Tilmann Märk Universität Innsbruck
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1 Tilmann Märk Universität Innsbruck
2 Slowakia Hungary Germany Tyrol Italy Czech republic Vienna Slowenia Switzerland
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4 Institut für Ionenphysik und Angewandte Physik EURATOM ÖAW Ion Physics / Plasma Physics Clusterphysics Mass Spectrometry Environmental Physics and Analysis
5 Institut für Ionenphysik Elementary processes considered: 1. Inelastic electron interactions with atoms/molecules/nanoparticles (ionization and attachment) 2. Ion/surface interaction 1. Intrinsic fundamental interest 2. Provide data needed for plasma modelling and diagnosis 3. Radiation damage EURATOM ÖAW Data acquisition Data analysis and assessment Data compilation (ADAS, IAEA)
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7 4.Photons
8 Origin of life (photosynthesis) Life in space Radiation damage at a molecular level Improved radiation therapy
9 The genotoxic effects of ionizing radiation (α,β,γ,χ) in living cells (therapeutic, diagnostic) are not only due to the primary impact. Single and double strand breaks may be induced by secondary species: =secondary electrons with kinetic energies below about 20 ev thermalized and solvated by inelastic collisons within <<10-12 s =4x10 4 electrons per 1 MeV primary
10 EURATOM ÖAW Outline Part I: Fundamentals A. Ionization processes and Ions produced B. Ionization mechanisms Part II: Kinetics and energetics for the production of cations and anions Part III: Electron attachment Part IV: Ion/surface interactions
11 EURATOM ÖAW Part I: Fundamentals A. Ionization processes and Ions produced Direct Ionization Indirect ionization Stable ions unstable (metastable) ions Singly-charged ions Multiply-charged ions Parent ions fragment ions Cations - anions
12 Electron-Particle Interaction e + atom : e + molecule : e + cluster : electronic excitation electronic excitation vibrational excitation rotational excitation dissociation multiple collisions intra-cluster reactions
![Electron-Particle Interaction ABC + e [ABC + ]* A + + BC + KER](/docs-images/91/106328645/images/13-0.jpg "Primary ionization event Energy storage and disposal Final reaction")
13 Electron-Particle Interaction ABC + e [ABC + ]* A + + BC + KER Primary ionization event Energy storage and disposal Final reaction products
14 Electron impact ionization processes A + e A + e elastic scattering A* + e excitation A** + e double excitation (A** A + + e) A + + 2e ionization A +* + 2e excited ion (A +* A ++ + e) A e double ionization A - + hv attachment
15 Electron impact ionization processes AB + e AB + e elastic scattering AB* + e excitation AB** + e double excitation (AB** AB + + e) AB + + 2e ionization AB +* + 2e excited ion (AB +* AB ++ + e) AB e double ionization AB - + hv attachment (AB - A - + B) AB + e AB(v,k) + e vibrational, rotational excitation A + B dissociation A + + B + 2e dissociative ionization A + + B + + 3e dissociative double ionization A + + B +- + e ion pair formation AB e double ionization
16 Direct and indirect ionization processes
17 EURATOM ÖAW Part I: Fundamentals B. Ionization mechanisms Franck Condon principle Unimolecular dissociation
18 V(r) in ev Ionization mechanism I: The Franck Condon principle H 2 + e H 2 + H 2 + H H 2 + H 2 + H + H ev d = Distance in 10-8 cm E=100 ev: v=6x10 8 cm/s; t=s/v=10-8 /6x10 8 ~2x10-17 s «t v ~10-14 s
19 Electron impact ionization: mechanism The Franck Condon principle Reflection principle Franck Condon Factors
20 Electron impact ionization: mechanism The Franck Condon Range and Cases E=100 ev: v=6x10 8 cm/s; t=s/v=10-8 /6x10 8 ~2x10-17 s «t v ~10-14 s
21 Electron impact ionization: mechanism The Franck Condon principle
22 V(r) in ev H 2 + e H 2 + H 2 + H + v a H 2 + H 2 + H + H (18.08) (15.47) BE (H-H + ) = ev Distance in 10-8 cm
23 AE and BE of molecules
24 HEM data analysis: O 3 + e O 3 + (O 3 ) 2 + e (O 3 ) 2 + Fit function: σ(e) = b + σ o (E-IE) p 100 O 3 + /O 3 10 ΑΕ: ± 0.02 ev Ion signal (arb. units) (O 3 ) 2 + /(O 3 ) n ΑΕ: ± 0.2 ev Corrected electron energy (ev)
25 HEM data analysis: O 3 + e O 3 + (O 3 ) 2 + e (O 3 ) 2 + Binding energy of ozone dimer ion: O 3 + IE(O + 3 ) 12.70(2) ev O 3 D(O O 3 ): 2.70 ev IE((O 3 ) + 2 ) 10.10(22) ev D(O 3 - O 3 ): 0.13 ev O O 3 (O 3 ) 2 + (O 3 ) 2
26 dimer geometry twisted boat O 2 O 4+
27 Photoelectron spectroscopy:adiabatic & vertical IE
28 Photoelectron spectroscopy:adiabatic & vertical IE
29 Ionization mechanism II: Vibrational predissociation ABC + e parent & fragment ions Decay paths for parent ion formed: ABC +* A + + BC A + + B + C AB + + C A + + B + C A + B + + C A + BC + A + B + + C A + B + C + AB + C + A + B + C +
30 Ionization mechanism II: Vibrational predissociation C n H 2n+2 + e parent & fragment ions
31 Ionization mechanism II: Vibrational predissociation C 3 H 8 + e parent & fragment ions (decay paths & relative abundance in mass spectrum)
32 Unimolecular (metastable) dissociation 3 major mechanisms: 1. Vibrational (statistical) predissociation 2. Electronic predissociation 3. (Rotational) tunneling through a barrier
33 Vibrational (statistical) predissociation
34 Electronic predissociation: Transition forbidden by (i) some selection rule or (ii) hindered by small overlap integral
35 Tunneling through barrier
36 Tunneling through barrier V eff effective potential energy combination of V plus rotational energy of diatomic V potential for L=0 J =K rotational quantum numbe
37 Electron impact ionization: mechanism Time evolution of the ionization process
38 Electron impact ionization: mechanism Time evolution of the ionization process
39 Diamond Graphite Buckminster Fullerene C 60 Strictly speaking only fullerenes are made exclusively from carbon.
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42 C 60 + e C 60 + C 58 + BE + KS IE = 7.6 ev AE = 43.7 ev
43 + Experiment (gas phase) C 58 + C2 Experiment (solid/surface) Theory C Dissociation energy (ev) 0 Laskin 97 Hansen 97 Sommer 96 Wörgötter 96 Weis 96 Laskin 95 Sommer 95 Leifer 95 Baba 95 Kolodney 95b Kolodney 95a Novoa 94 Xu 94 Hamza 94 Kolodney 94 Eckhoff 93 Foltin 93 Zhang 92 Stanton 92 Yi 92 Whetten 92 Busmann 92 Yoo 92 Wurz 92 Sandler 92 Beck 91 Lifshitz 91 Klots 91 Radi 90 Situation in 1997: about 30 published results on the C 60 binding energy no agreement within experiment and no agreement between theory and experiment
44 experiment, original recent experiment, experiment, re-analyzed original recent experiment, original Tomita 01 Matt 99b Matt 99a Laskin 98 Laskin 97 Hansen 97 Sommer 96 Wörgötter 96 Weis 96 Laskin 95 Leifer 95 Kolodney 95b Kolodney 95a Foltin 93 Busmann 92 Yoo 92 Wurz 92 Sandler 92 Lifshitz 91 Klots 91 Radi Binding energy (ev)
45 Final result for the C 60+ binding energy Experiment: 17 Measurements - which have been analysed by using the complete today s knowledge- yield a binding energy (mean value) of 10.0 ± 0.2 ev Theory: A.D.Boese and G.E.Scuseria have carried out very accurate D(ensity)F(unctional)T(heory) calculations and obtain for the ionic C 60+ binding energy 10.2 ev
46 e 500 hν 61 ev Infrared multiphoton excitation, dissociation and ionization of C 60, M.Hippler, M.Quack, R.Schwarz, G.Seyfang, S.Matt, T.D.Märk, Chem.Phys.Lett. 278(1997)111
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48 Metastable decay of cluster ions: Results: Absolute binding energies for fullerenes C n+, 42 n BE (ev) C n fullerene size present measurements S.Tomita, J.A. Andersen, C Gottrup, P.Hvelplund and U.V.Pedersen :'Dissociacion Energy for C 2 los from Fullerene Cations in a Storage Ring' Physical RevieW Letters, 13 Aug. 2001, Vol 87, nr. 7 P.E.Barran, S.Firth, A.J.Stace, H.W.Kroto, K.HAnsen,and E.E.B. Campbell, Int. J. Mass Spectrom. Ion Process. 167/168,127 (1997)
49 C 60 + e parent & fragment ions C C C C C 60 + Ion current (Hz) Mass per charge (Thomson)
50 C 60 + e multiply charged ions 13 C 12 C59 7+ & 13C 2 12C Mass per charge (Thomson) Ion signal (Hz) C17 C 12 C16, 2+, C C50 C 12 C C C C C2 C , C C C C2 12 C58 7+
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