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

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${}_2$) in the B${}^1$B${}_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS${}_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B${}^1$B${}_2$ excited state in neutral CS${}_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS${}_2$, which is known to appear as a two-center scatterer.

References in corpus (6)

• Accurate retrieval of structural information from laser-induced photoelectron and high-harmonic spectra by few-cycle laser pulses
• Imaging an aligned polyatomic molecule with laser-induced electron diffraction
• Quantitative rescattering theory for laser-induced high-energy plateau photoelectron spectra
• Imaging of Alignment, Deformation and Dissociation of CS2 Molecules using Ultrafast Electron Diffraction
• Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
• Ab-Initio Surface Hopping and Multiphoton Ionisation Study of the Photodissociation Dynamics of CS${}_2$

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