A localized view on molecular dissociation via electron-ion partial covariance
| Autor: | Allum, F, Music, V, Inhester, L, Boll, R, Erk, B, Schmidt, P, Baumann, TM, Brenner, G, Burt, M, Demekhin, PV, Dörner, S, Ehresmann, A, Galler, A, Grychtol, P, Heathcote, D, Kargin, D, Larsson, M, Lee, JWL, Li, Z, Manschwetus, B, Marder, L, Mason, R, Meyer, M, Otto, H, Passow, C, Pietschnig, R, Ramm, D, Schubert, K, Schwob, L, Thomas, RD, Vallance, C, Vidanović, I, von Korff Schmising, C, Wagner, R, Walter, P, Zhaunerchyk, V, Rolles, D, Bari, S, Brouard, M, Ilchen, M |
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| Jazyk: | angličtina |
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | Communications chemistry 5(1), 42 (2022). doi:10.1038/s42004-022-00656-w |
| DOI: | 10.1038/s42004-022-00656-w |
| Popis: | Communications chemistry 5(1), 42 (2022). doi:10.1038/s42004-022-00656-w 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. Published by Macmillan Publishers Limited, part of Springer Nature, [London] |
| Databáze: | OpenAIRE |
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