Charge transfer processes in atom-molecule collision experiments
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1 Charge transfer processes in atom-molecule collision experiments Paulo Limão-Vieira, F Ferreira da Silva and G García Department of Physics, Universidade NOVA de Lisboa, Portugal and Consejo Superior de Investigaciones Científicas (CSIC), Madrid, Spain IAEA Technical Meeting Vienna, 20 December
2 The Atomic and Molecular Collisions Laboratory Asst. Prof. Filipe Ferreira da Silva Dr. Krystyna Regeta, Post-Doc PhD students: Mr. Tiago Cunha, PT Ms. Emanuele Lange, BR Ms. Mónica Mendes, PT Ms. Alexandra Loupas, PT Ms. Rebeca Meißner, D Funding through several schemes: IF-FCT IF/00380/2014 UID/FIS/00068/2013 PD/00193/2012 Technicians: Mr. João Faustino Mr. Afonso Moutinho FY2016 JSPS Invitation Fellowship 2
3 Our most close collaborations CSIC Madrid, ES Gustavo García University of Innsbruck, AT Paul Scheier Stephan Denifl Sophia University Tokyo, JP Hiroshi Tanaka Masamitsu Hoshino Flinders University, AU Michael Brunger Université de Lyon, FR Marie Christine Bacchus Czech Academy of Sciences, CZ Juraj Fedor 3
4 Data for plasma applications Elastic DCS; ICS; Total Cross Sections (experiment and theory); Electronic Excitation (experiment and theory) / high-resolution VUV spectroscopy Japan-Portugal-Spain-Australia (from 2003): GeF 4 ; SiF 4, CF 4 ; BF 3 ; C 4 F 6 ; CF 3 Cl; CF 2 Cl 2 ; CFCl 3 ; 1,3-C 4 F 6, c-c 4 F 6 and 2-C 4 F 6 ; CCl4; F 2 CO; C 2 F 4 COS; CS 2 ;H 2 O; CH 4 ; SiH 4 ; GeH 4 ; C 6 H 6 ; CH 3 F; CH 3 Cl; CH 3 Br; CH 3 I; O 2 UK-Portugal (2006): CF 3 I, C 2 F 4 and CF x (x = 1-3) radicals 4
5 Overview Motivation Negative ion formation Introduction Experimental set-up Results Conclusions electron transfer ion-pair formation acetic acid pyrimidines nitromethane 5
6 Motivation Collisional ionisation processes between atoms A and molecules BC A + + BC (1) IPF by charge transfer A + BC + (2) IPF by charge transfer A + + B + C (3) IPF by charge transfer/dissociative IPF A + + (B + C) + e (4) Ionisation A + BC AB + + C + e (5) AB + + C (6) AB + C + + e (7) Chemiionisation w/ rearrangement Chemiionisation w/ rearrangement Chemiionisation w/ rearrangement ABC + + e (8) Associative ionisation A + B + + C (9) Collision induced polar dissociation 6
7 Motivation Negative ions formation from molecular targets Electron transfer in atom-molecule collisions: K o hyp + AB [K + + AB ]* K + + AB K + + A + B K + + A + B K + AB* Studying chemical reactions understand radiation induced damage; Collisional excitation and dissociation; Site- and bond-selectivity (pyrimidines, purines, imidazole); The role of the collision complex pathways; Competitive (even concerted) fragmentation mechanisms in pyrimidines and purines. 7
8 Motivation access to parent molecular states which are not accessible in EA (states positive EA); role of vibrational excitation of the parent neutral molecule - collision dynamics DEA - resonances; direct and statistical dissociation; 8
9 E lab 1keV The crossed molecular beam setup in Lisbon 9
10 Complex internal rearrangement yielding OH - 1,00 0,75 0,50 a) OH CH 3 COOH CH 3 COO E lab = 100 ev 0,25 CH 3 Intensity (arb. units) 0,00 1,00 0,75 0,50 0,25 0,00 1,00 0,75 b) c) OH CH 3 OH OD CH 3 COOD CD 3 COOH CH 3 COO 0,50 0,25 CDH OD / CD 3 CD 3 COO 0,00 π* C=O σ* OH (?) Mass (m/z) Meneses, Widmann, Cunha, Gil, da Silva, Calhorda and PLV. Phys. Chem. Chem. Phys. (2017) DOI: /c6cp06375f 10
11 Uracil vs K 0 (100 ev) Hyper NCO Intensity (a.u.) C 4 H 3 N 2 O 2 C 2 H - - C 4 H 2 N 2 O 2 O - H Mass (a.m.u) Almeida, Antunes, Martins, Eden, Silva, Nunes, Garcia and PLV Phys. Chem. Chem. Phys. 13 (2011) Ptasinska et al. J. Chem. Phys. 123 (2005)
12 Site- and bond-selectivity 1-methyl thymine 3-methyl uracil 9-methyl adenine 6-dimethyladenine 12
13 Autodetachment suppression & Coulombic complex stabilization 13
14 Almeida, Kinzel, Silva, Puschnigg, Gschliesser, Scheier, Denifl, Garcia, Gonzalez and PLV, Phys. Chem. Chem. Phys. 15 (2013)
15 Ferreia da Silva, Matias, Almeida, García, Ingólfsson, Flosadóttir, Ómarsson, Ptasinska, Puschnigg, Scheier, PLV, Denifl J. Am. Soc. Mass. Spectrom. 24 (2013)
16 K + CH 3 NO 2 and K + CD 3 NO 2 uncertainty 20% Antunes, Almeida, Martins, Mason, García, Maneira, Nunes and PLV. Phys. Chem. Chem. Phys. 12 (2010)
17 Conclusions site and bond selective mechanism in purines; the electron donor can greatly affect the chemical pathways of the reaction (e.g. CH 3 NO 2 ); compared to an isolated TNI formed by free electron capture, the anion in the vicinity of a K + favours dissociation rather than autodetachment; K + may delay autodetachment, allowing for intramolecular electron transfer Branching ratios (uncertainties up to 20%) and the collision dynamics; Provide K + energy loss profiles. 17
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