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Energy Transfer into Molecular Vibrations and Rotations by Recoil in Inner-Shell Photoemission.

E Kukk1, T D Thomas2, D Céolin3

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Physical Review Letters
|September 1, 2018
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Summary
This summary is machine-generated.

Photoelectron recoil effects in carbon tetrafluoride (CF4) and carbon monoxide (CO) reveal hidden vibrational modes and energy partitioning. Recoil energy in CO favors rotational over vibrational excitation, aligning with Coriolis coupling models.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • X-ray Spectroscopy

Background:

  • Photoelectron spectroscopy is a powerful tool for probing molecular electronic structure.
  • Recoil effects in photoionization can influence spectral features, particularly in the tender X-ray region.
  • Understanding energy partitioning in molecular photoionization is crucial for theoretical models.

Purpose of the Study:

  • To investigate photoelectron recoil effects in CF4 and CO gases using tender X-rays.
  • To reveal vibrational modes in CF4 that are obscured by Franck-Condon excitations.
  • To determine the energy distribution between rotational and vibrational excitation in CO due to recoil.

Main Methods:

  • High-resolution photoelectron spectroscopy using a mixture of CF4 and CO gases.
  • Utilizing CF4 as an energy calibrant for precise measurements in the tender X-ray region.
  • Analysis of spectral envelopes to identify recoil-induced excitations and energy partitioning.

Main Results:

  • In CF4, recoil-induced excitations fully dominate the C 1s photoelectron spectrum, exposing previously hidden vibrational modes.
  • In CO, the ratio of rotational to vibrational recoil energy was determined to be 2.88(28).
  • This observed ratio significantly exceeds the prediction of the basic recoil model (ratio of 2).

Conclusions:

  • Photoelectron recoil effects play a significant role in shaping molecular photoelectron spectra, especially in the tender X-ray regime.
  • The experimental findings for CO align well with theoretical predictions when Coriolis coupling is considered, suggesting its importance in energy transfer.
  • This study demonstrates the utility of recoil effects in uncovering subtle molecular dynamics and validating theoretical frameworks.