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Variable Temperature Rate Coefficient Studies through a Coaxial Molecular Beam Radiofrequency Ring Electrode Ion TrapYuan, Bing January 2012 (has links)
The dissertation focuses on the temperature dependent rate coefficient measurement of reactions in the interstellar medium using a coaxial molecular beam ring electrode ion trap apparatus. The first chapter introduces the previous studies of ion-molecule reactions in the ISM, the types of instruments mainly used in the reaction rate coefficient study, the former research on the ring electrode ion trap and the gas phase reaction mechanisms. Compare to other instruments, our molecular beam - ring electrode ion trap is extremely good at ion cooling and temperature control for both ions and neutral molecules. Chapter two describes each part of the instrument used in detail. Ions produced by electron impact in the ion source chamber, are mass filtered and then reach the ring electrode ion trap. In the trap, ions collide with molecules in the molecular beam where reaction takes place. When the reaction is done, all the ions remained in the trap (the reactant and product ions) come out and move to the detector. The molecular beam terminates at residual gas analyzer which is used for the number density calibration. The third chapter shows how the temperature of ions and molecules are controlled separately in order to find the reaction mechanism. Ions are cooled by the pulsed He buffer in the ring electrode trap and a chopped beam is used to make sure the ions are cooled to the desired low temperature when the reaction takes place. Chapters four to six describe the three reactions being studied using this instrument: N₂⁺ + H₂O charge transfer reaction, H₃O⁺ + C₂H₄ proton transfer reaction and H3O⁺ + (C₂H₂)₂/C₂H₂ dimer reaction. The temperature dependent rate coefficient data of these reactions are explained by the average dipole orientation theory, statistical theory and Colussi's acetylene dimer model, respectively. Two temperatures are defined and applied in the experimental rate coefficients analysis: ion-molecule center of mass collision temperature and the reaction statistical temperature which is based on the numbers of degrees of freedom of both reactants.
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