Highly accurate theoretical spectroscopy for inner-shell electronic processes

• Project/Area Number: 21350019
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: National Institutes of Natural Sciences Okazaki Research Facilities
• Principal Investigator: EHARA Masahiro 大学共同利用機関法人自然科学研究機構(岡崎共通研究施設), 計算科学研究センター, 教授 (80260149)
• Co-Investigator(Kenkyū-buntansha): KOSUGI Nobuhiro 分子科学研究所, 光分子科学研究領域, 教授 (20153546)
• Project Period (FY): 2009 – 2011
• Project Status: Completed (Fiscal Year 2011)
• Budget Amount: ¥18,590,000 (Direct Cost: ¥14,300,000、Indirect Cost: ¥4,290,000); Fiscal Year 2011: ¥5,460,000 (Direct Cost: ¥4,200,000、Indirect Cost: ¥1,260,000); Fiscal Year 2010: ¥5,980,000 (Direct Cost: ¥4,600,000、Indirect Cost: ¥1,380,000); Fiscal Year 2009: ¥7,150,000 (Direct Cost: ¥5,500,000、Indirect Cost: ¥1,650,000)
• Keywords: 内殻電子過程 / 電子状態理論 / 共鳴状態 / オージェ過程 / 表面光化学 / 脱励起過程

Research Abstract

We performed theoretical inner-shell spectroscopy in which new inner-shell electronic states and complex electronic states were investigated by analyzing the recent experimental observations obtained using free electron laser and multiple coincidence spectroscopy. We proposed the double core-hole spectroscopy and established the chemical concept of the relaxation and inter-atomic relaxation energies in the double core-hole states. We also developed accurate electronic structure theories for describing multi-electron processes and resonance states which are relevant for the inner-shell electronic processes. We proposed the method for analyzing the photoelectron spectroscopy of surface-molecule interacting system and elusidated the importance of electron transfer.

Research Products

• [Journal Article] Sommerfeld, CAP/SAC-CI Method for Calculating Resonance States of Metastable Anions (2012)
  • Author(s): M. Ehara, T.
  • Journal Title: Chem. Phys. Lett Volume: 537 Pages: 107-112
  • DOI: 10.1016/j.cplett.2012.03.104
  • Peer Reviewed
• [Journal Article] SAC-CI and EOM-CC studies of electronically excited states of copper tetrachloride and copper tetrabromide dianions (2012)
  • Author(s): M.Ehara, P.Piecuch, J.J.Lutz, J.R.Gour
  • Journal Title: Chem.Phys. Volume: (in press) Pages: 94-110
  • DOI: 10.1016/j.chemphys.2011.09.022
  • Peer Reviewed
• [Journal Article] Double Core-Hole Spectroscopy for Chemical Analysis with an Intense X-Ray Femtosecond Laser (2011)
  • Author(s): Nora Berrah, 和田真一, 他18名
  • Journal Title: PNAS (Proceedings of National Academy of Sciences) Volume: 108(41) Issue: 41 Pages: 16912-16915
  • DOI: 10.1073/pnas.1111380108
  • Peer Reviewed
• [Journal Article] Auger Decay of Molecular Double Core Hole States (2011)
  • Author(s): M. Tashiro, K. Ueda, M. Ehara
  • Journal Title: J. Chem. Phys Volume: 135 Issue: 15 Pages: 154307-154307
  • DOI: 10.1063/1.3651082
  • Peer Reviewed
• [Journal Article] Molecular Double Core Hole Electron Spectroscopy of Nucleobases (2011)
  • Author(s): O. Takahashi, M. Tashiro, M. Ehara, K. Yamasaki, K. Ueda
  • Journal Title: J. Phys. Chem Volume: A115 Issue: 44 Pages: 12070-12082
  • DOI: 10.1021/jp205923m
  • Peer Reviewed
• [Journal Article] Symmetry and Vibrationally Resolved Absorption Spectra Near the N K Edge of N_2O : Experiment and Theory (2011)
  • Author(s): M. Ehara, H. Nakatsuji, K. Ueda, et al
  • Journal Title: Phys. Rev Volume: A83 Issue: 6 Pages: 1129-1134
  • DOI: 10.1103/physreva.83.062506
  • Peer Reviewed
• [Journal Article] Theoretical spectroscopy on K^<-2>, K^<-1>L^<-1>, and L^<-2> double core hole states of SiX_4 (X=H, F, Cl, and CH_3) molecules (2011)
  • Author(s): O.Takahashi, M.Tashiro, M.Ehara, K.Yamasaki, K.Ueda
  • Journal Title: Chem.Phys. Volume: 384 Issue: 1-3 Pages: 28-25
  • DOI: 10.1016/j.chemphys.2011.04.015
  • Peer Reviewed
• [Journal Article] Theoretical spectroscopy of O ls and N ls excited states of N_2O (2011)
  • Author(s): M.Ehara, H.Nakatsuji, K.Ueda, et al
  • Journal Title: J.Phys. : Conf.Ser. Volume: 288
  • Peer Reviewed
• [Journal Article] Excited-state geometry and vibrational frequency studied by the analytical energy gradients of the SAC-CI method I, application to HAX type molecules (2011)
  • Author(s): M.Ehara, F.Oyagi, Y.Abe, R.Fukuda, H.Nakatsuji
  • Journal Title: J.Chem.Phys. Volume: 135 Issue: 4
  • DOI: 10.1063/1.3617233
  • Peer Reviewed
• [Journal Article] Theoretical Spectroscopy of O 1s and N 1s excited states of N_2O (2011)
  • Author(s): M.Ehara, T.Horikawa, R.Fukuda, H.Nakatsuji, T.Tanaka, M.Hoshino, H.Tanaka, K.Ueda
  • Journal Title: J.Phys.Conf.Series Volume: in press
  • Peer Reviewed
• [Journal Article] Double Core-Hole Electron Spectroscopy for Open-Shell Molecules : Theoretical Perspective (2010)
  • Author(s): M. Tashiro, M. Ehara, K. Ueda
  • Journal Title: Chem. Phys. Lett Volume: 496 Pages: 217-222
  • DOI: 10.1016/j.cplett.2011.11.062
  • Peer Reviewed
• [Journal Article] Double Core Hole Creation and Subsequent Auger Decay in NH_3 and CH_4 Molecules (2010)
  • Author(s): J. H. D. Eland, M. Tashiro, P. Linusson, M. Ehara, K. Ueda, R. Feifel
  • Journal Title: Phys. Rev. Lett Volume: 105 Issue: 21
  • DOI: 10.1103/physrevlett.105.213005
  • Peer Reviewed
• [Journal Article] Molecular Double Core-Hole Electronic Spectroscopy for Chemical Analysis (2010)
  • Author(s): M. Tashiro, M. Ehara, H. Fukuzawa, K. Ueda, C. Buth, N. Kryzhevoi, L. S. Cederbaum
  • Journal Title: J. Chem. Phys Volume: 132 Issue: 18
  • DOI: 10.1063/1.3408251
  • Peer Reviewed
• [Journal Article] The Effect of Vibrational Motion on the Dynamics of Shape Resonant Photoioniz ation of BF_3 Leading to the E^2A_1 State of BF_3^+ (2010)
  • Author(s): R.R.Lucchese, R.Montuoro, K.Kotsis, M.Tashiro, M.Ehara, J.D.Bozek, A.Das, E.D.Poliakoff
  • Journal Title: Mol.Phys. Volume: 108 Pages: 1055-1067
  • Peer Reviewed
• [Journal Article] Vibrational Spectra and Geometry Relaxation in Core-Electronic Processes of N_2O and CO_2 (2010)
  • Author(s): M.Ehara, K.Ueda
  • Journal Title: J.Phys.Conf.Series Volume: 235
  • Peer Reviewed
• [Journal Article] Molecular Double Core-Hole Electronic Spectroscopy for Chemical Analysis (2010)
  • Author(s): M.Tashiro, M.Ehara, H.Fukuzawa, K.Ueda, C.Buth, N.Kryzhevoi, L.S.Cederbaum
  • Journal Title: J.Chem.Phys. Volume: 133
  • Peer Reviewed
• [Journal Article] Double Core-Hole Electron Spectroscopy for Open-Shell Molecules : Theoretical Perspective (2010)
  • Author(s): M.Tashiro, M.Ehara, K.Ueda
  • Journal Title: Chem.Phys.Left. Volume: 496 Pages: 217-222
  • Peer Reviewed
• [Journal Article] Double Core Hole Creation and Subsequent Auger Decay in NH_3 and CH_4 Molecules (2010)
  • Author(s): J.H.D.Eland, M.Tashiro, P.Linusson, M.Ehara, K.Ueda, R.Feifel
  • Journal Title: Phys.Rev.Lett. Volume: 105
  • Peer Reviewed
• [Journal Article] Low-lying Valence Excited States of Open-shell Triatomic Molecules Studied Using the Electron-attached and Ionized SAC-CI and EOM-CC Methodologies (2009)
  • Author(s): M. Ehara, J. R. Gour, P. Piecuch
  • Journal Title: Mol. Phys Volume: 107 Issue: 8-12 Pages: 871-880
  • DOI: 10.1080/00268970802672668
  • Peer Reviewed
• [Journal Article] Relativistic Effect in the K-shell Ionizations : SAC-CI general-R Study Based on DK2 Hamiltonian (2009)
  • Author(s): M. Ehara, K. Kuramoto, H. Nakatsuji
  • Journal Title: Chem. Phys Volume: 356 Issue: 1-3 Pages: 195-198
  • DOI: 10.1016/j.chemphys.2008.10.029
  • Peer Reviewed
• [Journal Article] High-precision Ab initio Core-level Spectroscopy (2009)
  • Author(s): M.Ehara
  • Journal Title: J.Phys.Conf.Series. 194
  • Peer Reviewed
• [Journal Article] Low-lying Valence Excited States of Open-shell Triatomic Molecules Studied Using the Electron-attached and Ionized Symmetry-Adapted Cluster-Configuration Interaction and Equation-of-Motion Coupled Cluster Methodologies (2009)
  • Author(s): M.Ehara, J.R.Gour, P.Piecuch
  • Journal Title: Mol.Phys. 107 Pages: 871-880
  • Peer Reviewed
• [Journal Article] Relativistic Effect in the K-shell Ionizations : SAC-CI general-R Study Based on DK2 Hamiltonian (2009)
  • Author(s): M.Ehara, K.Kuramoto, H.Nakatsuji
  • Journal Title: Chem.Phys. 356 Pages: 195-198
  • Peer Reviewed
• [Presentation] Recent Progress and Applications of SAC-CI (2011)
  • Author(s): M. Ehara
  • Organizer: The 5^<th> Asian Pacific Conference of Theoretical & Computational Chemistry
  • Place of Presentation: Rotorua, New Zealand
• [Presentation] Theoretical Spectroscopy and Photophysical Chemistry by SAC-CI (2011)
  • Author(s): M. Ehara
  • Organizer: Recent Advances in Many-Electron Theory II-2011
  • Place of Presentation: India
• [Presentation] Theoretical Spectroscopy on Photo-functional Molecules with SAC-CI (2011)
  • Author(s): M.Ehara
  • Organizer: The 4^<th> Japan-Czech-Slovak Symposium
  • Place of Presentation: Prague, Czech
• [Presentation] The SAC-CI Method : Theory and Applications (2011)
  • Author(s): M.Ehara
  • Organizer: The 8^<th> Thai Summer School of Computational Chemistry
  • Place of Presentation: Chiang Mai, Thailand
• [Presentation] Theoretical Spectroscopy and Photophysical Chemistry Based on Electronic Structure Theory (2011)
  • Author(s): M.Ehara
  • Organizer: ENSCP-IMS joint symposium
  • Place of Presentation: Paris, France
• [Presentation] Theoretical Spectroscopy and Photophysical Chemistry by SAC-CI (2011)
  • Author(s): M.Ehara
  • Organizer: Recent Advances in Many-electron Theory II-2011
  • Place of Presentation: Kolkata, India
• [Presentation] Theoretical Fine Spectroscopy and Photo-Physical Chemistry Studied by the SAC-CI Method (2010)
  • Author(s): M. Ehara
  • Organizer: Pacifichem 2010, Symposium# 10 : Computational Quantum Chemistry : Theory and Interactions with Experiment
  • Place of Presentation: Hawaii, USA
• [Presentation] Theoretical Fine Spectroscopy and Photophysical Chemistry with the SAC-CI Method (2010)
  • Author(s): M.Ehara
  • Organizer: Pacifichem 2010 Congress ; Symposium for "Computational Quantum Chemistry : Theory and Interactions with Experiment"
  • Place of Presentation: Hawaii, USA
• [Presentation] Photophysical Chemistry based on the SAC-CI Method (2010)
  • Author(s): M.Ehara
  • Organizer: The 1st Chlalongkorn-Institute for Molecular Science Joint Symposium
  • Place of Presentation: Bangkok, Thailand
• [Presentation] Theoretical Fine Spectroscopy and Photophysical Chemistry with the SAC-CI Method (2010)
  • Author(s): M.Ehara
  • Organizer: The 15th International Workshop Quantum Systems in Chemistry and Physics (QSCP-XV)
  • Place of Presentation: Cambridge, UK
• [Presentation] Theoretical Spectroscopy for Single and Double Core-Hole Ionization (2010)
  • Author(s): M.Ehara
  • Organizer: Recent Advances in Many-Electron Theories
  • Place of Presentation: Shankarpur, India
• [Presentation] Theoretical Fine Spectroscopy for Valence to Core-electron Chemistry and Dynamics (2009)
  • Author(s): M. Ehara
  • Organizer: The 4^<th> Asian Pacific Conference of Theoretical & Computational Chemistry
  • Place of Presentation: Port Dickson, Malaysia
• [Presentation] High-precision Theoretical Spectroscopy for Biological Chemosensor, Organic Light-Emitting Diodes, and Inner-shell Electronic Processes (2009)
  • Author(s): M. Ehara
  • Organizer: The 14^<th> International Workshop Quantum Systems in Chemistry and Physics(QSCP-XVI)
  • Place of Presentation: Madrid, Spain
• [Presentation] Core-level Theoretical Fine Spectroscopy (2009)
  • Author(s): M.Ehara
  • Organizer: The 3-rd Japan-Czech-Slovakia Joint Symposium for Theoretical/Computational Chemistry
  • Place of Presentation: Bratislava, Slovakia
• [Presentation] High-precision Ab initio Core-level Spectroscopy (2009)
  • Author(s): M.Ehara
  • Organizer: XXVI ICPEAC International Conference
  • Place of Presentation: Kalamazoo, Michigan, U.S.A
• [Book] 高精度電子状態理論による光機能分子の物性化学,未来材料 (2012)
  • Author(s): 江原正博,福田良一
  • Publisher: エヌ・ティー・エス
• [Book] Development of SAC-CI general-R Method for Theoretical Fine Spectrosocpy, in Recent Progress in Coupled Cluster Methods : Theory and Applications (2010)
  • Author(s): M. Ehara, H. Nakatsuji
  • Publisher: Springer
• [Book] Development of SAC-CI general-R Method for Theoretical Fine Spectroscopy in Recent Progress in Coupled Cluster Methods : Theory and Applications (2010)
  • Author(s): M.Ehara, H.Nakatsuji
  • Total Pages: 34
  • Publisher: Springer
• [Remarks] ホームページ研究室HP
  • URL: http://tc.ims.ac.jp
• [Remarks]
  • URL: http://tc.ims.ac.jp/research-j.html