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    Ultrafast Measurement and Control of Excited-State Dynamics Using Nonlinear Spectroscopy in the Extreme-Ultraviolet Regime

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    Author
    Yanez-Pagans, Sergio
    Issue Date
    2022
    Keywords
    Attosecond
    Extreme-ultraviolet
    Femtosecond
    Polaritons
    Spectroscopy
    Strong-field
    Advisor
    Sandhu, Arvinder
    
    Metadata
    Show full item record
    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, presentation (such as public display or performance) of protected items is prohibited except with permission of the author.
    Abstract
    The advent of ultrafast nonlinear spectroscopy with weak extreme-ultraviolet (XUV) and strong-field near-infrared (NIR) pulses has enabled investigations of electronic processes in atomic and molecular systems with femtosecond and attosecond resolution. Conventional XUV-NIR attosecond transient absorption (ATA) and multi-wave mixing (MWM) spectroscopies have successfully probed coherent electron dynamics in a wide range of quantum systems. However, these optical setups are often limited by the commensurate nature of the harmonic XUV pump and the driving NIR probe. In this work, we enhance the versatility of these techniques by using optical parametric amplification to generate tunable infrared (IR) pulses. This approach allows us to adjust the frequencies of the XUV and IR pulses independently of each other. To demonstrate the power of tunable ATA and MWM schemes, we apply these techniques to study and manipulate laser-induced couplings and autoionizing resonances embedded in the continuum of polyelectronic systems. We begin by investigating the degeneracy between autoionizing bright and light-induced states (LIS) in argon, which leads to the formation of entangled light-matter states known as polaritons. By tuning the IR pulse parameters we demonstrate control over polaritonic evolution and their decay pathways. In the next study, we use the incommensurate IR pulse to drive resonant background-free wave-mixing processes to probe quantum beats that arise from coherent electronic superpositions of singly- and doubly-excited states in krypton. Finally, we discuss the extension of these techniques to molecular systems and macroscopic propagation regimes. Our results further the understanding of autoionization (AI) dynamics in multielectron systems and demonstrate novel methods for the optical measurement and control of excited-state dynamics in the continuum.
    Type
    text
    Electronic Dissertation
    Degree Name
    Ph.D.
    Degree Level
    doctoral
    Degree Program
    Graduate College
    Physics
    Degree Grantor
    University of Arizona
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