Imaging the Renner–Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump–probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS₂) in the B̃ ¹ B₂ ex...

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Published inProceedings of the National Academy of Sciences - PNAS Vol. 116; no. 17; pp. 8173 - 8177
Main Authors Amini, Kasra, Sclafani, Michele, Steinle, Tobias, Le, Anh-Thu, Sanchez, Aurelien, Müller, Carolin, Steinmetzer, Johannes, Yue, Lun, Saavedra, José Ramón Martínez, Hemmer, Michaël, Lewenstein, Maciej, Moshammer, Robert, Pfeifer, Thomas, Pullen, Michael G., Ullrich, Joachim, Wolter, Benjamin, Moszynski, Robert, de Abajo, F. Javier García, Lin, C. D., Gräfe, Stefanie, Biegert, Jens
Format Journal Article
LanguageEnglish
Published United States National Academy of Sciences 23.04.2019
Subjects
attosecond wave packet
Carbonyls
Electron diffraction
Electron states
laser-induced electron diffraction
nonadiabatic dynamics
Physical Sciences
PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
Rotational spectra
Science & Technology
Spectroscopy
Stretching
structural dynamics
attosecond wave packet
laser-induced electron diffraction
nonadiabatic dynamics
structural dynamics
electron diffraction
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Summary:Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump–probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS₂) in the B̃ ¹ B₂ excited electronic state using laser-induced electron diffraction (LIED).We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS₂ molecule with combined picometer and attosecond resolution using intrapulse pump–probe excitation and measurement. We invoke the Renner–Teller effect to populate the B̃ ¹ B₂ excited state in neutral CS₂, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS₂, which is known to appear as a two-center scatterer.
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FG02-86ER13491
USDOE Office of Science (SC)
2Present address: Department of Physics, Missouri University of Science and Technology, Rolla, MO 65409.
Author contributions: J.B. designed research; K.A., M.S., T.S., A.-T.L., A.S., C.M., J.S., L.Y., J.R.M.S., M.H., M.L., R. Moshammer, M.G.P., J.U., B.W., and J.B. performed research; A.-T.L., C.M., J.S., L.Y., J.R.M.S., R. Moszynski, F.J.G.d.A., C.D.L., and S.G. contributed new reagents/analytic tools; K.A., M.S., T.S., A.S., and M.G.P. analyzed data; and K.A., M.S., T.S., A.-T.L., M.L., R. Moshammer, T.P., J.U., R. Moszynski, F.J.G.d.A., C.D.L., S.G., and J.B. wrote the paper.
1K.A., M.S., and T.S. contributed equally to this work.
Edited by Shaul Mukamel, University of California, Irvine, CA, and approved March 8, 2019 (received for review October 10, 2018)
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1817465116