A localized view on molecular dissociation via electron-ion partial covariance

書誌事項

公開日
2022-03-28
権利情報
  • https://creativecommons.org/licenses/by/4.0
  • https://creativecommons.org/licenses/by/4.0
DOI
  • 10.1038/s42004-022-00656-w
公開者
Springer Science and Business Media LLC

説明

<jats:title>Abstract</jats:title><jats:p>Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d<jats:sub>3/2</jats:sub> and 4d<jats:sub>5/2</jats:sub> atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.</jats:p>

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