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.
Tuthill, Daniel R., et al. "Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies." Journal of Molecular Spectroscopy, vol. 372, no. C, Aug. 2020. https://doi.org/10.1016/j.jms.2020.111353
Tuthill, Daniel R., Mauger, François, Scarborough, Timothy D., Jones, Robert R., Gaarde, Mette B., Lopata, Kenneth, Schafer, Kenneth J., & DiMauro, Louis F. (2020). Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies. Journal of Molecular Spectroscopy, 372(C). https://doi.org/10.1016/j.jms.2020.111353
Tuthill, Daniel R., Mauger, François, Scarborough, Timothy D., et al., "Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies," Journal of Molecular Spectroscopy 372, no. C (2020), https://doi.org/10.1016/j.jms.2020.111353
@article{osti_1802355,
author = {Tuthill, Daniel R. and Mauger, François and Scarborough, Timothy D. and Jones, Robert R. and Gaarde, Mette B. and Lopata, Kenneth and Schafer, Kenneth J. and DiMauro, Louis F.},
title = {Multidimensional molecular high-harmonic spectroscopy: A road map for charge migration studies},
annote = {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.},
doi = {10.1016/j.jms.2020.111353},
url = {https://www.osti.gov/biblio/1802355},
journal = {Journal of Molecular Spectroscopy},
issn = {ISSN 0022-2852},
number = {C},
volume = {372},
place = {United States},
publisher = {Elsevier},
year = {2020},
month = {08}}
Ditchburn, Robert William; Tunstead, J.; Yates, J. G.
Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 181, Issue 987, p. 386-399https://doi.org/10.1098/rspa.1943.0016
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145https://doi.org/10.1098/rsta.2017.0481