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Electron Collision Data of C-H Compound Molecules for Plasma Modeling Framework for Our Research Proposal The IAEA’s Co-ordinated Research Program on ” Atomic and Molecular Data for Plasma Modeling” Hiroshi Tanaka Department of Physics Sophia University, Tokyo, JAPAN 1 st Research Co-ordination Meeting of the IAEA’s Co-ordinated Research Program on ” Atomic and Molecular Data for Plasma Modeling” IAEA, Vienna, Austria 26-28 Sep. 2005
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RESEARCHER’S INSTITUTE Department of Physics Sophia University Tokyo JAPAN CONTACT DETAILS: Telephone: +81-3-3238-3472 Facsimile: +81-3-3238-3341 E-mail: h_tanaka@sophia.ac.jp
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PROPOSED TITLE OF RESEARCH TOPIC ( under Co-ordinated Research Project the research will support ) Electron Collision Data of C-H Compound Molecules for Plasma Modeling
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SUMMARY OF THE PROPOSED RESEARCH Target Molecules: H-C molecules produced from the internal wall materials of fusion chambers Research directions for three year project: 1 st year: compilation and analysis of data already available in literature that relates to this filed of plasma modeling. 2 nd year : analyzing recent data from our collaboration group in conjunction with related data from other laboratories on cross sections from these molecules. 3 rd year: propose directions for experimentalists and theorists to come up with new cross section data that would make the database for each molecule as complete as feasible as relates to the application to the fusion- and plasma processing- plasmas.
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PROJECT PERSONNEL Chief Scientific Investigator: Hiroshi TANAKA (Prof. Sophia Univ. Japan) Other Supporting Scientific Staff: Mineo KIMURA (Prof. Kyushu Univ. JAPAN) Casten MAKOCHEKANWA (Dr. JSPS Fellow JAPAN ) Masamitsu HOSHINO (Dr.Sophia Univ. JAPAN) Hyuck CHO (Prof. Chungnam Nat’l Univ. South KOREA) Michael J. BRUNGER(Prof. Flinders Univ. of Southen AU AU) Stephen J. BUCKMAN(Prof., Australian Nat’l Univ. AU)
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DESCRIPTION OF RESEARCH OBJECTIVES AND ANTICIPATED OUTCOMES Main Objectives: ■ Understanding electron-C-H compound molecule interactions in the fundamental collision processes for Fusion and Plasma processing Plasmas ■ The comprehensive evaluation and analysis of the previous related cross section data available in literature from all over the world within the framework of IAEA International Bulletin on Atomic and Molecular Data for Fusion.
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DESCRIPTION OF RESEARCH OBJECTIVES AND ANTICIPATED OUTCOMES continued ■ Compilation of new data from our group as well as from other research groups into the database. data from our group will be systematically compiled for the more than 30 molecules studied so far for the collision processes: elastic, vibrational and electronic excitations, and total cross sections. ■ Propose new directions for producing missing but necessary experimental and theoretical data for these processes Currently, from a world wide perspective, the data source for these absolute cross sections are from these Australian, South Korean, and Japanese experimental groups involved in this collaboration. Other possible sources may include the Polish, Danish, Spanish, Brazilian, and Switzerland
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WORK PLAN Year 1: Evaluation and analysis of related data available in literature but scattered in different places all over the world within the framework of IAEA International Bulletin on Atomic and Molecular Data for Fusion. Year 2: Compilation and addition of new data from our group as well as from other research groups to the database. In the same process, data from our group will be systematically compiled for the more than 30 molecules studied so far for the collision processes: elastic, vibrational and electronic excitations, and total cross sections. Year 3: Proposal of new directions for producing missing but necessary experimental and theoretical data for these processes related to fusion and plasma processing plasmas.
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Brief description of facilities available Only limited to measurement of absolute cross sections 1) Sophia University (JP): three cross beam spectrometers 2) Flinders University of Southern Australia (AU): two cross beam spectrometers 3) Australian National University (AU): two cross beam spectrometers 4) Chungnam National University (SOK): one cross beam spectrometer 5) Kyushu University (JP): data analysis
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PROPOSED COMMENCEMENT DATE 1 September 2005
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Preliminary stage Review articles after 1990, 1. International Bulletin on Atomic and Molecular Data for Fusion, 42(1992)-58(2000) published by IAEA, 2. Collision Data Involving Hydro-Carbon Molecules, H. Tawara, Y. Itikawa, H. Nishimura, H. Tanaka, and Y. Nakamura, NIFS-DATA-6 July (1990) 3. Atomic Data and Nuclear Data Tables 76 (2000) 1 4. One Century of Experiments on Electron-Atom and Molecule Scattering: a Critical Review of Integral Cross-sections Ⅱ -Polyatomic Moecules, Ⅲ -Hydrocarbons and Halides, G. P. Karwasz, R. S. Brusa, and A. Zecca La Rivista del Nuvo Cimento 24 (1) (4) 2001 5. Analytic Cross Sections for Electron Collisions with Hydrocarbons: CH 4, C 2 H 6, C 2 H 4, C 2 H 2, C 3 H 8, and C 3 H 6, T. Shirai, T. Tabata, H. Tawara, and Y. Itikawa, Atomic Data and Nuclear Data Tables 80, 147-204 (2002) 6. Interaction of Photons and Electrons with Molecules, M.J.Brunger and S.J.Buckman, Photon and Electron Interactions with Atoms, Molecules, and Ions, vilI/17, sub-volume C ed Y. Itikawa Landorf-Beurnstein (2003, Berlin: Springer) p6-118 7. Collision Processes of C 2, 3 H y and C 2, 3 H y Hydrocarbons with electrons and Protons R. K.Janev and D. Reiter, Phys. Plasma 11 (2004) 780 8. Vibrational Excitation of Polyatomic Molecules by Electron Collisions Y. Itikawa, J. Phys. B: At. Mol. Opt. Phys 37 R1-24 (2004)
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Ongoing Data Collection Network
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Data Needs for Electron Interaction with Plasma Processing and Fusion Plasma Gases H.TANAKA, M. HOSHINO, and C. MAKOCHEKANWA Department of Physics Sophia University Tokyo, Japan 1 st Research Co-ordination Meeting of the IAEA’s Co-ordinated Research Program on ” Atomic and Molecular Data fror Plasma Modeling” IAEA, Vienna, Austria 26-28 Sep. 2005
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Collaboration International Chugnam National University ( Prof. Cho S. Korea) Australian National University (Prof. Buckman AU) Flinders University of Southern Australia (Prof. Brunger AU) The Open University (Prof. Mason UK) Domestic Kyushu University (Prof. Kimura, Collaboration Theoretical) NIFS (Prof. Kato under the Japan-Korea CUP program) JAERI (Dr. Kubo under the Fusion Plasma Project in Japan) Tohoku University(Prof. Ueda, SR experiment at Spring-8) RIKEN (Prof. Yamazaki, Highly Charged Ion Research)
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Group Members Dr. M. Hoshino (Dr. Research Associate) Dr. C. Makochekanwa (Dr. JSPS Fellow, Kyushu Univ.) T. Tanaka (D1) H.Kato (M2) K.Nakagawa (M2) Y.Miyamoto (M2) K.Oguri (M2)
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SPring-8 RIKEN Sophia electron photon ion scattered electron ejected electron secondary-photo -Auger-electron positive / negative ion, radical Atom Atom Molecule Molecule Research Sites Surface Surface
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Data providers (Atomic physicists) * theory * experiment Data users in various application fields * fusion science * astrophysics * industrial plasmas * environmental physics * medical (radiotherapy) etc. Data centers data compilation data evaluation (important but not easy) dissemination and updating of database retrievable online database = easy to access, use, find data Data requests Data needs Data provide Data search Hard to find or request data Data search for check International A&M data center network IAEA, NIFS, NIST, ORNL, GAPHIOR, etc. Data provide feedback Views from Database assessed data on electron collision cross sections
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Electron Interaction with Molecule Collision Processes of Interest Quantitative Differential Cross Section Measurements Electron Energy-loss Spectroscopy (EELS): Elastic Scattering DCS Resonant Phenomena in Vibrational Excitation Electronic Excitation Process, GOS Quadra- Pole- Mass Spectroscopy (QMSS) Non-radiative Dissociation Products (Threshold Ionization Spectroscopy) Dissociative Attachment Processes Low Energy Electron Diffraction (LEED ) Surface and Phase Transition
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Definition of various Cross Section ・ Differential Cross Section for channel “n” ・ Integral and Momentum transfer Cross Section Crossed beam method ・ Total Cross Section Transmission experiment Swarm experiment ※ Upper limit of cross sections Boltzmann equation Measurements of electron collision-cross sections
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Collision Data for Molecules by Electron Impact investigated at Sophia University CH 4, C 2 H 6, C 3 H 8, C 2 H 4, C 3 H 4, C 3 H 6 CF 4, C 2 F 6, C 3 F 8, C 2 F 4, c-C 4 F 8, C 6 F 6, C 3 F 6 CF 3 H, CF 2 H 2, CFH 3 CF 3 Cl, CF 3 Br, CF 3 I CF 2 Cl 2, CFCl 3 SiH 4, Si 2 H 6, SiF 4, GeH 4 NF 3, C 60 N 2 O, CO 2, COS, H 2 O, CS 2, XeF 2, HCN F 2 CO
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Activities on Data Compilation NIFS: Compile the previous related data available in literature but scattered in different places all over JAPAN for Plasma Processing JAERI: Provide the electron collision data of the C-H double bond compound molecules for Fusion Our Data Base to be prepared in IAEA,NIFS Report, and AAMOP
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On-going and Near -future Measurements EELS: Elastic Scattering: C 3 H 6 isomers, C 3 F 6 Vibrational Excitation : C 3 F 6, COF 2 Electronic Excitation : C 3 F 6, COF 2, H 2 O, DNA bases Excited Molecular Target: vibratinally excited H 2, CO 2 QMSS: Radical Detection: CH x (X=3 1) from CH 4 Negative Ion Detection: Gas- and Condensed-Phase LEED: Anti-ferromagnetic Surface: NiO, CoO, FeO
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Why C 3 H 6, C 3 F 6, and COF 2 ? Data Base for Alternative Gases in Plasma Etching Process Data Base for Hydro-carbon Molecules near the Edge Plasma of Fusion Plasma
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New trends in processing system design Two approaches have been introduced: Vertically integrated computer-aided design for device processing (VicAddress) (Prof. Makabe’s group, Japan) Intelligent nano-prosessing technology for nanometer-processing techniques with in-time monitoring and simulation (System-on chip (SoC) design) (Prof. Samukawa’s group, Japan) Plasma Processing will be still in core methodology!
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Gas-phase C + A A + + B - A + AB Q(ε) K j Feed Gas Database Governing Equation Source from T. Makabe Modeling flows for plasma processing
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Gases commonly used for plasma etching MaterialsClassificationMolecular species SiFluorides CF 4, SF 6, NF 3, SiF 4, BF 3, CBrF 3, XeF 2 Chlorofluorides CClF 3, CCl 2 F 2, CCl 3 F, C 2 ClF 5, C 2 Cl 2 F 4 Chlorides CCl 4, SiCl 4, PCl 3, BCl 3, Cl 2, HCl Bromides Br 2, HBr Si dioxideFluoride/hydrogen CHF 3, CF 4 +H 2 Fluorocarbons C 2 F 6, C 3 F 8, C 4 F 8 Al alloys Chlorides CCl 4, BCl 3, SiCl 4, Cl 2, HCl Chlorofluorides CCl 2 F 2, CCl 3 F Bromides Br 2, BBr 3 Current database needs to elaborate on the optimum conditions between the device designer and the process engineer.
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Green Chemistry High-performance etching of SiO 2 at high efficiency with small amounts of PFC gases Etching of SiO 2 using alternative gases with low GWP value Cleaning alternative gases for electronics devices with low GWP value (targets in ASET/ RITE/ Mirai / Projects of NEDO in JAPAN) In parallel with the trends, more ecologically friendly processing technology is demanded: (ASET: Association of Super-advanced Electronics Technology) (RITE: Research Institute of Innovative Technology for the Earth) (NEDO:New Energy and Industrial Technology Development Organization)
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Alternative Candidates compared with feed gases commonly used GWP: Global Warming Potential NFPA: National Fire Protection Association
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ITER (International Thermonuclear Reactor) agreed in June to be built in Cadarache, France Data Needs for Carbon impurities (H-C molecules) produced by physical and chemical sputtering CH 3, CH 4, C 2 H 2, C 2 H 4, C 2 H 6, C 3 H 8 Vibrationally (Hot) excited Molecules H 2, D 2
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Electron Collision Cross Section Data e + C 2 H 4 prototype of double bond H-C elastic scattering q m vibrationalexcitation q v electronic excitation q e ionization q i From M. Hayashi
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C 3 X 6 elastic DCS (X = H, F) △:C3H6 ■:C3F6 △:C3H6 ■:C3F6 Double bond X 2 C 2 X 2 (C 2 H 4,C 2 F 4 ) X 2 C 2 XCX 3 (C 3 H 6, C 3 F 6 )
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Neutral Radical Detection Parent neutral CH 4 + CH 3 + CH 2 + CH + C+C+ CH 4 12.614.315.122.225 CH 3 9.815.117.725 CH 2 10.317.420.2 CH13.020.3 C16.8 Table 1. Ionization thresholds e + CH 4 CH 3 + H + e e + CH 3 CH 3 + +2e
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Deduction for unknown DCS
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COF 2 vibrational excitation
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COF 2 Electronic Excitation
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-24- e-e- 600℃ 120 0℃ 250 0℃ Hot Molecular Beam Source Sheath heater Electron Bombardment
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C 1s -1 2 u excitation O 1s -1 2 u excitation Results Comparison
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Outlook EELS: Elastic Scattering: C 3 H 6 C 3 F 6 COF 2 Vibrational Excitation : C 3 H 6 C 3 F 6 COF 2 Electronic Excitation : C 3 F 6 COF 2 (H 2 O, DNA bases) QMSS: Radical Detection: CH x (X = 3 0) from CH 4 Our Data Base to be prepared in IAEA,NIFS Report, and AAMOP
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Future Plan Radical Detection: OH from H 2 O Excited Molecular Target: vibratinally excited H 2,CO 2 Negative Ion Detection: Gas- and Condensed-Phase
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H 2 O vibrational excitation
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H 2 O electronic excitation
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H 2 O GOS
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Alternative CandidatesFeed Gases commonly used GWP: Global Warming PotentialA.L.T: Atmospheric Life Time
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