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Title: Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO) 5 to Fe(CO) 4EtOH

Abstract

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 [Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the 1A 1 state of Fe(CO) 4. A sub-picosecond time constant of the spin crossover from 1B 2 to 3B 2 is rationalized by the proposed 1B 21A 13B 2 mechanism. Ultrafast ligation of the 1B 2 Fe(CO) 4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B 2 Fe(CO) 4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B 21A 11A' Fe(CO) 4EtOH pathway and the time scale of the 1A 1 Fe(CO) 4 state ligation is governed by the solute-solvent collision frequency. In conclusion, our studymore » 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.« less

Authors:
 [1];  [2];  [3];  [1];  [4];  [4];  [4];  [3];  [3];  [5];  [6];  [6];  [6];  [7];  [7];  [4];  [8];  [9];  [10];  [2] more »;  [4];  [1] « less
  1. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy; Univ. Potsdam, Potsdam (Germany). Institut fur Physik und Astronomie
  2. Stockholm Univ. (Sweden). Department of Physics
  3. Max Planck Institute for Biophysical Chemistry, Am Fassberg, Gottingen (Germany)
  4. Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). PULSE Institute
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  8. MAX-lab, Lund (Sweden)
  9. Utrecht Univ. Utrecht (Netherlands). Department of Chemistry
  10. 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 Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1242357
Alternate Identifier(s):
OSTI ID: 1335953
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
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. 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., and Föhlisch, A. Tue . "Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO)5 to Fe(CO)4EtOH". United States. doi: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 = {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 [Wernet et al., Nature 520, 78 (2015)]. 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. In conclusion, 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},
journal = {Structural Dynamics},
number = 4,
volume = 3,
place = {United States},
year = {2016},
month = {2}
}

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