Crossed-beam universal-detection reactive scattering of radical beams characterized by laser-induced-fluorescence: the case of C-2 and CN

Year: 2010

Authors: Leonori F., Hickson K.M., Le Picard S.D., Wang X., Petrucci R., Foggi P., Balucani N., Casavecchia P.

Autors Affiliation: Univ Perugia, Dipartimento Chimica, I-06123 Perugia, Italy; Univ Bordeaux, CNRS, UMR 5255, Inst Mol Sci, F-33405 Talence, France; Univ Rennes 1, CNRS, UMR 6251, Inst Phys Rennes, F-35042 Rennes, France; Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China

Abstract: Continuous supersonic beams of dicarbon (C-2) and cyano (CN) radicals have been generated by a high-pressure radio-frequency discharge beam source starting from dilute mixtures in rare gases of suitable precursor molecules. Their internal quantum state distributions have been characterized by laser-induced-fluorescence (LIF) in a new crossed molecular beam-laser apparatus. These supersonic beams have been used to study the reactive scattering of C-2 and CN radicals with unsaturated hydrocarbons. This paper reports here on the C-2 and CN radical beam characterization by LIF and on dynamics studies of the reactions CN+C2H2 (acetylene) and CN+CH3CCH (methylacetylene) by the crossed molecular beam scattering technique with universal mass spectrometric detection and time-of-flight analysis. The role of CN rovibrational excitation on the dynamics of the CN+C2H2 reaction is discussed with reference to previous dynamics and kinetics studies. These reactions are of interest in the chemistry of planetary atmospheres (Titan) and the interstellar medium as well as in combustion.

Journal/Review: MOLECULAR PHYSICS

Volume: 108 (7-9)      Pages from: 1097  to: 1113

More Information: It is our greatest pleasure to dedicate this article to Professor Richard N. Zare on his seventieth birthday. His contributions to Molecular Reaction and Photon-Induced Dynamics via pioneering and state-of-the-art experiments have been a source of inspiration for many researchers in the field. We acknowledge financial support from the Italian MIUR (Ministero Istruzione Universita Ricerca) under projects PRIN (2007-H9S8SW). This work has also been supported in the initial stages by the European Union Marie-Curie human resources and mobility programme, including post-doctoral fellowships for K. M. Hickson and X. Wang, under contract MCRTN-CT-2004-512302, Molecular Universe, and through the Coordination Action 001637 (Europlanet). R. Petrucci thanks FSE (Fondo Sociale Europeo)-Regione Umbria – Ministero del Lavoro e delle Politiche Sociali for a fellowship. We thank P. Sharkey, A. Paladini, R. Cireasa, M. Pasquini and R. Piani for their contribution in setting up the LIF system and E. B. Jochnowitz for help in the spectra simulations of C2. SDLP also acknowledges support from the French Agence Nationale de Recherche, Programme Blanc \’Cold reactions of neutral species, CRNS\’. Finally, PC and SDLP acknowledge the Galileo Programme 2008/2009 between Perugia and Rennes. The Perugia, Rennes and Bordeaux authors acknowledge the COST Action CM0805 \’The Chemical Cosmos-Understanding chemistry in astronomical environments\’.
KeyWords: Dynamics; Fluorescence; Hydrocarbons; Laser optics; Laser produced plasmas; Light scattering; Mass spectrometry; Quantum theory; Reaction kinetics; Supersonic aircraft, CN radicals; Crossed molecular beams; Laser induced fluorescence; Radical beams; Reaction dynamics; Unsaturated hydrocarbons, Molecular beams
DOI: 10.1080/00268971003657110

Citations: 39
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