2007 Fiscal Year Final Research Report Summary
Dynamics of Site-Specific Ion Desorption Reactions
| Project/Area Number |
16205002
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| Research Category |
Grant-in-Aid for Scientific Research (A)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Physical chemistry
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| Research Institution | Hiroshima University |
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Principal Investigator |
TANAKA Kenichiro Hiroshima University, Graduate School of Science, Professor (90106162)
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| Co-Investigator(Kenkyū-buntansha) |
SEKITANI Tetsuji Hiroshima University, Graduate School of Science, Associate Professor (30259981)
WADA Shinichi Hiroshima University, Graduate School of Science, Assistant Professor (60304391)
TAKAHASHI Osamu Hiroshima University, Graduate School of Science, Assistant Professor (60253051)
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| Project Period (FY) |
2004 – 2007
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| Keywords | Soft X-ray / Synchrotron Radiation / Auger Decay / Core Electron Excitation / Photon Stimulated Ion Desorption / Site-Specific Reaction / Self-Assembled Monolayer / Density Functional Theory |
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| Research Abstract |
We investigated site-selective chemical bond scission by core excitation for methyl-ester terminated self-assembled monolayer (SAM) in order to improve the selectivity and to elucidate the dynamics of this reaction, and obtained many important results as follows:
(1) Primary bond scission occurs within ester group and its selectivity becomes much higher than PMMA. We have succeeded to evaluate direct and indirect processes quantitatively and obtained the selectivity is more than 90% for SAM and 60% for PMMA.
(2) From polarization dependent experiments, it was found that ions which desorb selectively indicate significant polarization dependence, while non-selective ions rarely show the dependence. These findings indicate that initial memory of primary excitation is effectively conserved during reactions. From these results we proposed an active control of chemical bond scission just by changing an angle of incident radiation.
(3) Selective bond scission of O-CH_3 could be achieved at both
… More
resonant excitations of o^*(O-CH_3)← C_<1s>(O-CH_3) and O_<1s>(O-CH_3). Distribution of CH_n^+ (n=1-3), however, is different at the position of primary excited atoms. At C excitation, Auger final energy is concentrated within removing CH_3+ and is effectively used for further fragmentation (named as "Hard-Cut"), but at O excitation, Auger energy easily diffuses into the substrate and not effectively used for the fragmentation (named as "Soft-Cut").
(4) The dynamics of resonant core-excited states have been investigated theoretically by DFT theory and succeeded to find systematic relationship between chemical bond and potential gradient in the core-excited state, which plays an important role for the selective bond scission. Some general regularities were found: The gradient of core-excited state becomes more negative with increasing sum of the atomic numbers of bonding pair atoms, atomic number by core-excited atom, and the bond order. These rules are important to predict and design the site-selective bond scission reactions. Less
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Research Products
(178 results)
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[Journal Article] Configuration dependence of photon stimulated ion desworption from methyl ester compounds induced by core excitation2007
Author(s)
H., Kizaki, Y., Matsumoto, H., Ban, K., Morishita, S., Wada, K., Tanaka
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Journal Title
Surf. Sci 601
Pages: 3956-3960
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Electron-ion coincidence spectroscopic study of site-specific fragmentation caused by Si : 2p core-level photoionization of F_3SiCH_2CH_2Si(CH_3)3 vapor2007
Author(s)
S., Nagaoka, G., Prumper, M., Hino, M., Takemoto, Y., Tamenori, J., Harries, I., H., Suzuki, O., Takahashi, K., Okada, K., Tabayashi, X.-J., Liu, T., Lischke, K., Ueda
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Journal Title
Phys. Rev 75
Pages: 020502
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Probing the electron delocal ization in liquid water and ice at attosecond timescales2007
Author(s)
D., Nordlund, H., Ogasawara, H., Bluhm, O., Takahashi, M., Odelius, M., Nagasono, L., G., M., Pettersson, A. Nilsson
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Journal Title
Phys. Rev. Lett 99
Pages: 217406-4
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Auger Decay Calculations with Core-hole Excited State Molecular Dynamics Simulations of Water2006
Author(s)
O., Takahashi, M., Odelius, D., Nordlund, H., Bluhm, A., Nilsson, L., G., M., Pettersson
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Journal Title
J. Chem. Phys 124
Pages: 064307
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Theoretical study of ion desorption from PMMA and PiPAc thin Elms through core-excitation2006
Author(s)
O., Takahashi, K., Tabayashi, S., Wada, R., Sumii, K., Tanaka, M., Odelius, L., G., M., Pettersson
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Journal Title
J. Chem. Phys 124
Pages: 124901(1-8)
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Dissociation mechanisms and dynamics of doubly charged CD_3CN molecules and (CD_3CN)n clusters observed by PEPIPICO spectroscopy2006
Author(s)
C., Harada, S., Tada, K., Yamamoto, H., Yoshida, A., Hiraya, S., Wada, K., Tanaka, K., Tabayashi
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Journal Title
Radiat. Phys. Chem 75
Pages: 2085-2089
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Structure of water adsorbed on the open Cu(110) surface : H-up, H-down, or both2006
Author(s)
T., Schiros, S., Hach, H., Ogasawara, O., Takahashi, H., Ostrom, K., Andersson, L., G., M., Pettersson, A., Hodgson, A., Nilsson
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Journal Title
Chem. Phys. Lett 429
Pages: 415-419
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Inner-shell excitation spectroscopy and fragmentation of small hydrogen-bonded clusters of formic-acid at the oxygen K-edge2006
Author(s)
K., Tabayashi, K., Yamamoto, O., Takahashi, Y., Tamenori, J., R., Harries, T., Gejo, M., Iseda, T., Tamura, K., Honma, I., H., Suzuki, S., Nagaoka, T., Ibuki
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Journal Title
J. Chem. Phys 125
Pages: 194307(1-10)
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Studies of the X-ray Absorption Spectra of Some Methylcyano Esters2005
Author(s)
O., Takahashi, K., Saito, M., Mitani, H., Yoshida, F., Tahara, T., Sunami, K., Waki, Y., Senba, A., Hiraya, L., G., M., Pettersson
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Journal Title
J. Electron Spectros. Rel. Phenom 142
Pages: 113-119
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Molecularly Intact and Dissociative Adsorption of Water on Clean Cu(110) : A Comparison with the Water/Ru(001) system2005
Author(s)
K., Andersson, A., Gomez, C., Glover, D., Nordlund, H., Ostrom, T., Schiros, O., Takahashi, H., Ogasawara, L., G., M., Pettersson, A., Nilsson
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Journal Title
Surf. Sci 585
Pages: 183-189
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Polarization-dependent dissociation selectively induced by core-electron excitation in methyl ester terminated self-assembled monolayer2005
Author(s)
H., Kizaki, S., Wada, E., O., Sako, R., Sumii, S., Waki, K., Isari, T., Sekitani, K., Tanaka
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Journal Title
J. Electron Spectros. Rel. Phenom 144-147
Pages: 447-451
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Dissociation mechanisms and dynamics of core-excited (N_2O) cluster2005
Author(s)
K., Tabayashi, S., Tada, J., Aoyama, K., Saito, H., Yoshida, S., Wada, A., Hirava, K., Tanaka
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Journal Title
J. Electron Spectros. Rel. Phenom 144-147
Pages: 179-182
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Ion desorption of surface-oriented methyl-ester compounds using a self-assembled monolayer by core-electron excitations : Polarization - dependence measurements2005
Author(s)
S., Wada, R., Sumii, H., Kizaki, Y., Iizuka, Y., Matsumoto, T., Sekitani, K., Tanaka
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Journal Title
Surf. Sci 593
Pages: 283-290
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Production of methyl-oxonium ion and its complexes in the core-excited (HC(O)OCH_3)n clsters : H/H+ transfer from the α carbonyl2005
Author(s)
S., Tada, C., Harada, S., Wada, A., Hiraya, K., Tanaka, K., Tabayashi
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Journal Title
J. Chem. Phys 123
Pages: 124309(1-9)
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Study of adsorption structure of benzene and toluene on Si(111)7×7 surfaces2004
Author(s)
H., Tomimoto, T., Sekitani, R., Sumii, E., O., Sako, S., Wada, K., Tanaka
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Journal Title
Surf. Sci 566-568
Pages: 664-670
Description
「研究成果報告書概要(欧文)」より
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[Journal Article] Molecular adsorption of (CH_3)2S on Ag(111) studied by S K-edge XAFS and XPS2004
Author(s)
S., Yagi, Y., Nakano, E., Ikenaga, S., A., Sardar, J., A., Syed, K., Tanaka, E., Hashimoto, M., Taniguchi
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Journal Title
Surf. Sci 566-568
Pages: 746-750
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Control of chemical bond scission by site-specific core excitation2008
Author(s)
K., Tanaka, S., Wada, H., Kizaki, Y., Matsumoto, R., Sumii, T., Sekitani
Organizer
12th Hiroshima Int. Symp. on Synchrotron Radiation
Place of Presentation
Hiroshima
Year and Date
2008-03-13
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Control of chemical bond scission by site-specific core excitation2007
Author(s)
K., Tanaka, S., Wada, H., Kizaki, Y., Matsumoto, R., Sumii, T., Sekitani
Organizer
2nd Asia-Oceania Forum for Synchrotron Radiation Research
Place of Presentation
Taiwan
Year and Date
2007-11-02
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Adsorption and its structure of methyl mercaptoacetate on Cu(111) surface by XPS and NEXAFS spectroscopy2006
Author(s)
S., Wada, M., Takigawa, K., Matsushita, H., Kizaki, K., Tanaka
Organizer
24th European Conf. on Surface Science (ECOSS-20)
Place of Presentation
Paris, France
Year and Date
2006-09-05
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Configuration dependence of photon stimulated ion desorption from methyl ester compounds induced by core excitation2006
Author(s)
H., Kizaki, Y., Matsumoto, H., Ban, K., Morishita, S., Wada, K., Tanaka
Organizer
24th European Conf. on Surface Science (ECOSS-20)
Place of Presentation
Paris, France
Year and Date
2006-09-05
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Photon stimulated neutral desorption from methyl-ester terminated self-assembled monolayer by resonant C1s excitation2006
Author(s)
Y., Matsumoto, K., Morishita, K., Matsushita, S., Wada, K., Tanaka
Organizer
24th European Conf. on Surface Science (ECOSS-20)
Place of Presentation
Paris, France
Year and Date
2006-09-05
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Polarization dependence of photon stimulated ion desorption in carbon core-excited ethyl-ester terminated self-assembled monolayer2006
Author(s)
Y., Matsumoto, S., Wada, K., Kawabata, H., Kizaki, R., Sumii, K., Tanaka
Organizer
24th European Conf. on Surface Science (ECOSS-20)
Place of Presentation
Paris, France
Year and Date
2006-09-05
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Theoretical Study of ion desorption from PMMA and PiPAc thin films through core-excitation2006
Author(s)
O., Takahashi, K., Tabayashi, S., Wada, R., Sumii, K., Tanaka, M., Odelius, L., G., M., Pettersson
Organizer
5th Int. Symp. Ultrafast Surface Dynamics (USD-5)
Place of Presentation
Abashiri, Japan
Year and Date
2006-05-25
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Site-specific ionic dissociation for methyl ester terminated organic films on silver in C1s core-excitation region2005
Author(s)
H., Kizaki, K., Kawabata, M., Takigawa, R., Sumii, S., Wada, T., Sekitani, K., Tanaka
Organizer
9th Hiroshima Int. Symp. on Synchrotron Radiation
Place of Presentation
Hiroshima
Year and Date
2005-03-10
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Study of electronic states in shape resonance regions for organic films using is photoelectron spectroscopy2005
Author(s)
Y., Iizuka, S., Wada, H., Murakami, M., Kuratomi, M., Takigawa, T., Sekitani, K., Tanaka
Organizer
9th Hiroshima Int. Symp. on Synchrotron Radiation
Place of Presentation
Hiroshima
Year and Date
2005-03-10
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Ionic desorption mechanism in core-electron excitation of surface-oriented methyl ester compound using self-assembled monolayer : polarization-dependence measurement2004
Author(s)
S., Wada, R., Sumii, H., Kizaki, Y., Iizuka, Y., Matsumoto, T., Sekitani, K., Tanaka
Organizer
10th Int. Workshop on Desorption Induced by Electronic Transitions (DIET-10)
Place of Presentation
Susono, Japan
Year and Date
2004-11-10
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Study on ion desorption process of methyl ester terminated self-assembled monolayer induced by core excitation using Auger electron-photoion coincidence spectroscopy2004
Author(s)
T., Sekitani, H., Tsuchie, Y., Nanbu, S., Waki, S., Wada, K., Tanaka
Organizer
10th Int. Workshop on Desorption Induced by Electronic Transitions (DIET-10)
Place of Presentation
Susono, Japan
Year and Date
2004-11-10
Description
「研究成果報告書概要(欧文)」より
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[Presentation] Polarization-dependent dissociation selectively induced by core-electron excitation in methyl ester terminated self-assembled monolayer2004
Author(s)
S., Wada, R., Sumii, H., Kizaki, Y., Matsumoto, E., O., Sako, T., Sekiguchi, T., Sekitani, K., Tanaka
Organizer
14th Int. Conf. on Vacuum Ultraviolet Radiation Physics (VUV-XIV)
Place of Presentation
Cairns, Australia
Year and Date
2004-07-22
Description
「研究成果報告書概要(欧文)」より
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