Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH
Abstract
Here, we utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO)5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO)4 which are observed following a charge transfer photoexcitation of Fe(CO)5 as reported in our previous study. We find that branching of the reaction pathway likely happens in the 1A1 state of Fe(CO)4. A sub-picosecond time constant of the spin crossover from 1B2 to 3B2 is rationalized by the proposed 1B2 → 1A1 → 3B2 mechanism. Ultrafast ligation of the 1B2 Fe(CO)4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B2 Fe(CO)4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B2 → 1A1 → 1A' Fe(CO)4EtOH pathway and the time scale of the 1A1 Fe(CO)4 state ligation is governed by the solute-solvent collision frequency. Our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.
- Authors:
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- Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Univ. Potsdam, Potsdam (Germany). Institut fur Physik und Astronomie
- Stockholm Univ. (Sweden). Department of Physics
- Max Planck Institute for Biophysical Chemistry, Am Fassberg, Gottingen (Germany)
- Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). PULSE Institute
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- MAX-lab, Lund (Sweden)
- Utrecht Univ. Utrecht (Netherlands). Department of Chemistry
- Max Planck Institute for Biophysical Chemistry, Am Fassberg, Gottingen (Germany); Gottingen Univ. (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1242357
- Alternate Identifier(s):
- OSTI ID: 1335953
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Structural Dynamics
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2329-7778
- Publisher:
- American Crystallographic Association/AIP
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 43 PARTICLE ACCELERATORS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Kunnus, K., Josefsson, I., Rajkovic, I., Schreck, S., Quevedo, W., Beye, M., Weniger, C., Grübel, S., Scholz, M., Nordlund, D., Zhang, W., Hartsock, R. W., Gaffney, K. J., Schlotter, W. F., Turner, J. J., Kennedy, B., Hennies, F., de Groot, F. M. F., Techert, S., Odelius, M., Wernet, Ph., and Föhlisch, A. Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH. United States: N. p., 2016.
Web. doi:10.1063/1.4941602.
Kunnus, K., Josefsson, I., Rajkovic, I., Schreck, S., Quevedo, W., Beye, M., Weniger, C., Grübel, S., Scholz, M., Nordlund, D., Zhang, W., Hartsock, R. W., Gaffney, K. J., Schlotter, W. F., Turner, J. J., Kennedy, B., Hennies, F., de Groot, F. M. F., Techert, S., Odelius, M., Wernet, Ph., & Föhlisch, A. Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH. United States. https://doi.org/10.1063/1.4941602
Kunnus, K., Josefsson, I., Rajkovic, I., Schreck, S., Quevedo, W., Beye, M., Weniger, C., Grübel, S., Scholz, M., Nordlund, D., Zhang, W., Hartsock, R. W., Gaffney, K. J., Schlotter, W. F., Turner, J. J., Kennedy, B., Hennies, F., de Groot, F. M. F., Techert, S., Odelius, M., Wernet, Ph., and Föhlisch, A. 2016.
"Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH". United States. https://doi.org/10.1063/1.4941602. https://www.osti.gov/servlets/purl/1242357.
@article{osti_1242357,
title = {Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH},
author = {Kunnus, K. and Josefsson, I. and Rajkovic, I. and Schreck, S. and Quevedo, W. and Beye, M. and Weniger, C. and Grübel, S. and Scholz, M. and Nordlund, D. and Zhang, W. and Hartsock, R. W. and Gaffney, K. J. and Schlotter, W. F. and Turner, J. J. and Kennedy, B. and Hennies, F. and de Groot, F. M. F. and Techert, S. and Odelius, M. and Wernet, Ph. and Föhlisch, A.},
abstractNote = {Here, we utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO)5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO)4 which are observed following a charge transfer photoexcitation of Fe(CO)5 as reported in our previous study. We find that branching of the reaction pathway likely happens in the 1A1 state of Fe(CO)4. A sub-picosecond time constant of the spin crossover from 1B2 to 3B2 is rationalized by the proposed 1B2 → 1A1 → 3B2 mechanism. Ultrafast ligation of the 1B2 Fe(CO)4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B2 Fe(CO)4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B2 → 1A1 → 1A' Fe(CO)4EtOH pathway and the time scale of the 1A1 Fe(CO)4 state ligation is governed by the solute-solvent collision frequency. Our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.},
doi = {10.1063/1.4941602},
url = {https://www.osti.gov/biblio/1242357},
journal = {Structural Dynamics},
issn = {2329-7778},
number = 4,
volume = 3,
place = {United States},
year = {Tue Feb 09 00:00:00 EST 2016},
month = {Tue Feb 09 00:00:00 EST 2016}
}
Web of Science
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