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Elucidation of Photoexcited Dynamics at the Photochromic Surface Using Femtosecond Electronic Sum-Frequency Generation Spectroscopy

Research Project

Project/Area Number 18K14180
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionOsaka University

Principal Investigator

Sotome Hikaru  大阪大学, 基礎工学研究科, 助教 (60758697)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000)
Fiscal Year 2020: ¥390,000 (Direct Cost: ¥300,000、Indirect Cost: ¥90,000)
Fiscal Year 2019: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000)
Fiscal Year 2018: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Keywordsフォトクロミック分子 / 超高速分光 / 電子和周波発生分光 / 光機能 / フォトクロミック反応 / 電子和周波発生分光法 / 光異性化反応 / 時間分解分光 / 光機能界面 / 過渡吸収分光 / 励起状態ダイナミクス
Outline of Final Research Achievements

Photochromic reactions at the surface play an important role in photoswitching of physical properties and control of molecular orientation at the surface. For elucidation of photoinduced responses and functions of photofunctional materials, we constructed an apparatus for femtosecond time-resolved electronic sum-frequency generation spectroscopy and applied it to observation of ultrafast isomerization reactions of photochromic molecules to reveal its molecular mechanism and factors for dominating the overall reactions. We selected photochromic samples suitable to the measurements at the surface by using transient absorption and time-resolved vibrational spectroscopies. In the measurements at the surface, we introduced a rotational sample stage to avoid degradation of samples and perform the stable measurements. A series of attempts in the present study paved a way to applications of this time-resolved technique to a variety of sample systems such as functional materials.

Academic Significance and Societal Importance of the Research Achievements

本研究の主眼であるフォトクロミック分子系は、表面物性の光スイッチングや液晶分子配向において界面機能を担っており、これまではバルク溶液における光計測から明らかになった反応速度や反応量子収率などの知見をもとに材料設計がなされてきたが、これを表面にあるがままの形態で計測することをめざした本研究の分光計測技術の開発や得られた成果は、表面・界面の材料物性研究の足がかりになると考えられる。

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • 2018 Research-status Report
  • Research Products

    (44 results)

All 2021 2020 2019 2018

All Journal Article (11 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 11 results,  Open Access: 2 results) Presentation (33 results) (of which Int'l Joint Research: 13 results,  Invited: 1 results)

  • [Journal Article] Slow photoionization via higher excited states of N,N-dimethylaniline in ethanol solution probed by femtosecond transient absorption spectroscopy under two-pulse two-photon excitation2021

    • Author(s)
      Koga Masafumi、Miyake Yuto、Hayasaka Mizuki、Sotome Hikaru、Miyasaka Hiroshi
    • Journal Title

      The Journal of Chemical Physics

      Volume: 154 Issue: 5 Pages: 054304-054304

    • DOI

      10.1063/5.0028018

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Geometrical Evolution and Formation of the Photoproduct in the Cycloreversion Reaction of a Diarylethene Derivative Probed by Vibrational Spectroscopy2020

    • Author(s)
      Sotome Hikaru、Okajima Hajime、Nagasaka Tatsuhiro、Tachii Yuka、Sakamoto Akira、Kobatake Seiya、Irie Masahiro、Miyasaka Hiroshi
    • Journal Title

      ChemPhysChem

      Volume: 21 Issue: 14 Pages: 1524-1530

    • DOI

      10.1002/cphc.202000315

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Ultrafast capture of electrons ejected by photoionization leading to the formation of a charge-separated state at a high energy level2020

    • Author(s)
      Kawakami Tomomi、Koga Masafumi、Sotome Hikaru、Miyasaka Hiroshi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 31 Pages: 17472-17481

    • DOI

      10.1039/d0cp02029j

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Dominant Factor of the Cycloreversion Reactivity of Diarylethene Derivatives as Revealed by Femtosecond Time-Resolved Absorption Spectroscopy2020

    • Author(s)
      Hikaru Sotome, Kanako Une, Tatsuhiro Nagasaka, Seiya Kobatake, Masahiro Irie, Hiroshi Miyasaka
    • Journal Title

      J. Chem. Phys.

      Volume: 152 Issue: 3 Pages: 034301-034301

    • DOI

      10.1063/1.5134552

    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Journal Article] Restriction of the Conrotatory Motion in Photo-Induced 6π Electrocyclic Reaction: Formation of the Excited State of the Closed-Ring Isomer in the Cyclization2020

    • Author(s)
      Tatsuhiro Nagasaka, Hikaru Sotome, Soichiro Morikawa, Lucas Martinez Uriarte, Michel Sliwa, Tsuyoshi Kawai, Hiroshi Miyasaka
    • Journal Title

      RSC Adv.

      Volume: 10 Issue: 34 Pages: 20038-20045

    • DOI

      10.1039/d0ra03523h

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Crystallization-induced emission of 1,2-bis(3-methyl-5-(4-alkylphenyl)-2-thienyl)perfluorocyclopentenes: A mechanical and thermal recording system2019

    • Author(s)
      Tatsumoto Nakahama; Daichi Kitagawa; Hikaru Sotome; Syoji Ito; Hiroshi Miyasaka; Seiya Kobatake*
    • Journal Title

      Dyes and Pigments

      Volume: 160 Pages: 450-456

    • DOI

      10.1016/j.dyepig.2018.08.031

    • NAID

      120006955107

    • URL

      https://ocu-omu.repo.nii.ac.jp/records/2019813

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Ionization Dynamics of a Phenylenediamine Derivative in Solutions as Revealed by Femtosecond Simultaneous and Stepwise Two-Photon Excitation2019

    • Author(s)
      M. Koga, Y. Yoneda, H. Sotome, H. Miyasaka
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 21 Issue: 6 Pages: 2889-2898

    • DOI

      10.1039/c8cp06530f

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Cyclization reaction dynamics of an inverse type diarylethene derivative as revealed by time-resolved absorption and fluorescence spectroscopies2019

    • Author(s)
      Hikaru Sotome; Daichi Kitagawa; Tatsumoto Nakahama; Syoji Ito; Seiya Kobatake; Masahiro Irie*; Hiroshi Miyasaka*
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: Published online Issue: 17 Pages: 0-0

    • DOI

      10.1039/c8cp07393g

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Multiphoton-Gated Cycloreversion Reaction of a Fluorescent Diarylethene Derivative as Revealed by Transient Absorption Spectroscopy2018

    • Author(s)
      T. Nagasaka, T. Kunishi, H. Sotome, M. Koga, M. Morimoto, M. Irie, H. Miyasaka
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 30 Pages: 19776-19783

    • DOI

      10.1039/c8cp01467a

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Cycloreversion Reaction of a Fulgide Derivative in Higher Excited States Attained by Femtosecond Two-Photon Pulsed Excitation2018

    • Author(s)
      T. Nagasaka, H. Sotome, Y. Yoshida, Y. Yokoyama, H. Miyasaka
    • Journal Title

      J. Phys. Chem. C

      Volume: 122 Issue: 43 Pages: 24987-24995

    • DOI

      10.1021/acs.jpcc.8b06271

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Stepwise Two-Photon-Induced Electron Transfer from Higher Excited States of Noncovalently Bound Porphyrin-CdS/ZnS Core/Shell Nanocrystals2018

    • Author(s)
      T. Uno, M. Koga, H. Sotome, H. Miyasaka, N. Tamai, Y. Kobayashi
    • Journal Title

      J. Phys. Chem. Lett.

      Volume: 9 Issue: 24 Pages: 7098-7104

    • DOI

      10.1021/acs.jpclett.8b03106

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Presentation] 多連光パルス列を用いたPump-Repump-Probe分光法における信号増幅法の開発2021

    • Author(s)
      五月女 光, 古賀 雅史, 澤田 知弥, 宮坂 博
    • Organizer
      日本化学会第101春季年会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 構造ダイナミクス解明に向けたフェムト秒誘導ラマン分光装置の開発2020

    • Author(s)
      森田 悠介, 五月女 光, 宮坂 博
    • Organizer
      2020年web光化学討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 吸収スペクトルの温度依存性測定による蛍光性ジアリールエテンのUrbach tailを支配する因子の解明2020

    • Author(s)
      奥井 優里, 新免 遼, 長坂 龍洋, 五月女 光, 森本 正和, 入江 正浩, 宮坂 博
    • Organizer
      2020年web光化学討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Coherent Control of Photochromic Reactions of 6pi Electron Systems Using Multiple Femtosecond Pulses2020

    • Author(s)
      Hikaru Sotome
    • Organizer
      Trombay Symposium on Radiation & Photochemistry 2020 (TSRP-2020)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Elucidation of Exceptional Electrocyclic Reaction Dynamics of a Dithiazolylarylene Derivative2019

    • Author(s)
      Tatsuhiro Nagasaka, Hikaru Sotome, Ryosuke Sei, Tsuyoshi Kawai, Hiroshi Miyasaka
    • Organizer
      35th Symposium on Chemical Kinetics and Dynamics
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Elucidation of 6π-electrocyclic Reaction Dynamics of a Dithiazolylarylene Derivative2019

    • Author(s)
      Tatsuhiro Nagasaka, Hikaru Sotome, Ryosuke Sei, Tsuyoshi Kawai, Hiroshi Miyasaka
    • Organizer
      The 29th International Conference on Photochemistry
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Cycloreversion Reactivity of Photochromic Diarylethene Derivatives: Negative Correlation between the S1 State and Higher State Excited by Stepwise Two-Photon Absorption2019

    • Author(s)
      Hikaru Sotome, Tatsuhiro Nagasaka, Seiya Kobatake, Hiroshi Miyasaka
    • Organizer
      The 14th Femtochemistry Conference
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Development of a stimulated Raman spectrometer and its application to in situ structural tracking of molecular assembly processes in solution2019

    • Author(s)
      SOTOME Hikaru, MORITA Yusuke, MIYASAKA Hiroshi
    • Organizer
      2019年光化学討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] ジケトピロロピロール超分子ポリマーにおける励起子及びコヒーレントフォノンダイナミクス2019

    • Author(s)
      五月女 光, 深谷菜摘, 大城宗一郎, 山口茂弘, 宮坂 博
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] 特異的な6π電子環状反応を示すジチアゾリルアリーレン誘導体の反応メカニズムの解明2019

    • Author(s)
      長坂 龍洋,五月女 光,Sliwa Michel,Uriarte Lucas,河合 壯,宮坂 博
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] Cyclization reaction dynamics of an inverse type diarylethene derivative in solution and solid phases2019

    • Author(s)
      H. Sotome, D. Kitagawa, T. Nakahama, S. Ito, S. Kobatake, H. Miyasaka
    • Organizer
      9th International Symposium On Photochromism
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Elucidation of Cyclization and Cycloreversion Reaction Dynamics of a Dithiazolylarylene Derivative2019

    • Author(s)
      T. Nagasaka, R. Sei, H. Sotome, T. Kawai, H. Miyasaka
    • Organizer
      International Conference on Materials for the Millenium (MATCON 2019)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] 6π Electrocyclic Reaction Dynamics of a Dithiazolylarylene Derivative2019

    • Author(s)
      T. Nagasaka, R. Sei, H. Sotome, T. Kawai, H. Miyasaka
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] 振動自由度を利用したジアリールエテン誘導体の多光子開環反応の高次制御2019

    • Author(s)
      五月女 光・立井 佑果・小畠 誠也・宮坂 博
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] ピレノール誘導体ートリエチルアミン系における超高速プロトン移動反応ダイナミクス2019

    • Author(s)
      藤本 晋伍・五月女 光・宮坂 博
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] Contribution of the S1-S1 Annihilation and Photothermal Effect to the Cycloreversion Reaction in Diarylethene Nanoparticles2019

    • Author(s)
      T. Kurata, H. Sotome, J. Su, J. Piard, R. Metivier, K. Nakatani, H, Miyasaka
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] Coherent Control of the Two-Photon Cycloreversion Reaction of a Photochromic Diarylethene Derivative Using Vibrational Degree of Freedom2019

    • Author(s)
      H. Sotome, Y. Tachii, S. Kobatake, H. Miyasaka
    • Organizer
      Handai-Kandai-GiessenDai Joint Seminar on Materials
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Cycloreversion Reaction of a Fulgide Derivative in Higher Excited States Attained by Stepwise Two-Photon Excitation2018

    • Author(s)
      T. Nagasaka, H. Sotome, Y. Yokoyama, H. Miyasaka
    • Organizer
      27th IUPAC International Symposium on Photochemsitry
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Two-Photon Cycloreversion Reaction of a Diarylethene Derivative with a Methoxy Group2018

    • Author(s)
      S. Fujimoto, H. Sotome, H. Miyasaka
    • Organizer
      27th IUPAC International Symposium on Photochemsitry
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Stepwise and Simultaneous Two-Photon Cycloreversion Reaction Dynamics of a Dithazolylarylene Derivative: Effects of Structural Relaxation and Symmetry2018

    • Author(s)
      T. Nagasaka, H. Sotome, T. Kawai, H. Miyasaka
    • Organizer
      2018年光化学討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] 過渡吸収二色性測定によるジアリールエテン誘導体の逐次2光子開環反応における中間状態の励起状態ダイナミクスの解明2018

    • Author(s)
      立井 佑果・五月女 光・小畠 誠也・宮坂 博
    • Organizer
      2018年光化学討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] 時間分解吸収・蛍光測定によるジチアゾリルアリーレン誘導体の6π電子環状反応メカニズムの解明2018

    • Author(s)
      清 亮輔・藤本 晋伍・長坂 龍洋・五月女 光・河合 壯・宮坂 博
    • Organizer
      2018年光化学討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] メトキシ基をもつジアリールエテン誘導体の多光子開環反応ダイナミクス2018

    • Author(s)
      藤本 晋伍・長坂 龍洋・五月女 光・小畠 誠也・宮坂 博
    • Organizer
      2018年光化学討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] 6π電子系の開環反応における高位励起状態の反応性:構造緩和と対称性の影響2018

    • Author(s)
      長坂 龍洋・五月女 光・河合 壯・横山 泰・宮坂 博
    • Organizer
      第12回分子科学討論会2018福岡
    • Related Report
      2018 Research-status Report
  • [Presentation] ジアリールエテン誘導体の逐次2光子開環反応:中間状態の振動コヒーレンスの位相選択による反応収量の関係2018

    • Author(s)
      立井 佑果・五月女 光・小畠 誠也・宮坂 博
    • Organizer
      第12回分子科学討論会2018福岡
    • Related Report
      2018 Research-status Report
  • [Presentation] ジアリールエテン誘導体の開環反応ダイナミクス:紫外及び赤外時間分解吸収分光による開環体生成の直接観測2018

    • Author(s)
      五月女 光・岡島 元・長坂 龍洋・立井 佑果・坂本 章・宮坂 博
    • Organizer
      第12回分子科学討論会2018福岡
    • Related Report
      2018 Research-status Report
  • [Presentation] 高位励起状態における6π電子系の開環反応:対称性と構造緩和の影響2018

    • Author(s)
      長坂龍洋・五月女 光・河合 壯・横山 泰・宮坂 博
    • Organizer
      第8回CSJフェスタ2018
    • Related Report
      2018 Research-status Report
  • [Presentation] 振動自由度を利用したジアリールエテン誘導体の多光子開環反応の高次制御2018

    • Author(s)
      五月女 光・立井佑果・小畠誠也・宮坂 博
    • Organizer
      第12回物性科学領域横断研究会
    • Related Report
      2018 Research-status Report
  • [Presentation] 高位励起状態における6π電子系の開環反応2018

    • Author(s)
      長坂 龍洋・五月女 光・河合 壮・横山 泰・宮坂 博
    • Organizer
      第12回物性科学領域横断研究会
    • Related Report
      2018 Research-status Report
  • [Presentation] Photosynergetic Responses of Diarylethene Nanoparticles Leading to Cycloreversion Reaction2018

    • Author(s)
      T. Kurata, H. Sotome, J. Su, J. Piard, R. Metivier, K. Nakatani, H. Miyasaka
    • Organizer
      10th Asian Photochemistry Conference
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Stepwise Two-photon Cycloreversion Reaction of a Diarylethene Derivative Controlled via Vibrational Coherence2018

    • Author(s)
      Y. Tachii, H. Sotome, S. Kobatake, H. Miyasaka
    • Organizer
      10th Asian Photochemistry Conference
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Exceptional Reaction Mechanism of 6Pi-Electrocyclic Process of a Dithiazolylarylene Derivative2018

    • Author(s)
      H. Sotome, R. Sei, T. Nagasaka, S. Fujimoto, T. Kawai, H. Miyasaka
    • Organizer
      10th Asian Photochemistry Conference
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Two-Photon Cycloreversion Reaction Dynamics of a Dithiazolylarylene Derivative2018

    • Author(s)
      T. Nagasaka, H. Sotome, T. Kawai, H. Miyasaka
    • Organizer
      10th Asian Photochemistry Conference
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research

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Published: 2018-04-23   Modified: 2022-01-27  

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