Abstract
The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Up to now, to directly image the onset of Jahn-Teller symmetry breaking remains unreached. Here we employ ultrafast ion-coincidence Coulomb explosion imaging with sub-10 fs resolution and unambiguously image the ultrafast dynamics of Jahn-Teller deformations of {{rm{CH}}}_{4}^{+} cation in symmetry space. It is unraveled that the Jahn-Teller deformation from C3v to C2v geometries takes a characteristic time of 20 ± 7 fs for this system. Classical and quantum molecular dynamics simulations agree well with the measurement, and reveal dynamics for the build-up of the C2v structure involving complex revival process of multiple vibrational pathways of the {{rm{CH}}}_{4}^{+} cation.
Highlights
The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields
Accessing the short-time structural dynamics caused by the JT effect, i.e., the onset of symmetry breaking from an initially symmetric configuration, remains a great challenge, and a direct experimental imaging of structural symmetry breaking in real time has not yet been realized, even in the ultrafast diffraction imaging experiment of excited CF3I molecule, the JT distortion has not been resolved from the measured data due to insufficient resolution[2]
One sees that the kinetic energy release (KER) spectra are dominated by time-independent features at KER ~5 eV caused by the interaction with only one of the laser pulses[22]
Summary
The Jahn-Teller effect is an essential mechanism of spontaneous symmetry breaking in molecular and solid state systems, and has far-reaching consequences in many fields. Accessing the short-time structural dynamics caused by the JT effect, i.e., the onset of symmetry breaking from an initially symmetric configuration, remains a great challenge, and a direct experimental imaging of structural symmetry breaking in real time has not yet been realized, even in the ultrafast diffraction imaging experiment of excited CF3I molecule, the JT distortion has not been resolved from the measured data due to insufficient resolution[2] Accessing these structural dynamics is key to understanding the early stages of photo-triggered chemical bond cleavage and molecular dynamics (MD) leading to energy and charge transfer processes[18]. As the CH populates the CH þ 4 in its which subsequently deforms þ 4 cation reaches
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