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.
Publication Source (Journal or Book title)
Journal of Molecular Spectroscopy
Tuthill, D., Mauger, F., Scarborough, T., Jones, R., Gaarde, M., Lopata, K., Schafer, K., & DiMauro, L. (2020). Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies. Journal of Molecular Spectroscopy, 372 https://doi.org/10.1016/j.jms.2020.111353