Nonadiabatic transition in photochemical reactions studied by time-resolved spectroscopy of molecular orbitals

• Project/Area Number: 15H03702
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Atomic/Molecular/Quantum electronics
• Research Institution: Hokkaido University
• Principal Investigator: sekikawa taro 北海道大学, 工学研究院, 准教授 (90282607)
• Co-Investigator(Renkei-kenkyūsha): TAKETSUGU Tetsuya 北海道大学, 大学院理学研究院, 教授 (90280932)
• Research Collaborator: IIKUBO Ryo ; TENTAKU Tateharu ; ARAKI Kotaro ; ATOBE Ryunosuke
• Project Period (FY): 2015-04-01 – 2018-03-31
• Project Status: Completed (Fiscal Year 2017)
• Budget Amount: ¥17,290,000 (Direct Cost: ¥13,300,000、Indirect Cost: ¥3,990,000); Fiscal Year 2017: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000); Fiscal Year 2016: ¥6,500,000 (Direct Cost: ¥5,000,000、Indirect Cost: ¥1,500,000); Fiscal Year 2015: ¥9,100,000 (Direct Cost: ¥7,000,000、Indirect Cost: ¥2,100,000)
• Keywords: 高次高調波 / 時間分解光電子分光 / 光化学反応 / 非断熱遷移 / 分子軌道 / 光電子分光 / 円錐交差 / 共役分子 / 置換基効果 / 共役ジエン

Outline of Final Research Achievements

Relaxation dynamics of 1,3-pentadiene(PD) and 2,5-dimethyl-2,4-hexadiene(DH) were investigated by time-resolved photoelectron spectroscopy to elucidate the effects of the steric hinderence or the mass by the methyl groups on the relaxation dynamics of the conjugated dienes.
Our theoretical calculation reveals that the molecular structure of DH at a conical intersection is totally different from those of BD and PD, which might be attributable to the steric hinderence. Upon returning to the ground state, the stimulated vibrational modes in DH and PD are different because of the different structure at the conical intersections. This difference appears in the photoelectron specra.

Research Products

• [Int'l Joint Research] Stockholm University(スウェーデン)
• [Int'l Joint Research] stockholm university(sweden)
• [Int'l Joint Research] national research council(canada)
• [Journal Article] Ultrafast photonics: Tailoring extreme-ultraviolet light (2017)
  • Author(s): T. Sekikawa, K. L. Ishikawa
  • Journal Title: Nature Photonics Volume: 11 Issue: 4 Pages: 209-210
  • DOI: 10.1038/nphoton.2017.44
  • Peer Reviewed
• [Journal Article] Bond Selective Probe by Time-Resolved Photoelectron Spectroscopy: Ring-Opening Dynamics of 1,3-Cyclohexadiene (2016)
  • Author(s): R. Iikubo, T. Sekikawa, Y. Harabuchi, and T. Taketsugu
  • Journal Title: Faraday Discussions Volume: 194 Pages: 147-160
  • DOI: 10.1039/c6fd00063k
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Electronic and non-adiabatic dynamics: general discussion (2016)
  • Author(s): A. J. Orr-Ewing, O. Schalk, J. P. Marangos, H. J. Worner, R. J. D. Miller, W. Domcke, K. Ueda, D. M. Neumark, A. Stolow, D. Dowek, S. Mukamel, T. Sekikawa
  • Journal Title: Faraday Discussions Volume: 194 Pages: 209-257
  • DOI: 10.1039/c6fd90070d
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Excited State Non-Adiabatic Dynamics of N-Methylpyrrole: A Time-Resolved Photoelectron Spectroscopy and Quantum Dynamics Study (2016)
  • Author(s): G. Wu, S. P. Neville, O. Schalk, T. Sekikawa, M. N. R. Ashfold, G. A. Worth, and A. Stolow
  • Journal Title: Journal of Chemical Physics Volume: 144 Issue: 1 Pages: 2463-2468
  • DOI: 10.1063/1.4938423
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] 単一次数高調波光源による気相分子の時間分解光電子分光 (2015)
  • Author(s): 関川太郎，飯窪亮，原渕祐，佐藤壮太，武次徹也，萱沼洋輔
  • Journal Title: レーザー研究 Volume: 43 Pages: 833-837
  • NAID: 130007957178
  • Peer Reviewed / Acknowledgement Compliant
• [Presentation] Photochemical reaction of functional molecules probed by time-resolved photoelectron spectroscopy (2017)
  • Author(s): Taro Sekikawa
  • Organizer: The 8th Asian Workshop on Generation and Application of Coherent XUV and X-ray Radiation
  • Place of Presentation: Hsinchu (Taiwan)
  • Year and Date: 2017-03-27
  • Int'l Joint Research / Invited
• [Presentation] Relaxation dynamics in conjugated diene systems studied by femtosecond time-resolved mass spectrometry (2017)
  • Author(s): 跡部龍之介,天宅建晴,関川太郎,佐藤壮太,原渕祐,武次徹也,赤木浩,板倉隆二
  • Organizer: 光・量子ビーム科学合同シンポジウム2017
• [Presentation] 高次高調波分光による超高速光異性化反応の観測 (2017)
  • Author(s): 金島圭佑, 二ノ田有輝, 関川太郎
  • Organizer: 第78回応用物理学会秋季学術講演会
• [Presentation] キラル分子からの円偏光高次高調波発生 (2017)
  • Author(s): 原田要一, 新田優輝, 金島圭佑, 関川 太郎
  • Organizer: 第78回応用物理学会秋季学術講演会
• [Presentation] 時間分解高次高調波分光による 1,3-シクロヘキサジエンの超高速光開環反応の解明 (2017)
  • Author(s): 二ノ田有輝,金島圭佑,関川太郎
  • Organizer: 第５３回応用物理学会北海道支部/第１４回日本光学会北海道支部合同学術講演会
• [Presentation] 時間分解高次高調波分光による超高速光開環反応の解明 (2017)
  • Author(s): 金島圭佑,二ノ田有輝,関川太郎
  • Organizer: レーザー学会学術講演会第38回年次大会
• [Presentation] 二色円偏光合成電場よるキラル分子からの円偏光高次高調波発生 (2017)
  • Author(s): 原田要一,原口英介,芝 悠真,金島圭佑,関川太郎
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] Controlling the Relaxation Pathways by Substituent Effects in Conjugated Dienes (2017)
  • Author(s): T. Tentaku, R. Atobe, K. Araki, S. Satoh, Y. Harabuchi, T. Taketsugu, and T. Sekikawa
  • Organizer: CLEO/Europe-EQEC
  • Int'l Joint Research
• [Presentation] Tailoring Relaxation Pathways in Conjugated Dienes Studied by Time-Resolved Photoelectron Spectroscopy (2017)
  • Author(s): T. Tentaku, S. Satoh, Y. Harabuchi, T. Taketsugu, T. Sekikawa,
  • Organizer: The 13th Femtochemistry Conference
  • Int'l Joint Research
• [Presentation] Nonadiabatic Dynamics in Functional Molecules Studied by Time-resolved Photoelectron Spectroscopy (2017)
  • Author(s): T. Sekikawa
  • Organizer: 2nd International Symposium on Attosecond Science
  • Int'l Joint Research / Invited
• [Presentation] Nonadiabatic Dynamics in Functional Molecules Studied by Time-resolved Photoelectron Spectroscopy (2017)
  • Author(s): Y. Ninota, K. Kaneshima, and T.Sekikawa,
  • Organizer: 2nd International Symposium on Attosecond Science
  • Int'l Joint Research
• [Presentation] Circular Dichroism in High Harmonic Generation from Chiral Molecules (2017)
  • Author(s): Y. Harada, E. Haraguchi, K. Kaneshima, and T. Sekikawa
  • Organizer: High-Intensity Lasers and High-Field Phenomena
  • Int'l Joint Research
• [Presentation] 置換基効果を利用した共役ジエン系の励起緩和経路の制御 (2017)
  • Author(s): 天宅建晴,荒木孝太郎,跡部龍之介,佐藤壮太,原渕祐,武次徹也,関川太郎
  • Organizer: 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)
• [Presentation] Structural dynamics of photochemical reactions probed by time-resolved photoelectron spectroscopy using high harmonic pulses (2016)
  • Author(s): Ryo Iikubo, Taro Sekikawa, Yu Harabuchi and Tetsuya Taketsugu
  • Organizer: Ultrafast Imaging of Photochemical Dynamics Faraday Discussion
  • Place of Presentation: Edinburgh (UK)
  • Year and Date: 2016-08-31
  • Int'l Joint Research / Invited
• [Presentation] Bond Selective Probe by Time-Resolved Photoelectron Spectroscopy: Ring-Opening Dynamics of 1,3-Cyclohexadiene (2016)
  • Author(s): R. Iikubo, T. Sekikawa, Y. Harabuchi, and T. Taketsugu
  • Organizer: 20th International Conference on Ultrafast Phenomena
  • Place of Presentation: Santa Fe (USA)
  • Year and Date: 2016-07-17
  • Int'l Joint Research
• [Presentation] Bond Selective Probe by Time-Resolved Photoelectron Spectroscopy: Ring-Opening Dynamics of 1,3-Cyclohexadiene (2016)
  • Author(s): R. Iikubo, T. Sekikawa, Y. Harabuchi, and T. Taketsugu
  • Organizer: Conference on Lasers and Electro-Optics
  • Place of Presentation: San Jose (USA)
  • Year and Date: 2016-06-06
  • Int'l Joint Research
• [Presentation] 1,4- シクロヘキサジエンにおける水素原子の脱離ダイナミクス (2016)
  • Author(s): 荒木孝太郎，天宅建晴，跡部龍之介，関川太郎，原渕祐，佐藤 壮太，武次 徹也
  • Organizer: 応用物理学会春季学術講演会
  • Place of Presentation: 東京工業大学大岡山キャンパス（東京都目黒区）
  • Year and Date: 2016-03-21
• [Presentation] フェムト秒時間分解質量分析による共役ジエンの光励起緩和ダイナミクスの観測 (2016)
  • Author(s): 跡部龍之介,天宅建晴,関川太郎,佐藤壮太,原渕祐,武次徹也,赤木浩,板倉隆二
  • Organizer: 第10回分子科学討論会
  • Place of Presentation: 神戸ファッションマート（兵庫県・神戸市）
• [Presentation] 高次高調波を用いた時間分解光電子分光による共役系ジエンの置換基効果 (2016)
  • Author(s): 天宅建晴,跡部龍之介,荒木孝太郎,関川太郎,佐藤壮太,原渕祐,武次徹也,赤木浩,板倉隆二
  • Organizer: 第10回分子科学討論会
  • Place of Presentation: 神戸ファッションマート（兵庫県・神戸市）
• [Presentation] 時間分解光電子分光による1,2-ブタジエンの光化学反応ダイナミクスの研究 (2015)
  • Author(s): 飯窪亮, 藤原丈久, 関川太郎, 原渕祐, 佐藤壮太, 武次徹也, 萱沼洋輔
  • Organizer: 第9回分子科学討論会
  • Place of Presentation: 東京工業大学大岡山キャンパス（東京都目黒区）
  • Year and Date: 2015-09-19
• [Presentation] 共役系ジエンにおける超高速光励起緩和ダイナミクスの研究 (2015)
  • Author(s): 天宅建晴，荒木孝太郎，関川太郎
  • Organizer: 応用物理学会秋季学術講演会
  • Place of Presentation: 名古屋国際会議場（愛知県名古屋市）
  • Year and Date: 2015-09-13
• [Presentation] Ring-opening dynamics of 1,3-cyclohexadiene studied by time-resolved molecular orbital spectroscopy (2015)
  • Author(s): T. Sekikawa, R. Iikubo, Y. Harabuchi, and T. Taketsugu
  • Organizer: The Hamburg Conference on Femtochemistry
  • Place of Presentation: DESY, Hamburg (Germany)
  • Year and Date: 2015-07-15
  • Int'l Joint Research
• [Presentation] Photodissociation of 1,2-Butadiene Studied by Time-Resolved Molecular Orbital Spectroscopy Using Single-Order High Harmonic Pulses (2015)
  • Author(s): R. Iikubo, T. Fujiwara, ∙T. Sekikawa, Y. Harabuchi, T. Taketsugu, and Y. Kayanuma
  • Organizer: Conference on Lasers and Electro-Optics Europe & European Quantum Electronics
  • Place of Presentation: Munich(Germany)
  • Year and Date: 2015-06-21
  • Int'l Joint Research
• [Presentation] Photodissociation of 1,2-Butadiene Studied by Time-Resolved Molecular Orbital Spectroscopy Using Single-Order High Harmonic Pulses (2015)
  • Author(s): R. Iikubo, T. Fujiwara, T. Sekikawa, Y. Harabuchi, T. Taketsugu, and Y. Kayanuma,
  • Organizer: 4th Advanced Lasers and Photon Sources Conference ALPS’15
  • Place of Presentation: Pacifico Yokohama(Yokohama, Kanagawa)
  • Year and Date: 2015-04-23
  • Int'l Joint Research
• [Book] Optical Technologies for Extreme-Ultraviolet and Soft X-ray Coherent Sources (2015)
  • Author(s): T. Sekikawa
  • Total Pages: 19
  • Publisher: Springer