Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies

• Published in: Journal of molecular spectroscopy Vol. 372; no. C
• Main Authors: Tuthill, Daniel R., Mauger, François, Scarborough, Timothy D., Jones, Robert R., Gaarde, Mette B., Lopata, Kenneth, Schafer, Kenneth J., DiMauro, Louis F.
• Format: Journal Article
• Language: English
• Published: United States Elsevier 11.08.2020
• Subjects: ATOMIC AND MOLECULAR PHYSICS; charge migration; copper minimum; HHG short trajectory selection; high-harmonic spectroscopy; physics; spectroscopy; two-center interference
• ISSN: 0022-2852; 1096-083X

This work 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.