Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)5, Fe(CO)4, and Fe(CO)3
Abstract
The prototypical photoinduced dissociation of Fe(CO)5 in the gas phase is used to test time-resolved x-ray photoelectron spectroscopy for studying photochemical reactions. Upon one-photon excitation at 266 nm, Fe(CO)5 successively dissociates to Fe(CO)4 and Fe(CO)3 along a pathway where both fragments retain the singlet multiplicity of Fe(CO)5. The x-ray free-electron laser FLASH is used to probe the reaction intermediates Fe(CO)4 and Fe(CO)3 with time-resolved valence and core-level photoelectron spectroscopy, and experimental results are interpreted with ab initio quantum chemical calculations. Changes in the valence photoelectron spectra are shown to reflect changes in the valence-orbital interactions upon Fe–CO dissociation, thereby validating fundamental theoretical concepts in Fe–CO bonding. Chemical shifts of CO 3σ inner-valence and Fe 3p core-level binding energies are shown to correlate with changes in the coordination number of the Fe center. We interpret this with coordination-dependent charge localization and core-hole screening based on calculated changes in electron densities upon core-hole creation in the final ionic states. This extends the established capabilities of steady-state electron spectroscopy for chemical analysis to time-resolved investigations. Lastly, it could also serve as a benchmark for how charge and spin density changes in molecular dissociation and excited-state dynamics are expressed in valence and core-level photoelectronmore »
- Authors:
-
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany)
- Stockholm Univ., Stockholm (Sweden)
- European XFEL GmbH, Schenefeld (Germany)
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany)
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany); Stockholm Univ., Stockholm (Sweden)
- Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
- European XFEL GmbH, Schenefeld (Germany)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1468956
- Grant/Contract Number:
- AC02-76SF00515; EXC1074; 05K10PK2
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 149; Journal Issue: 4; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Leitner, T., Josefsson, I., Mazza, T., Miedema, P. S., Schröder, H., Beye, M., Kunnus, K., Schreck, S., Düsterer, S., Föhlisch, A., Meyer, M., Odelius, M., and Wernet, Ph. Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)5, Fe(CO)4, and Fe(CO)3. United States: N. p., 2018.
Web. doi:10.1063/1.5035149.
Leitner, T., Josefsson, I., Mazza, T., Miedema, P. S., Schröder, H., Beye, M., Kunnus, K., Schreck, S., Düsterer, S., Föhlisch, A., Meyer, M., Odelius, M., & Wernet, Ph. Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)5, Fe(CO)4, and Fe(CO)3. United States. doi:https://doi.org/10.1063/1.5035149
Leitner, T., Josefsson, I., Mazza, T., Miedema, P. S., Schröder, H., Beye, M., Kunnus, K., Schreck, S., Düsterer, S., Föhlisch, A., Meyer, M., Odelius, M., and Wernet, Ph. Fri .
"Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)5, Fe(CO)4, and Fe(CO)3". United States. doi:https://doi.org/10.1063/1.5035149. https://www.osti.gov/servlets/purl/1468956.
@article{osti_1468956,
title = {Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)5, Fe(CO)4, and Fe(CO)3},
author = {Leitner, T. and Josefsson, I. and Mazza, T. and Miedema, P. S. and Schröder, H. and Beye, M. and Kunnus, K. and Schreck, S. and Düsterer, S. and Föhlisch, A. and Meyer, M. and Odelius, M. and Wernet, Ph.},
abstractNote = {The prototypical photoinduced dissociation of Fe(CO)5 in the gas phase is used to test time-resolved x-ray photoelectron spectroscopy for studying photochemical reactions. Upon one-photon excitation at 266 nm, Fe(CO)5 successively dissociates to Fe(CO)4 and Fe(CO)3 along a pathway where both fragments retain the singlet multiplicity of Fe(CO)5. The x-ray free-electron laser FLASH is used to probe the reaction intermediates Fe(CO)4 and Fe(CO)3 with time-resolved valence and core-level photoelectron spectroscopy, and experimental results are interpreted with ab initio quantum chemical calculations. Changes in the valence photoelectron spectra are shown to reflect changes in the valence-orbital interactions upon Fe–CO dissociation, thereby validating fundamental theoretical concepts in Fe–CO bonding. Chemical shifts of CO 3σ inner-valence and Fe 3p core-level binding energies are shown to correlate with changes in the coordination number of the Fe center. We interpret this with coordination-dependent charge localization and core-hole screening based on calculated changes in electron densities upon core-hole creation in the final ionic states. This extends the established capabilities of steady-state electron spectroscopy for chemical analysis to time-resolved investigations. Lastly, it could also serve as a benchmark for how charge and spin density changes in molecular dissociation and excited-state dynamics are expressed in valence and core-level photoelectron spectroscopy.},
doi = {10.1063/1.5035149},
journal = {Journal of Chemical Physics},
number = 4,
volume = 149,
place = {United States},
year = {2018},
month = {7}
}
Web of Science
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Time-resolved electron spectroscopy for chemical analysis of photodissociation: Photoelectron spectra of Fe(CO)$_5$ , Fe(CO)$_4$ , and Fe(CO)$_3$
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