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A localized view on molecular dissociation via electron-ion partial covariance
Felix Allum1,2, Valerija Music3,4,5, Ludger Inhester6
1The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford, OX1 3TA, UK. fallum@stanford.edu.
Communications Chemistry
|January 25, 2023
Summary
This study uses ultrafast X-ray pulses to track the chemical changes in a chiral molecule after ultraviolet photodissociation. The technique allows for site-specific investigations of molecular photochemistry.
Area of Science:
- * Molecular spectroscopy
- * Chemical physics
- * Ultrafast science
Background:
- * Inner-shell photoelectron spectroscopy offers element-specific insights into molecular structure.
- * Core-electron binding energies are sensitive to the molecular environment.
- * Femtosecond light sources enable time-resolved studies of molecular photochemistry.
Purpose of the Study:
- * To investigate the ultraviolet photodissociation of 1-iodo-2-methylbutane using time-resolved spectroscopy.
- * To probe the ultrafast evolution of iodine 4d binding energies.
- * To develop and apply advanced spectroscopic methods for site-specific photochemical investigations.
Main Methods:
- * Employed extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH).
- * Utilized electron-ion partial covariance imaging to analyze two-dimensional photoelectron spectra.
- * Combined experimental data with theoretical calculations for time-resolved electron spectra.
Main Results:
- * Successfully disentangled the 4d3/2 and 4d5/2 atomic and molecular levels in the time-resolved spectra.
- * Isolated spectral features arising from different photofragmentation pathways.
- * Demonstrated the capability to track ultrafast electronic changes at a specific atomic site.
Conclusions:
- * The developed method provides a key step towards site-specific investigations of molecular photochemistry.
- * This approach enables the study of structural and chemical changes from a specific spectator site.
- * Offers a powerful tool for understanding complex photochemical processes at the ultrafast timescale.
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