A Study of Heavy-Rydberg Ion-Pair Formation through Rydberg-Atom-Molecule Collisions

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dc.contributor.advisorDunning, F. Barryen_US
dc.creatorBuathong, Sittien_US
dc.date.accessioned2019-05-17T16:21:22Zen_US
dc.date.available2019-05-17T16:21:22Zen_US
dc.date.created2018-12en_US
dc.date.issued2018-08-30en_US
dc.date.submittedDecember 2018en_US
dc.date.updated2019-05-17T16:21:22Zen_US
dc.description.abstractThermal collisions between potassium Rydberg atoms with intermediate values of quantum number n and target molecules that capture free low-energy electrons are investigated. The velocity, binding energy, and angular distributions of heavy-Rydberg ion-pair states formed through such collisions are measured. The experimental data are analyzed with the aid of semiclassical Monte Carlo simulations to investigate the dynamics of electron attachment to a variety of target species. Multiple reaction channels involving short- and long-lived intermediates are seen for electron capture by 1,1,1-C2Cl3F3 and CBrCl3 (where dissociation of CBrCl3 intermediates involves production of Br- and Cl- ions). Electron attachment to BrCN produces long-lived BrCN-* intermediates whose dissociation results in the creation of rotationally-hot CN- anions. Electron capture by Fe(CO)5 leads to formation of Fe(CO)5-* intermediates which can fragment producing Fe(CO)4- anions, either directly or after partial redistribution of the excess energy within the intermediate has occurred. Electron transfer in Rydberg atom collisions with C2Cl4 provide no evidence of formation of long-lived C2Cl4 ions, only Cl- ions are seen. Moreover, strong Rydberg atom scattering is observed following collisions of K(12p) Rydberg states with CH3NO2. This finding is consistent with a theory which predicts that collisions between Rydberg atoms with intermediate values of n and polar molecules can lead to strong resonant quenching of Rydberg states, i.e., n and l changing, through formation of short-lived K+...CH3NO2- ion-pair states. Finally, the improvements in sensitivity to electron capture reaction dynamics that might be achieved using different Rydberg species and a crossed molecular beam are examined. Simulations are performed to demonstrate that the use of a hyperthermal helium Rydberg atomic beam and a crossed beam of target molecules such as CCl4, BrCN and CF3I can provide new insights into dissociative electron attachment reactions. The calculations show that not only can much detailed information on translational energy release distributions and intermediate lifetimes be obtained, but also on the electron radial probability density distributions in the Rydberg atoms themselves.en_US
dc.format.mimetypeapplication/pdfen_US
dc.identifier.citationBuathong, Sitti. "A Study of Heavy-Rydberg Ion-Pair Formation through Rydberg-Atom-Molecule Collisions." (2018) Diss., Rice University. <a href="https://hdl.handle.net/1911/105862">https://hdl.handle.net/1911/105862</a>.en_US
dc.identifier.urihttps://hdl.handle.net/1911/105862en_US
dc.language.isoengen_US
dc.rightsCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.en_US
dc.subjectHeavy-Rydberg ion-pair statesen_US
dc.subjectRydberg statesen_US
dc.subjectElectron attachmenten_US
dc.subjectHyperthermal Rydberg atomsen_US
dc.titleA Study of Heavy-Rydberg Ion-Pair Formation through Rydberg-Atom-Molecule Collisionsen_US
dc.typeThesisen_US
dc.type.materialTexten_US
thesis.degree.departmentPhysics and Astronomyen_US
thesis.degree.disciplineNatural Sciencesen_US
thesis.degree.grantorRice Universityen_US
thesis.degree.levelDoctoralen_US
thesis.degree.nameDoctor of Philosophyen_US
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