Elucidation of reaction mechanism of site-specific chemical bond scission on self-assembled monolayers as a reaction platform

2011 Fiscal Year Final Research Report

• Project/Area Number: 21350014
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: Hiroshima University
• Principal Investigator: TANAKA Kenichiro 広島大学, 大学院・理学研究科, 名誉教授 (90106162)
• Co-Investigator(Kenkyū-buntansha): WADA Shin-ichi 広島大学, 大学院・理学研究科, 助教 (60304391) ; SEKITANI Tetsuji 広島大学, 大学院・理学研究科, 准教授 (30259981)
• Project Period (FY): 2009 – 2011
• Keywords: サイト選択的反応 / 内殻電子励起 / 軟X線光化学 / 光刺激イオン脱離 / 反応制御 / 自己組織化単分子膜 / オージェ崩壊過程

Research Abstract

As one of dreams of chemists, we have studied site-selective chemical bond scission by core electron excitation, and found that the selectivity of this reaction is much improved when the reaction takes place on the self-assembled monolayer(SAM) surface. The main purpose of this study is to answer the question why chemical bond scission can be controlled well on SAM surface. From systematic studies of the relevance of the selectivity of chemical bond scission and the kind and length of the main chain of SAM, it was found that the selectivity is much influenced by the lifetime of the reaction precursor. The reaction probability decreases with decreasing the lifetime by shortening the main chain of SAM, but the selectivity increases.

Research Products

• [Journal Article] Experimental verification of the chemical sensitivity of two-site double core-hole states formed by an x-ray FEL (2012)
  • Author(s): P. Salen, P. van der Meulen, H. T. Schmidt, R. D. Thomas, M. Larsson, R. Feifel, M. N. Piancastelli, L. Fang, B. Murphy, T. Osipov, N. Berrah, E. Kukk, K. Ueda, J. D. Bozek, C. Bostedt, S. Wada, R. Richter, V. Feyer, K. C. Prince
  • Journal Title: Phys. Rev. Lett. Volume: 108 Pages: 153003(1-5)
  • Peer Reviewed
• [Journal Article] Angle-resolved electron spectroscopy of laser-assisted Auger decay induced by afew-femtosecond X-ray pulse (2012)
  • Author(s): M. Meyer, P. Radcliffe, T. Tschentscher, J. T. Costello, A. L. Cavalieri, I. Grguras, A. R. Maier, R. Kienberger, J. Bozek, C. Bostedt, S. Schorb, R. Coffee, M. Messerschmidt, C. Roedig, E. Sistrunk, L. F. Di Mauro, G. Doumy, K. Ueda, S. Wada, S. Dusterer
  • Journal Title: Phys. Rev. Lett. Volume: 108 Pages: 063007(1-5)
  • Peer Reviewed
• [Journal Article] Core-to-Rydberg band shift and broadening of hydrogen bonded ammonia clusters studied with nitrogen K-edge excitation spectroscopy (2012)
  • Author(s): T. Yamanaka, K. Tabayashi, O. Takahashi, K. Tanaka, H. Namatame, M. Taniguchi
  • Journal Title: J. Chem. Phys Volume: 136(1) Pages: 014308(1-11)
  • Peer Reviewed
• [Journal Article] Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser (2011)
  • Author(s): N. Berrah, L. Fang, B. Murphy, T. Osipov, K. Ueda, E. Kukk, R. Feifel, P. van der Meulen, P. Salen, H. T. Schmidt, R. D. Thomas, M. Larsson, R. Richter, K. C. Prince, J. D. Bozek, C. Bostedt, S. Wada, M. N. Piancastelli, M. Tashiro, and M. Ehara
  • Journal Title: PNAS(Proc. Nat. Acad. Sci.) Volume: 108(41) Pages: 16912-16915
  • Peer Reviewed
• [Journal Article] 基礎から学ぶマススペクトロメトリ-/質量分析の源流,第4回光イオン化法の特徴 (2010)
  • Author(s): 田中健一郎, 小谷野猪之助
  • Journal Title: 質量分析 Volume: 58(1) Pages: 13-16
  • Peer Reviewed
• [Journal Article] 基礎から学ぶマススペクトロメトリ-/質量分析の源流,第5回内殻励起反応 (2010)
  • Author(s): 和田真一, 田中健一郎
  • Journal Title: 質量分析 Volume: 58(1) Pages: 17-27
  • Peer Reviewed
• [Journal Article] Development of a compact electron ion coincidence analyzer using a coaxially symmetric mirror electron energy analyzer and a miniature polar-angle-resolved time-of-flight ion mass spectrometer with four concentric anodes (2009)
  • Author(s): E. Kobayashi, A. Nambu, K. Mase, K. Isari, K. Tanaka, M. Mori, K. K. Okudaira, N. Ueno
  • Journal Title: Rev. Sci. Instr Volume: 80(4) Pages: 043303(1-6)
  • Peer Reviewed
• [Presentation] Structural change of photosensitive organic nano-crystals : Toward UV pump-X-ray probe measurements (2012)
  • Author(s): S. Wada
  • Organizer: Dis. Meeting on FEL experi. Elect./ molec. Dynamics
  • Place of Presentation: 京都市
  • Year and Date: 2012-03-29
• [Presentation] Molecular chain effect in soft X-ray photostimulated ion desorption from self-assembled monolayers of benzene derivatives (2012)
  • Author(s): M. Ogawa, S. Wada, R. Koga, J. Kajikawa, H. Hayashita, T. Sekitani, K. Tanaka, A, Hiraya
  • Organizer: 第16回広島放射光国際シンポジウム
  • Place of Presentation: 東広島市
  • Year and Date: 2012-03-01
• [Presentation] Ion desorption by core-excitation of methyl-ester terminated biphenyl SAM (2012)
  • Author(s): R. Koga, S. Wada, M. Ogawa, J. Kajikawa, H. Hayashita, T. Sekitani, K. Tanaka, A, Hiraya
  • Organizer: 第16回広島放射光国際シンポジウム
  • Place of Presentation: 東広島市
  • Year and Date: 2012-03-01
• [Presentation] Surface-site-selective study of valenceele ctronic states of Si(111)-7x7 adsorbed with water using Si-L23VV Auger electron Si-2p photoelectron coincidence measurements (2012)
  • Author(s): S. Arae, J. Kajikawa, H. Hayashita, M. Ogawa, S. Ohno, S. Wada, T. Sekitani, Y. Sato, S. Hanaoka, T. Kakiuchi, K. Mase, M. Okusawa, M. Tanaka
  • Organizer: 第16回広島放射光国際シンポジウム
  • Place of Presentation: 東広島市
  • Year and Date: 2012-03-01
• [Presentation] Construction and evaluation of Auger-photoelectron coincidence apparatus at BL13 of HiSOR (2012)
  • Author(s): T. Kakiuchi, Y. Sato, S. Hanaoka, J. Kajikawa, H. Hayashita, M. Ogawa, S. Arae, S. Wada, T. Sekitani, S. Nagaoka, M. Tanaka, K. Mase
  • Organizer: 第16回広島放射光国際シンポジウム
  • Place of Presentation: 東広島市
  • Year and Date: 2012-03-01
• [Presentation] NEXAFS spectroscopy of excited triplet state of anthraquinone by UV pump-X-ray probe technique (2012)
  • Author(s): T. Tsuru, S. Wada, H. Hayashita, H. Yoshida, A, Hiraya
  • Organizer: 第16回広島放射光国際シンポジウム
  • Place of Presentation: 東広島市
  • Year and Date: 2012-03-01
• [Presentation] フッ素置換したベンゼンチオール自己組織化単分子膜の内殻励起イオン脱離反応 (2012)
  • Author(s): 小川舞, 和田真一, 由布圭, 平野敦士, 石田敬樹, 平谷篤也, 田中健一
  • Organizer: 第25回日本放射光学会年会
  • Place of Presentation: 鳥栖市
  • Year and Date: 2012-01-08
• [Presentation] LCLSで始まったXFEL利用研究 (2011)
  • Author(s): 和田真一
  • Organizer: 日本分光学会中国四国支部年次講演会「X線領域の自由電子レーザー(XFEL)の最前線」
  • Place of Presentation: 東広島市
  • Year and Date: 2011-12-02
• [Presentation] 芳香族自己組織化単分子膜で見られる内殻励起反応の特異性 (2011)
  • Author(s): 和田真一, 油布圭, 平野敦士, 石田敬樹, 田中健一郎
  • Organizer: 第5回分子科学討論会
  • Place of Presentation: 札幌
  • Year and Date: 2011-09-23
• [Presentation] Coulomb explosion imaging of small organic molecules at LCLS (2011)
  • Author(s): B. Erk, A. Rudenko, D. Rolles, B. Rudek, L. Foucar, S. Epp, M. Cryle, I. Schlichting, C. Bostedt, S. Schorb, J. Bozek, A. Rouzee, A. Hundertmark, T. Marchenko, M. Simon, F. Filsinger, L. Christensen, S. de, S. Trippel, S. Wada, K. Ueda, C. D. Schroeter, J. Ullrich
  • Organizer: 27^<th> Int. Conf. on Photonic, Electronic and Atomic Collisions(XXVIIICPEAC)
  • Place of Presentation: Belfast, UK
  • Year and Date: 2011-08-02
• [Presentation] X-ray FEL induced double core-hole formation in polyatomic molecules (2011)
  • Author(s): P. Salen, P. van der Meulen, R. D. Thomas, H. T. Schmidt, M. Larsson, R. Feifel, M. Piancastelli, L. Fang, T. Osipov, B. Murphy, P. Juranic, N. Berrah, E. Kukk, K. Ueda, R. Richter, K. C. Prince, J. D. Bozek, C. Bostedt, S. Wada, M. Tashiro, M. Ehara, F. Tarantelli
  • Organizer: 27^<th> Int. Conf. on Photonic, Electronic and Atomic Collisions
  • Place of Presentation: Belfast, UK
  • Year and Date: 2011-08-01
• [Presentation] Multiple ionization and double core-hole production in molecules using the LCLS X-ray FEL (2011)
  • Author(s): L. Fang, T. Osipov, B. Murphy, P. Juranic, N. Berrah, E. Kukk, K. Ueda, R. Feifel, P. van der Meulen, P. Salen, H. Schmidt, R. Thomas, M. Larsson, R. Richter, K. C. Prince, J. D. Bozek, C. Bostedt, S. Wada, M. Piancastelli, M. Tashiro, M. Ehara, F. Tarantelli
  • Organizer: 27^<th> Int. Conf. on Photonic, Electronic and Atomic Collisions(XXVII ICPEAC)
  • Place of Presentation: Belfast, UK
  • Year and Date: 2011-07-28
• [Presentation] Why chemical bond scission can be controlled well on the self-Assembled monolayer surface? (2011)
  • Author(s): K. Tanaka, M. Ogawa, S. Wada, T. Sekitani, H. Yoshida, A. Hiraya
  • Organizer: 第27回化学反応討論会
  • Place of Presentation: 東京
  • Year and Date: 2011-06-10
• [Presentation] Prospects of Nano-scale Material Science at SACLA (2011)
  • Author(s): S. Wada
  • Organizer: 1^<st> Dis. Meeting on MAXIC@ SACLA
  • Place of Presentation: 佐用町光都
  • Year and Date: 2011-06-09
• [Presentation] 自己組織化単分子膜上で何故内殻励起反応の選択性が向上するか? (2011)
  • Author(s): 田中健一郎, 小川舞, 和田真一, 関谷徹司, 吉田啓晃, 平谷篤也
  • Organizer: 第24回日本放射光学会年会
  • Place of Presentation: つくば市
  • Year and Date: 2011-01-08
• [Presentation] Anionic dissociation of methyl-ester thin films induced by inner-shell excitations (2010)
  • Author(s): S. Wada, A. Hirano, K. Yufu, H. Ishida and K. Tanaka
  • Organizer: 37^<th> Int. Conf. on Vacuum Ultra Violet and X-ray Phys
  • Place of Presentation: Vancouver, Canada
  • Year and Date: 2010-07-15
• [Presentation] Desorption mechanism of anion fragments induced by inner-shell excitations of ester compounds (2010)
  • Author(s): S. Wada, A. Hirano, K. Yufu, H. Ishida, A. Hiraya, K. Tanak
  • Organizer: 第26回化学反応討論会
  • Place of Presentation: 東広島
  • Year and Date: 2010-06-03
• [Presentation] Soft X-ray photo-stimulated ion desorption from self-assembled monolayers of fluorinated benzene derivatives (2010)
  • Author(s): M. Ogawa, S. Wada, K. Yufu, A. Hirano, H. Ishida, A. Hiraya, K. Tanaka
  • Organizer: 第26回化学反応討論会
  • Place of Presentation: 東広島
  • Year and Date: 2010-06-02
• [Presentation] Why chemical bond scission can be controlled well on the self-Assembled monolayer surface? (2010)
  • Author(s): K. Tanaka
  • Organizer: 58^<th> Conf. on Mass Spectrom. Allied Topics(ASMS 2010)
  • Place of Presentation: Salt Lake City, USA
  • Year and Date: 2010-05-24
• [Presentation] Soft X-ray chemistry-Control of chemical bond scission (2010)
  • Author(s): K. Tanaka
  • Organizer: Topical Conference on Interaction of EM Radiation with Atoms, Molecules & Clusters(TC-2010)
  • Place of Presentation: Indore, India
  • Year and Date: 2010-03-04
• [Presentation] Selective chemical bond scission of organic thin films by core electron excitation (2009)
  • Author(s): K. Tanaka
  • Organizer: 5^<th> Sweden-Japan Joint Workshop on Advanced Spectroscopy of Organic Materials for Electronics Applications(ASOMEA-5)
  • Place of Presentation: Krusenberg Herrgard, Sweden
  • Year and Date: 2009-10-02
• [Presentation] Core-excitation induced photochemical reactions of benzene derivative SAMs (2009)
  • Author(s): S. Wada
  • Organizer: 5^<th> Sweden-Japan Joint Workshop on Advanced Spectroscopy of Organic Materials for Electronics Applications(ASOMEA-5)
  • Place of Presentation: Krusenberg Herrgard, Sweden
  • Year and Date: 2009-10-02
• [Presentation] Control of chemical bond scission by site-specific core excitation of surface molecules (2009)
  • Author(s): K. Tanaka
  • Organizer: 26^<th> Europian Conference on Surface Science(ECOSS26)
  • Place of Presentation: Parma, Italy
  • Year and Date: 2009-09-03
• [Book] 質量分析の源流 (2011)
  • Author(s): 田中健一郎,和田真一,他7名,平岡賢三編
  • Total Pages: 243
  • Publisher: (株)国際文献印刷社