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Photoelectron Imaging and Photofragmentation of Molecular and Cluster Anions

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Photoelectron Imaging and Photofragmentation of Molecular and Cluster Anions Photoelectron Imaging and Photofragmentation of Molecular and Cluster Anions Item Type text; Electronic Dissertation Authors Khuseynov, Dmitry Publisher The University of Arizona. Rights Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author. Download date 07/10/2021 05:03:05 Link to Item http://hdl.handle.net/10150/317044 PHOTOELECTRON IMAGING AND PHOTOFRAGMENTATION OF MOLECULAR AND CLUSTER ANIONS by Dmitry Khuseynov __________________________ A Dissertation Submitted to the Faculty of the DEPARTMENT OF CHEMISTRY AND BIOCHEMISTRY In Partial Fulfillment of the Requirements For the Degree of DOCTOR OF PHILOSOPHY WITH A MAJOR IN CHEMISTRY In the Graduate College THE UNIVERSITY OF ARIZONA 2 0 1 4 2 THE UNIVERSITY OF ARIZONA GRADUATE COLLEGE As members of the Dissertation Committee, we certify that we have read the dissertation prepared by Dmitry Khuseynov, entitled Photoelectron Imaging and Photofragmentation of Molecular and Cluster Anions and recommend that it be accepted as fulfilling the dissertation requirement for the Degree of Doctor of Philosophy. _______________________________________________________________________ Date: 16 April 2014 Andrei Sanov _______________________________________________________________________ Date: 16 April 2014 Oliver Monti _______________________________________________________________________ Date: 16 April 2014 Steven Schwartz _______________________________________________________________________ Date: 16 April 2014 Dennis Lichtenberger Final approval and acceptance of this dissertation is contingent upon the candidate’s submission of the final copies of the dissertation to the Graduate College. I hereby certify that I have read this dissertation prepared under my direction and recommend that it be accepted as fulfilling the dissertation requirement. ________________________________________________ Date: 16 April 2014 Dissertation Director: Andrei Sanov 3 STATEMENT BY AUTHOR This dissertation has been submitted in partial fulfillment of the requirements for an advanced degree at the University of Arizona and is deposited in the University Library to be made available to borrowers under rules of the Library. Brief quotations from this dissertation are allowable without special permission, provided that an accurate acknowledgement of the source is made. Requests for permission for extended quotation from or reproduction of this manuscript in whole or in part may be granted by the head of the major department or the Dean of the Graduate College when in his or her judgment the proposed use of the material is in the interests of scholarship. In all other instances, however, permission must be obtained from the author. SIGNED: ______________________________________ Dmitry Khuseynov 4 ACKNOWLEDGEMENTS I would like to thank Professor Andrei Sanov for being the best research advisor I have ever had the privilege to work for. His enthusiasm and appreciation of science were a constant inspiration for me to be a better scientist in all of the meanings of the word. I am infinitely thankful for his patience and support and for a great sense of humor about all of the pranks we played on him over the years. I am very grateful to Professor Daniel Goebbert for being a great mentor and a friend during my first couple of years in the group. His endless patience in teaching me lab techniques and the science behind photoelectron imaging has helped to shape me as a researcher and as a teacher. Thank you to my colleague Dr. Lori Culberson for being an awesome friend throughout the Ph.D. process, for encouraging me, and for all of the discussions we had about science and graduate life. Thanks to Andrew Dixon for working with me on many experiments over the years, for proofreading a bulk of my dissertation and for our scientific discussions. Thanks to him, Chris Blackstone and Adam Wallace for being such positive new presences in the lab. Thanks to Dr. Kostyantyn Pichugin and Dr. Emily Grumbling for welcoming me in the lab and for their mentorship in the beginning of my graduate career. Thanks to Matthew Fontana for his valuable help in the tetracyanoethylene experiment and to Daniel Dokuchitz for working with me on the fumaronitrile project. I couldn’t have hoped for more responsible and enthusiastic mentees. I am very appreciative of Mike Read and Kevin Bao of the electronic shop, and Ed Autz and Lee Macomber of the machine shop for their support and expertise. Without their help in fixing the equipment or designing new parts it would be impossible to improve or even maintain a working instrument. Infinite thanks to graduate program coordinator Lori Boyd for her patience and kindness and for going above and beyond in assisting all of the graduate students in the program. Thanks to my dissertation committee, Professors Andrei Sanov, Oliver Monti, Steven Schwartz, and Dennis Lichtenberger for their helpful feedback. I would like to also acknowledge the Science Foundation of Arizona, the Technology and Research Initiative Fund in Imaging, the Galileo Fellowship, the University of Arizona, and the National Science Foundation for supporting and funding various aspects of my graduate education. Thanks to all of my friends in the Chemistry and Biochemistry department and in the Tucson community. Thanks to my brother, Artem Khuseynov, for his cooperation (and support). Probasch! Finally, special thanks to Alex Petlick for her love and encouragement. 5 DEDICATION To my family for their support and love, for keeping me grounded and teaching me how to find humor in every situation 6 Table of Contents LIST OF FIGURES .......................................................................................................... 11 LIST OF TABLES ............................................................................................................ 21 ABSTRACT ...................................................................................................................... 24 CHAPTER 1 GENERAL INTRODUCTION .................................................................. 28 CHAPTER 2 EXPERIMENTAL METHODS ................................................................. 36 2.1. Overview ................................................................................................................ 36 2.2. Vacuum hardware .................................................................................................. 36 2.3. Ion production ........................................................................................................ 37 2.4. Linear time-of-flight mass spectrometer ................................................................ 39 2.5. Laser systems ......................................................................................................... 41 2.6. Reflectron time-of-flight mass spectrometer ......................................................... 43 2.7. Photoelectron imaging ........................................................................................... 44 CHAPTER 3 OXYGEN CLUSTER ANIONS REVISITED: SOLVENT-MEDIATED DISSOCIATION OF THE CORE O4 ANION WITHIN O2n (H2O)m CLUSTERS ....... 49 3.1. Introduction ........................................................................................................ 49 3.2. Experimental section .......................................................................................... 51 3.3. Results ................................................................................................................ 52 3.3.1. Photoelectron imaging spectroscopy .......................................................... 52 3.3.2. Photofragment mass-spectrometry.............................................................. 55 3.4. Discussion .............................................................................................................. 55 3.5. Conclusion ............................................................................................................. 64 CHAPTER 4 PHOTODISSOCIATION OF NITROMETHANE CLUSTER ANIONS . 70 4.1. Introduction ............................................................................................................ 70 4.2. Experimental and theoretical methods ................................................................... 73 4.3. Results .................................................................................................................... 74 4.4. Discussion. Dissociation mechanisms ................................................................... 76 4.4.1. Overview ......................................................................................................... 76 4.4.2. Electronic states .............................................................................................. 77 − − 4.4.3. CH3NO2 \ CH3 + NO2 .................................................................................. 79 − − 4.4.4. CH3NO2 \ OH + CH2NO .............................................................................. 80 7 4.5. Discussion. Solvation effects. ................................................................................ 81 4.6. Conclusion and future directions ........................................................................... 83 Table 4.1 Relevant reaction energetics. .........................................................................
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