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Attosecond Probing of Electron Dynamics in Atoms and Molecules Using Tunable Mid-Infrared Drivers

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Attosecond Probing of Electron Dynamics in Atoms and Molecules Using Tunable Mid-Infrared Drivers Attosecond Probing of Electron Dynamics in Atoms and Molecules using Tunable Mid-Infrared Drivers DISSERTATION Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Timothy Thomas Gorman, B.S., M.S. Graduate Program in Physics The Ohio State University 2018 Dissertation Committee: Professor Louis F. DiMauro, Advisor Professor Jay A. Gupta Professor Daniel J. Gauthier Professor Douglass Schumacher © Copyright by Timothy Thomas Gorman 2018 Abstract The spectral intensity and phase of the complex photoionization and photorecombi- nation dipole matrix elements of gas phase atoms and molecules were studied with sub- femtosecond time resolution and sub-eV energy resolution using attosecond spectroscopy and high-harmonic spectroscopy. Using attosecond spectroscopy, the phases of two-photon transitions near autoionizing resonances were studied in Ar and He with harmonic combs of odd harmonics only as well as combs of even and odd harmonics. The Ar 3s3p64p and the He 2s2p resonances were explored using the Reconstruction of Attosecond Beat- ing by Interference of Two-Photon Transitions (RABBITT) method and by probing omega oscillations that occur with pulse trains comprised of even and odd harmonics. The RAB- BITT measurements revealed that the 3s3p64p resonance produced phase excursions of ¤ 0.2 rad and that the 2s2p resonance exhibited phase excursions of ¤ 0.5 rad. These results are in excellent agreement with ab initio calculations solving the time-dependent Schrödinger equation. The RABBITT measurements also revealed a small phase structure (¤0.05 rad) in Ar, which is attributed to the tentatively-labeled 3s23p44s4p resonance. The complexity of this resonance is beyond current modeling capabilities. Comparatively, the omega-oscillation experiments revealed resonant phase excursions for the Ar 3s3p64p and He 2s2p resonances that starkly deviate from theoretical predictions using the same the- oretical framework. These measurements emphasize that two-photon ionization involving electron correlations is incomplete and in need of further investigation. Using high-harmonic spectroscopy, the first measurements fully characterizing the spec- tral intensity and phase of the methyl chloride molecular Cooper minimum (CM) were performed. These experiments revealed that the CM of methyl chloride is located at ¤ 43 eV and is accompanied by a ¤ 120 as group delay minimum. The key to accurately identifying this resonance was the development of an in-house algorithm that was able to accurately calculate attochirp contributions present in the measurements. Also using high- harmonic spectroscopy, the spectral intensity and phase of two-center interferences in CO2, i OCS, and N2O were studied in the molecular frame. These measurements determined that the phase jump associated with CO2 two-center interference is negative in sign, settling an existing discrepancy in the literature. This result is also in agreement with theory calcula- tions performed using a time-dependent density functional theory framework. Additionally, the complex interplay of the OCS Cooper-like minimum (¤ 43 eV, ¤ 140as) and the molec- ular structure of OCS in the recombination dipole matrix element of the highest occupied molecular orbital was explored and characterized. The careful understanding of such com- plex interferences is expected to serve as the foundation for future measurements studying attosecond electron correlations in molecules. ii I would like to dedicate this dissertation to my wife, Dr. Emily Gorman, and my mother and father, Denise and Thomas Gorman, for always believing in me. iii Acknowledgments First and foremost, I would like to thank my two advisors, Professors Louis DiMauro and Pierre Agostini. They have provided me with a world-class research laboratory, a friendly and productive working environment, and priceless guidance throughout my entire graduate student career. I would also like to thank my undergraduate research advisors, Dr. Perry Yaney and the late Dr. Peter Powers, for first introducing me to lasers and all of their excitement at the University of Dayton. In no particular order, I would also like to thank the many other people who have positively impacted my research career: • Drs. Chantal Sudbrack and Timothy Gabb at the NASA Glenn Research Center for expanding my research knowledge into metals processing. • Drs. Stephen Schoun and Antoine Camper for first introducing me to attosecond science and molecular alignment. • Drs. Cosmin Blaga and Yu Hang “Marco” Lai for working with me to better under- stand strong field ionization, laser pulse characterization, and laser operation. • Drs. Hyunwook Park and Zhou Wang for teaching me about laser-cluster interac- tions, and particularly Dr. Wang for excellent debates concerning challenging physics questions. • Dietrich Kiesewetter for great acquisition and analysis software, which he developed for the group, for participating in physics discussions that helped expand my under- standing of relevant physics topics, and for many hours spent together learning how to build complex interferometers. • Dr. Timothy Scarborough, with whom all of the work in this dissertation was done in collaboration. Tim has an excellent work ethic, is a critical thinker, and is an all iv around good person to work with. I could not have asked for a better colleague with whom to perform my dissertation research. • Greg Smith and Stephen Hageman for many long, detailed physics discussions. I gained much of my physics knowledge through conversations with them. • Andrew Piper and Daniel Tuthill for productive discussions concerning autoionizing resonances. • Our research collaborators at Louisiana State University, including Dr. Ken Schafer, Dr. Mette Gaarde, Dr. François Mauger, and Dr. Paul Abanador for many in-depth discussions of high-harmonic spectroscopy. • Our research collaborators at the University of Virginia including Dr. Robert Jones, Dr. Péter Sándor, and Sanjay Khatri for teaching me about molecular strong-field ionization and surface harmonic generation. • Our research collaborators at the University of Central Florida, University of Auburn, and the Vienna University of Technology including Dr. Luca Argenti, Dr. Joachim Burgdörfer, Stefan Donsa, Saad Mehmood, Dr. Nicolas Douguet, Cariker Coleman, Dr. Guillaume Laurent, and John Vaughan for excellent discussions on autoionizing resonances. • Our research collaborators at CEA Saclay including Dr. Thierry Ruchon, Dr. Pascal Salieres, Dr. Romain Géneaux, Dr. Lou Barreau, and Celine Chappuis for originally teaching me about autoionizing resonances and orbital angular momentum of light. • All of the following people for useful and productive conversations: Kent Talbert, Eric Moore, Bryan Smith, Dr. Kaikai Zhang, Dr. Junliang Xu, Dr. Sha “Lisa” Li, Dr. Abraham Camacho, Dr. Douglass Schumacher, and Dr. Enam Chowdhury. • All of the following for being such great friends as I made my way through graduate school: Luke Gorman, Andrew Gorman, Julie Buchanan, Elizabeth Lannan, Solani v Harawa, Dr. Janet Harawa, Mike DeBrosse, Kevan Kramb, Dr. Christopher Jaymes, Dr. Steven Tjung, Thuc Mai, Dr. Matt Sheffield, Dr. Alex Dyhdalo, Michael Chilcote, and David Maguire. Lastly, I would like to thank all of the people I mentioned for always being willing to discuss my numerous questions, physics or otherwise. vi Vita 2012 . B.S. Physics. University of Dayton, Dayton, OH. 2014 . M.S. Physics. The Ohio State University, Columbus, OH. 2014 to present . Graduate Research Associate. The Ohio State University, Columbus, OH. Publications Zhang, K., Lai, Y. H., Diesen, E., Schmidt, B. E., Blaga, C. I., Xu, J., Gorman, T. T., Légaré, F., Saalmann, U., Agostini, P., Rost, J. M., and DiMauro, L. F. (2016). Universal pulse dependence of the low-energy structure in strong-field ionization. Physical Review A, 93(2):021403. Géneaux, R., Chappuis, C., Auguste, T., Beaulieu, S., Gorman, T. T., Lepetit, F., Di- Mauro, L. F., and Ruchon, T. (2017). Radial index of Laguerre-Gaussian modes in high- order-harmonic generation. Physical Review A, 95(5):051801. Scarborough, T. D., Gorman, T. T., Mauger, F., Sándor, P., Khatri, S., Gaarde, M. B., Schafer, K. J., Agostini, P., DiMauro, L. F. (2018). Full Characterization of a Molecular Cooper Minimum Using High-Harmonic Spectroscopy. Applied Sciences, 8(7):1129. Sándor, P., Sissay, A., Mauger, F., Abanador, P. M., Gorman, T. T., Scarborough, T. D., Gaarde, M. B., Lopata, K., Schafer K. J., Jones, R. R. (2018). Angle dependence of strong- field single and double ionization of carbonyl sulfide. Physical Review A 98(4):043425. vii Fields of Study Major Field: Physics viii Table of Contents Page Abstract........................................................................................................................ i Dedication .................................................................................................................... iii Acknowledgements ..................................................................................................... iv Vita................................................................................................................................ vii Table of Contents ....................................................................................................... xii List of Figures .............................................................................................................xxxii List of Tables ...............................................................................................................xxxiii
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