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005     20250715175556.0
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100 1 _ |a Allum, Felix
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245 _ _ |a A localized view on molecular dissociation via electron-ion partial covariance
260 _ _ |a [London]
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|b Macmillan Publishers Limited, part of Springer Nature
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520 _ _ |a 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 chiral (R/S)-1-iodo-2-methylbutane, probed by XUV pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we introduce 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$_{3/2}$ and 4d$_{5/2}$ 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. We thus pave the way for approaching femto-stereochemistry with FELs.
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700 1 _ |a Music, Valerija
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773 _ _ |a 10.1038/s42004-022-00656-w
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