Univ. of Oxford (United Kingdom); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Universität Kassel (Germany); European XFEL, Schenefeld (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
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 4d3/2 and 4d5/2 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.
Allum, Felix, et al. "A localized view on molecular dissociation via electron-ion partial covariance." Communications Chemistry, vol. 5, no. 1, Mar. 2022. https://doi.org/10.1038/s42004-022-00656-w
@article{osti_1866598,
author = {Allum, Felix and Music, Valerija and Inhester, Ludger and Boll, Rebecca and Erk, Benjamin and Schmidt, Philipp and Baumann, Thomas M. and Brenner, Günter and Burt, Michael and Demekhin, Philipp V. and others},
title = {A localized view on molecular dissociation via electron-ion partial covariance},
annote = {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 4d3/2 and 4d5/2 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.},
doi = {10.1038/s42004-022-00656-w},
url = {https://www.osti.gov/biblio/1866598},
journal = {Communications Chemistry},
issn = {ISSN 2399-3669},
number = {1},
volume = {5},
place = {United States},
publisher = {Springer Nature},
year = {2022},
month = {03}}
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); EPSRC Programme Grants; Deutsche Forschungsgemeinschaft (DFG); Max Planck Society; Volkswagon Foundation; Helmholtz Initiative; National Science Foundation (NSF)
Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 633https://doi.org/10.1016/j.nima.2010.06.178