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

Amini, Kasra; Sclafani, Michele; Steinle, Tobias; Le, Anh-Thu; Sanchez, Aurelien; Müller, Carolin; Steinmetzer, Johannes; Yue, Lun et al. · Proc Natl Acad Sci U S A · 2019

basic_science · Level V

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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 (CS<sub>2</sub>) 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 CS<sub>2</sub> 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 CS<sub>2</sub>, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS<sub>2</sub>, which is known to appear as a two-center scatterer.