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Attosecond High-Harmonic Spectroscopy of Atoms and Molecules Using Mid-Infrared Sources

Schoun, Stephen Bradley
http://orcid.org/0000-0002-7977-0379
http://rave.ohiolink.edu/etdc/view?acc_num=osu1436853089

Abstract Details

2015, Doctor of Philosophy, Ohio State University, Physics.
The amplitude and phase of the complex photoionization/photorecombination dipole matrix element of atoms and simple linear molecules is measured with sub-femtosecond time resolution and sub-electronvolt spectral resolution using High Harmonic Spectroscopy (HHS). The first known measurement of the dipole phase jump at a Cooper minimum is reported for the 3p orbital of argon. Also, the angle-dependent dipole of nitrogen is measured using rotationally-aligned molecular ensembles. In contrast with previous studies, which were limited by traditional shorter-wavelength near-infrared laser sources, only a single orbital is sufficient to explain the nitrogen results, which are in excellent agreement with accurate theoretical scattering-wave dipole calculations. All of these experiments benefit from the extended extreme-ultraviolet cutoff, and improved spectral resolution, afforded by the use of long-wavelength mid-infrared driving laser sources. This work extends our understanding of the interaction of light and matter on the timescale of the electron's motion, the attosecond (1 as = 10-18 s). The experimental results presented here lend credence to the methodology of molecular self-imaging by laser-induced ionization and recombination of a molecule's own electron. The successes and limitations of HHS as a tool for ultrafast atomic and molecular imaging are discussed. Finally, the feasibility is examined of using HHS to measure the temporal evolution of complicated chemical dynamics with attosecond precision.
Louis DiMauro, Professor (Advisor)
Frank De Lucia, Professor (Committee Member)
Jay Gupta, Professor (Committee Member)
Douglass Schumacher, Professor (Committee Member)
255 p.
Physics
attosecond; RABBITT; high-order harmonic generation; high harmonic generation, HHG; high harmonic spectroscopy; HHS; XUV; photoionization

Recommended Citations

Citations

  • Schoun, S. B. (2015). Attosecond High-Harmonic Spectroscopy of Atoms and Molecules Using Mid-Infrared Sources [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1436853089

    APA Style (7th edition)

  • Schoun, Stephen. Attosecond High-Harmonic Spectroscopy of Atoms and Molecules Using Mid-Infrared Sources. 2015. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1436853089.

    MLA Style (8th edition)

  • Schoun, Stephen. "Attosecond High-Harmonic Spectroscopy of Atoms and Molecules Using Mid-Infrared Sources." Doctoral dissertation, Ohio State University, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=osu1436853089

    Chicago Manual of Style (17th edition)

osu1436853089
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© 2015, all rights reserved.
This open access ETD is published by The Ohio State University and OhioLINK.