Probing the interplay between geometric and electronic-structure features via high-harmonic spectroscopy

Gorman, T. T.; Scarborough, T. D.; Abanador, P. M.; Mauger, F.; Kiesewetter, D.; Sándor, P.; Khatri, S.; Lopata, K.; Schafer, K. J.; Agostini, P.; Gaarde, M. B.; DiMauro, L. F.

doi:10.1063/1.5086036

Title: Probing the interplay between geometric and electronic-structure features via high-harmonic spectroscopy

Journal Article · Tue May 14 00:00:00 EDT 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5086036· OSTI ID:1609522

Gorman, T. T. ^[1];

^[1];

^[2];

^[2]; Kiesewetter, D. ^[1];

^[3]; Khatri, S. ^[3];

^[2]; Schafer, K. J. ^[2]; Agostini, P. ^[1]; Gaarde, M. B. ^[2]; DiMauro, L. F. ^[1]

The Ohio State Univ., Columbus, OH (United States)
Louisiana State Univ., Baton Rouge, LA (United States)
Univ. of Virginia, Charlottesville, VA (United States)

We present molecular-frame measurements of the recombination dipole matrix element (RDME) in CO₂, N₂O, and carbonyl sulfide (OCS) molecules using high-harmonic spectroscopy. Both the amplitudes and phases of the RDMEs exhibit clear imprints of a two-center interference minimum, which moves in energy with the molecular alignment angle relative to the laser polarization. Here, we find that whereas the angle dependence of this minimum is consistent with the molecular geometry in CO₂ and N₂O, it behaves very differently in OCS; in particular, the phase shift which accompanies the two-center minimum changes sign for different alignment angles. Our results suggest that two interfering structural features contribute to the OCS RDME, namely, (i) the geometrical two-center minimum and (ii) a Cooper-like, electronic-structure minimum associated with the sulfur end of the molecule. We compare our results to ab initio calculations using time-dependent density functional theory and present an empirical model that captures both the two-center and the Cooper-like interferences. We also show that the yield from unaligned samples of two-center molecules is, in general, reduced at high photon energies compared to aligned samples, due to the destructive interference between molecules with different alignments.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States); Louisiana State Univ., Baton Rouge, LA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-04ER15614; SC0012462

OSTI ID:: 1609522

Alternate ID(s):: OSTI ID: 1512532

Journal Information:: Journal of Chemical Physics, Vol. 150, Issue 18; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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