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Proc Natl Acad Sci U S A. 2019 Apr 5. pii: 201817465. doi: 10.1073/pnas.1817465116. [Epub ahead of print]

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

Author information

1
ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels (Barcelona), Spain.
2
Department of Chemistry, University of Warsaw, 02-093 Warsaw, Poland.
3
Department of Physics, J. R. Macdonald Laboratory, Kansas State University, Manhattan, KS 66506-2604.
4
Institute of Physical Chemistry, Friedrich-Schiller University, 07743 Jena, Germany.
5
ICREA, 08010 Barcelona, Spain.
6
Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
7
Physikalisch-Technische Bundesanstalt, D-38116 Braunschweig, Germany.
8
Abbe Center of Photonics, Friedrich-Schiller University, 07745 Jena, Germany.
9
ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels (Barcelona), Spain; jens.biegert@icfo.eu.

Abstract

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 [Formula: see text] 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 [Formula: see text] 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.

KEYWORDS:

attosecond wave packet; electron diffraction; laser-induced electron diffraction; nonadiabatic dynamics; structural dynamics

PMID:
30952783
DOI:
10.1073/pnas.1817465116

Conflict of interest statement

The authors declare no conflict of interest.

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