲の実空間観察に成功した。結合を担う電子に関しても原理的には観察が可能になると考えられるが、現状では分解能、装置安定性、検出器感度などの問題で今後の課題になると考えられる。更に、DCT法を用いたポテンシャル再生なども可能になり、試料が十分薄い条件では、原子レベルのポテンシャル、電荷密度分布観察が可能であると考えられる。その真価を検証するため、グラフェンの原子電場直接観察を試みた。その結果、単原子レイヤーであるグラフェンの原子周囲の電場分布を直接観察することに成功し、その空間分布、強度が原子の配位環境、すなわち結合と密接関連すること示唆された。更に、酸化物の清浄表面に貴金属ナノクラスターを形成する技術を構築し、モデル的な金属微粒子/セラミックス界面の作製に成功した。

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

平成30年度は①原子分解能DPC STEM法による原子電場定量解析手法の確立、②原子分解能DPC STEM法による局所電荷密度分布直接観察法の開発、③原子分解能 DPC STEM法の像形成理論解析、④モデル界面作製と原子分解能DPC STEM構造解析を並行して行い、いずれの項目についても一定の成果を得ることができた。特に、①、②、③に関してはハイインパクトな論文発表も行っており、計画以上に進んでいる。④に関しては、試料作製が確立しつつあるため、来年度の界面観察に応用する予定である。

Strategy for Future Research Activity

来年度は、引き続き各研究を鋭意推進するとともに、最終年度にあたりこれまでの成果を取り纏め、原子分解能DPC STEMに基づく実空間電荷密度マッピング法を確立し、材料応用展開は進めていく。得られた知見に関しては、適宜論文、学会発表などで外部報告する予定である。

  • Research Products

    (44 results)

All 2019 2018 Other

All Int'l Joint Research (1 results) Journal Article (17 results) (of which Int'l Joint Research: 8 results,  Peer Reviewed: 17 results,  Open Access: 2 results) Presentation (26 results) (of which Int'l Joint Research: 16 results,  Invited: 23 results)

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

    • Country Name
      AUSTRALIA
    • Counterpart Institution
      Monash University
  • [Journal Article] Large angle illumination enabling accurate structure reconstruction from thick samples in scanning transmission electron microscopy2019

    • Author(s)
      H. G. Brown R. Ishikawa G. Sanchez-Santolino N. Shibata Y. Ikuhara L. J. Allen S. D. Findlay
    • Journal Title

      Ultramicroscopy

      Volume: 197 Pages: 112-121

    • DOI

      10.1016/j.ultramic.2018.12.010

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Thin-film stabilization of LiNbO3-type ZnSnO3 and MgSnO3 by molecular-beam epitaxy2019

    • Author(s)
      K. Fujiwara, H. Minato, J. Shiogai, A. Kumamoto, N. Shibata and A. Tsukazaki
    • Journal Title

      APL Materials

      Volume: 7 Pages: 22505

    • DOI

      10.1063/1.5054289

    • Peer Reviewed
  • [Journal Article] Atomic-scale origin of enhanced ionic conductivity at crystal defects2019

    • Author(s)
      B. Feng, R. Ishikawa, A. Kumamoto, N. Shibata and Y. Ikuhara
    • Journal Title

      Nano Letters

      Volume: 19 Pages: 2162?2168

    • DOI

      10.1021/acs.nanolett.9b00506

    • Peer Reviewed
  • [Journal Article] The core structure of 60 degrees mixed basal dislocation in alumina (alpha-Al2O3) introduced by in situ TEM nanoindentation2019

    • Author(s)
      B. Miao, S. Kondo, E. Tochigi, J.K. Wei, B. Feng, N. Shibata and Y. Ikuhara
    • Journal Title

      Scripta Materialia

      Volume: 163 Pages: 157-162

    • DOI

      10.1016/j.scriptamat.2019.01.011

    • Peer Reviewed
  • [Journal Article] Unusual Oxygen Partial Pressure Dependence of Electrical Transport of Single-Crystalline Metal Oxide Nanowires Grown by the Vapor?Liquid?Solid Process2019

    • Author(s)
      H. Anzai, T. Takahashi, M. Suzuki, M. Kanai, G. Zhang, T. Hosomi, T. Seki, K. Nagashima, N. Shibata and T. Yanagida
    • Journal Title

      Nano Letters

      Volume: 19 Pages: 1675-1681

    • DOI

      10.1021/acs.nanolett.8b04668

    • Peer Reviewed
  • [Journal Article] Probing the Internal Atomic Charge Density Distributions in Real Space2018

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

      ACS Nano

      Volume: 12 Pages: 8875-8881

    • DOI

      10.1021/acsnano.8b03712

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Direct electric field imaging of graphene defects2018

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

      Nature Communications

      Volume: 9 Pages: 3878

    • DOI

      10.1038/s41467-018-06387-8

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Atomic-Scale Structure Relaxation, Chemistry and Charge Distribution of Dislocation Cores in SrTiO32018

    • Author(s)
      P. Gao, R. Ishikawa, B. Feng, A. Kumamoto, N. Shibata and Y. Ikuhara
    • Journal Title

      Ultramicroscopy

      Volume: 184 Pages: 217-224

    • DOI

      10.1016/j.ultramic.2017.09.006

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effects of an oxygen potential gradient and water vapor on mass transfer in polycrystalline alumina at high temperatures2018

    • Author(s)
      T. Matsudaira, S. Kitaoka, N. Shibata, Y. Ikuhara, M. Takeuchi and T. Ogawa
    • Journal Title

      Acta materialia

      Volume: 151 Pages: 21-30

    • DOI

      10.1016/j.actamat.2018.03.021

    • Peer Reviewed
  • [Journal Article] Probing the limits of the rigid-intensity-shift model in differential-phase-contrast scanning transmission electron microscopy2018

    • Author(s)
      L. Clark, H. G. Brown, D. M. Paganin, M. J. Morgan, T. Matsumoto, N. Shibata, T. C. Petersen, and S. D. Findlay
    • Journal Title

      Physical Review A

      Volume: 97 Pages: 43843

    • DOI

      10.1103/PhysRevA.97.043843

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Inversion domain network stabilization and spinel phase suppression in ZnO2018

    • Author(s)
      J. Hoemke, E. Tochigi, T. Tohei, H. Yoshida, N. Shibata, Y. Ikuhara and Y. Sakka
    • Journal Title

      Journal of American Ceramic Society

      Volume: 101 Pages: 2616-2626

    • DOI

      10.1111/jace.15426

    • Peer Reviewed
  • [Journal Article] On the quantitativeness of grain boundary chemistry using STEM EDS: A ZrO2 Σ9 model grain boundary case study2018

    • Author(s)
      B. Feng, N.R. Lugg, A. Kumamoto, N. Shibata and Y. Ikuhara
    • Journal Title

      Ultramicoscopy

      Volume: 193 Pages: 33-38

    • DOI

      10.1016/j.ultramic.2018.05.010

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Theoretical framework of statistical noise in scanning transmission electron microscopy2018

    • Author(s)
      T. Seki, Y. Ikuhara and N. Shibata
    • Journal Title

      Ultramicoscopy

      Volume: 193 Pages: 118-125

    • DOI

      10.1016/j.ultramic.2018.06.014

    • Peer Reviewed
  • [Journal Article] Influence of Dislocations in Transition Metal Oxides on Selected Physical and Chemical Properties2018

    • Author(s)
      K. Szot, C. Rodenbucher, G. Bihlmayer, W. Speier, R. Ishikawa, N. Shibata and Y. Ikuhara
    • Journal Title

      Crystals

      Volume: 8 Pages: 241

    • DOI

      10.3390/cryst8060241

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Atomic-scale measurement of flexoelectric polarization at SrTiO3 dislocations2018

    • Author(s)
      P. Gao, S. Yang, R. Ishikawa, N. Li, B. Feng, A. Kumamoto, N. Shibata, P. Yu and Y. Ikuhara
    • Journal Title

      Physical Review Letters

      Volume: 120 Pages: 267601

    • DOI

      10.1103/PhysRevLett.120.267601

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Accurate measurement of electric potentials in biased GaAs compound semiconductors by phase-shifting electron holography2018

    • Author(s)
      S. Anada, K. Yamamoto, H. Sasaki, N. Shibata, M. Matsumoto, Y. Hori, K. Kinugawa, A. Imamura and T. Hirayama
    • Journal Title

      Microscopy

      Volume: 68 Pages: 159-166

    • DOI

      10.1093/jmicro/dfy131

    • Peer Reviewed
  • [Journal Article] 原子内部電場の直接観察2018

    • Author(s)
      柴田直哉
    • Journal Title

      応用物理

      Volume: 87 Pages: 828-832

    • Peer Reviewed
  • [Presentation] Electric field imaging of atomistic defects in graphene2019

    • Author(s)
      R. Ishikawa S. Findlay T. Seki G. Sanchez-Santolino Y. Kohno Y. Ikuhara N. Shibata
    • Organizer
      International Workshop of Ultra High-Resolution on Microscopy 2019
    • Int'l Joint Research
  • [Presentation] グラフェン欠陥における原子分解能電場解析2019

    • Author(s)
      石川亮 S. Findlay 関岳人 G. Sanchez-Santolino 河野祐二 幾原雄一 柴田直哉
    • Organizer
      日本セラミックス協会 2019年 年会
  • [Presentation] 先端電子顕微鏡法による材料の局所構造解析2019

    • Author(s)
      石川亮
    • Organizer
      第2回情報計測インフォマティクス
    • Invited
  • [Presentation] Towards subatomic-resolution electron microscopy ?Can we observe inside of atoms?-2019

    • Author(s)
      N. Shibata
    • Organizer
      International workshop of ultra high-resolution on microscopy
    • Int'l Joint Research / Invited
  • [Presentation] 先進原子分解能電子顕微鏡による電磁場観察の現状と展望2019

    • Author(s)
      柴田直哉
    • Organizer
      第4回分析TEMユーザーズミーティング
    • Invited
  • [Presentation] 先進原子分解能電子顕微鏡による材料局所電磁場解析2019

    • Author(s)
      柴田直哉
    • Organizer
      日本原子力学会 2019年春の年会
    • Invited
  • [Presentation] 原子分解能電磁場計測電子顕微鏡の開発と材料界面研究(学術賞受賞講演)2019

    • Author(s)
      柴田直哉
    • Organizer
      日本セラミックス協会2019年年会
    • Invited
  • [Presentation] Direct electromagnetic field imaging in materials and devices by DPC STEM2019

    • Author(s)
      N. Shibata
    • Organizer
      MST 36
    • Int'l Joint Research / Invited
  • [Presentation] Advanced electron microscopy for spinel related materials2018

    • Author(s)
      R. Ishikawa
    • Organizer
      9th International Workshop on Spinel Nitrides and Related Materials
    • Int'l Joint Research / Invited
  • [Presentation] Surface and Electric Field Imaging by Newly Designed Atomic-Resolution STEM2018

    • Author(s)
      R. Ishikawa N. Shibata Y. Ikuhara
    • Organizer
      Microscopy & Microanalysis 2018
    • Int'l Joint Research / Invited
  • [Presentation] グラフェン欠陥における原子分解能電場観察2018

    • Author(s)
      石川亮 S. Findlay 関岳人 G. Sanchez-Santolino 河野祐二 幾原雄一 柴田直哉
    • Organizer
      日本顕微鏡学会第74回学術講演会
  • [Presentation] Atomic-resolution differential phase contrast scanning transmission electron microscopy for materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      MRS spring meeting 2018
    • Int'l Joint Research / Invited
  • [Presentation] Advanced differential phase contrast scanning transmission electron microscopy for materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      2018 International Workshop on STEM, UCAS
    • Int'l Joint Research / Invited
  • [Presentation] Aberration-corrected DPC STEM for materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      Grand opening of IMRI and ISAMS-1, UC Irvine
    • Int'l Joint Research / Invited
  • [Presentation] Development of advanced scanning transmission electron microscopy for materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      JAFOE 2018
    • Int'l Joint Research / Invited
  • [Presentation] 先進DPC STEM法による材料電磁場解析2018

    • Author(s)
      柴田直哉
    • Organizer
      実用顕微評価技術セミナー2018、日本表面真空学会
    • Invited
  • [Presentation] 先進電子顕微鏡法を用いたセラミックス界面の原子・電子構造解析2018

    • Author(s)
      柴田直哉
    • Organizer
      フルラス・岡崎記念会2018年度講演会
    • Invited
  • [Presentation] Direct electromagnetic field imaging of materials and devices by atomic-resolution STEM2018

    • Author(s)
      N. Shibata
    • Organizer
      NCTC TEM/STEM Seminar and workshop, Bangkok
    • Int'l Joint Research / Invited
  • [Presentation] Aberration-corrected differential phase contrast STEM2018

    • Author(s)
      N. Shibata
    • Organizer
      EMSI 2018
    • Int'l Joint Research / Invited
  • [Presentation] Advanced DPC STEM for materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      Workshop on STEM with advanced detector
    • Int'l Joint Research / Invited
  • [Presentation] Direct electromagnetic field imaging of materials by advanced differential phase contrast STEM2018

    • Author(s)
      N. Shibata
    • Organizer
      19th International Microscopy Congress
    • Int'l Joint Research / Invited
  • [Presentation] 先進原子分解能STEM法による材料局所電磁場解析2018

    • Author(s)
      柴田直哉
    • Organizer
      日本金属学会秋期大会
    • Invited
  • [Presentation] Direct electromagnetic field imaging of interfaces by advanced STEM2018

    • Author(s)
      N. Shibata
    • Organizer
      iWOE 25
    • Int'l Joint Research / Invited
  • [Presentation] Atomic-scale understanding of ceramic interfaces by advanced electron microscopy2018

    • Author(s)
      N. Shibata
    • Organizer
      MS&T 18
    • Int'l Joint Research / Invited
  • [Presentation] Development of subatomic-resolution electron microscopy for advanced materials research2018

    • Author(s)
      N. Shibata
    • Organizer
      The 2nd workshop on functional materials science
    • Int'l Joint Research / Invited
  • [Presentation] Towards subatomic-resolution electron microscopy2018

    • Author(s)
      N. Shibata
    • Organizer
      CEMS-RIKEN
    • Invited

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Published: 2019-12-27  

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