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Modification of the bandgap of hexagonal BN and deep-ultraviolet luminescence dynamics of excitons in them

Research Project

Project/Area Number 20K20993
Research Category

Grant-in-Aid for Challenging Research (Exploratory)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 21:Electrical and electronic engineering and related fields
Research InstitutionTohoku University

Principal Investigator

CHICHIBU Shigefusa  東北大学, 多元物質科学研究所, 教授 (80266907)

Co-Investigator(Kenkyū-buntansha) 原 和彦  静岡大学, 電子工学研究所, 教授 (80202266)
小島 一信  東北大学, 多元物質科学研究所, 准教授 (30534250)
嶋 紘平  東北大学, 多元物質科学研究所, 助教 (40805173)
Project Period (FY) 2020-07-30 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥6,500,000 (Direct Cost: ¥5,000,000、Indirect Cost: ¥1,500,000)
Fiscal Year 2021: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Fiscal Year 2020: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Keywords窒化ボロン / 間接遷移 / 直接遷移 / 深紫外線 / 時間分解分光
Outline of Research at the Start

六方晶層状窒化ボロン(h-BN)は、2次元ハニカム構造を層状に積み重ねた、禁制帯幅の広い半導体である。そして間接遷移型半導体でありながら室温で210~230 nmの発光を呈するため、深紫外(DUV)光源用材料として期待できる。ごく最近、単一原子層h-BNの禁制帯が直接遷移型となる事が報告されたが真偽は定かではない。
本研究では、高純度h-BN単層膜をエピタキシャル成長させ、フェムト秒パルスDUVレーザやフェムト秒パルス電子線を用いて発光寿命や拡散長等を定量化し発光機構を明らかにする。本研究が実現されれば、h-BN以外の広禁制帯幅半導体の発光機構研究や物性の理解も可能となる。

Outline of Final Research Achievements

Hexagonal boron nitride (hBN) crystallizes in layers of a two-dimensional honeycomb BN structure. Since hBN exhibits high-efficiency emissions at 5.2-5.9 eV in spite of the indirect bandgap, hBN has a potential for the use in deep-ultraviolet light emitters. Recently, the presence of a direct bandgap has been reported in an isolated monolayer hBN (mBN). However, little is known about the luminescent properties of mBN. Here, temporally and spatially resolved luminescence measurements were carried out to elucidate the emission dynamics of indirect excitons (iXs) in hBN and direct excitons (dXs) in mBN epilayers. The room-temperature emission lifetimes of iXs in hBN were about 55 ps, which implies excellent radiative performance of hBN. Cathodoluminescence (CL) spectra at 13 K of mBN exhibited a distinct dX emission peak at around 6.04 eV superimposed on a broad 5.5-eV-band that originated from hBN. In addition, a CL peak at 6.035 eV that originated from graphitic BN was identified.

Academic Significance and Societal Importance of the Research Achievements

hBNが間接遷移型半導体でありながら光子エネルギー約5.8 eVの高効率深紫外線(DUV)発光を呈すること、hBNを単一層まで薄くしたmBNの禁制帯が直接遷移型となり6.04 eVの発光を呈する事に加え、グラファイト状積層構造のBernal BNも直接遷移型ではないかと思われる禁制帯を持ち6.035 eVの発光を呈する事を明らかにした事は学術的意義が大きいだけでなく、BNを用いたDUV発光素子の開発に繋がり殺菌や消毒を通じて安全な水・空気・サニタリー環境の提供を通じて社会貢献できる。また、本研究に用いた自作の陰極線蛍光計測系は禁制帯幅に制限されないためBN以外の2次元材料の評価に有用である。

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (21 results)

All 2023 2022 2021 2020 Other

All Int'l Joint Research (6 results) Journal Article (2 results) (of which Peer Reviewed: 2 results) Presentation (12 results) (of which Int'l Joint Research: 3 results,  Invited: 2 results) Remarks (1 results)

  • [Int'l Joint Research] Univ. Montpellier II(フランス)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Univ. Nottingham(英国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Univ. Montpellier II(フランス)

    • Related Report
      2021 Research-status Report
  • [Int'l Joint Research] Univ. Norttingham(英国)

    • Related Report
      2021 Research-status Report
  • [Int'l Joint Research] Univ. Montpellier II(フランス)

    • Related Report
      2020 Research-status Report
  • [Int'l Joint Research] Univ. Norttingham(英国)

    • Related Report
      2020 Research-status Report
  • [Journal Article] Recombination dynamics of indirect excitons in hexagonal BN epilayers containing polytypic segments grown by chemical vapor deposition using carbon-free precursors [Featured Article]2022

    • Author(s)
      Chichibu S. F.、Shima K.、Kikuchi K.、Umehara N.、Takiguchi K.、Ishitani Y.、Hara K.
    • Journal Title

      Applied Physics Letters

      Volume: 120 Issue: 23 Pages: 2319041-7

    • DOI

      10.1063/5.0090431

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Room-temperature intrinsic excitonic luminescence from a hexagonal boron nitride thin film grown on a sapphire substrate by low-pressure chemical vapor deposition using BCl<sub>3</sub> as a boron source2021

    • Author(s)
      Umehara Naoki、Adachi Takurou、Masuda Atsushi、Kouno Tetsuya、Kominami Hiroko、Hara Kazuhiko
    • Journal Title

      Japanese Journal of Applied Physics

      Volume: 60 Issue: 7 Pages: 075501-5

    • DOI

      10.35848/1347-4065/ac093f

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Presentation] Ultraviolet luminescence dynamics of hexagonal BN epilayers grown by chemical vapor deposition using carbon-free precursors2023

    • Author(s)
      T. Kasuya, K. Shima, K. Hara, and S. F. Chichibu
    • Organizer
      65th Electronic Materials Conference (EMC2023)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 炭素フリー原料を用いてサファイア基板上にCVD成長させたhBN薄膜の間接遷移励起子の発光ダイナミクス2023

    • Author(s)
      粕谷拓生, 嶋紘平, 梅原直己, 原和彦, 秩父重英
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 陰極線励起による単層六方晶BNのバンド端発光の観測2023

    • Author(s)
      嶋紘平, Tin S. Cheng, Christopher J. Mellor, Peter H. Benton, Christine Elias, Bernard Gil, Guillaume Cassabois, Sergei V. Novikov, 秩父重英
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 六方晶BN薄膜の減圧CVD成長の高温化2023

    • Author(s)
      大石 泰己, 渡邉 泰良, 田中 佑樹, 増田 克仁, 吉岡 陸, 増田 希良里, 小南 裕子, 原 和彦
    • Organizer
      発光型/非発光型ディスプレイ合同研究会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Emission dynamics of indirect excitons in hexagonal BN epilayers containing polytypic segments grown by chemical vapor deposition using carbon-free precursors2022

    • Author(s)
      S. F. Chichibu, K. Shima, K. Kikuchi, N. Umehara, K. Takiguchi, Y. Ishitani, and K. Hara
    • Organizer
      International Workshop on Nitride Semiconductors 2022 (IWN2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Near-band-edge recombination in monolayer hBN epitaxial films studied using cathodoluminescence spectroscopy2022

    • Author(s)
      K. Shima, C. Elias, T. S. Cheng, C. J. Mellor, P. H. Beton, S. V. Novikov, B. Gil, G. Cassabois, and S. F. Chichibu
    • Organizer
      International Workshop on Nitride Semiconductors 2022 (IWN2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 炭素フリー原料を用いてサファイア基板にCVD成長させた多型を含むhBN薄膜における間接遷移励起子の発光ダイナミクス2022

    • Author(s)
      秩父重英, 嶋紘平, 菊地清, 梅原直己, 瀧口佳祐, 石谷善博, 原和彦
    • Organizer
      第83回応用物理学会秋季学術講演会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 六方晶窒化ホウ素薄膜の減圧CVDにおける原料ガス導入タイミング2022

    • Author(s)
      吉岡 陸、田中 佑樹、渡邊 泰良、増田 克仁、大石 泰己、増田 希良里、小南 裕子、原 和彦
    • Organizer
      2022年 第69回応用物理学会春季学術講演会[25a-E203-6]
    • Related Report
      2021 Research-status Report
  • [Presentation] コールドウォール反応管を用いる六方晶窒化ホウ素薄膜の減圧CVDにおける原料供給量依存性2022

    • Author(s)
      増田 克仁、渡邊 泰良、田中 佑樹、吉岡 陸、大石 泰己、増田 希良里、小南 裕子、原 和彦
    • Organizer
      2022年 第69回応用物理学会春季学術講演会[25a-E203-7]
    • Related Report
      2021 Research-status Report
  • [Presentation] 炭素フリー原料を用いてサファイア基板に気相成長させたh-BN薄膜の空間分解カソードルミネッセンス評価2021

    • Author(s)
      秩父重英,嶋紘平,梅原直己,小島一信,原和彦
    • Organizer
      2021年 第82回応用物理学会秋季学術講演会[10p-N101-8]
    • Related Report
      2021 Research-status Report
  • [Presentation] Niバッファ層上への六方晶窒化ホウ素薄膜のCVD成長2021

    • Author(s)
      田中佑樹,渡邊泰良,吉岡陸,増田克仁,大石泰己,増田希良里,小南裕子,原和彦
    • Organizer
      2021年 第82回応用物理学会秋季学術講演会[23p-P07-1]
    • Related Report
      2021 Research-status Report
  • [Presentation] 時間空間分解カソードルミネッセンス法によるワイドバンドギャップ窒化物半導体の評価2020

    • Author(s)
      秩父重英
    • Organizer
      「放射線科学とその応用第186委員会」第36回研究会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Remarks] 東北大学 多元物質科学研究所 秩父研究室HP

    • URL

      http://www2.tagen.tohoku.ac.jp/lab/chichibu/html/index-j.html

    • Related Report
      2022 Annual Research Report

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Published: 2020-08-03   Modified: 2024-01-30  

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