Daniel R. Tuthill [1], François Mauger [2], Timothy D. Scarborough [1], Robert R. Jones [3], Mette B. Gaarde [2], Kenneth Lopata [4,5], Kenneth J. Schafer [2], Louis F. DiMauro[1]
[1] Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA
[2] Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA
[3] Department of Physics, University of Virginia, Charlottesville, Virginia 22904, USA
[4] Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA
[5] Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70808, US
Abstract:This review discusses recent experimental and theoretical analyses of high-harmonic spectroscopy in small molecules, with the aim of characterizing charge migration. We discuss the formulation of molecular high-harmonic spectra followed by methods to extract molecular-target-specific information, both in experiments and ab initio simulations. We present measured and simulated high-harmonic spectra from carbon dioxide and carbonyl sulfide to illustrate the necessity for multidimensional analyses for high-harmonic spectroscopies that include both the spectral amplitude and phase. Leveraging these results, we examine how such multidimensional analyses pave the way for the study of charge migration with high-harmonic spectroscopy and illustrate the beneficial role a static molecular feature can play when probing dynamics. Finally, we briefly expand our scope with an outlook on the critical role of integrating theoretical and experimental approaches, beyond just high-harmonic spectroscopy, for the development of versatile harmonic spectroscopic probes of charge migration.
Status: Published, J. Mol. Spec. 372, 111353 (2020).
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