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Title: Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy

Abstract

Iron N-heterocyclic carbene (NHC) complexes have received a great deal of attention recently because of their growing potential as light sensitizers or photocatalysts. Here, we present a sub-ps X-ray spectroscopy study of an FeIINHC complex that identifies absorption. Excited molecules relax back to the ground state along two pathways: After population of a hot 3MLCT state, from the initially excited 1MLCT state, 30 % of the molecules undergo ultrafast (150 fs) relaxation to the 3MC state, in comand quantifies the states involved in the deactivation cascade after light petition with vibrational relaxation and cooling to the relaxed 3MLCT state. The relaxed 3MLCT state then decays much more slowly (7.6 ps) to the 3MC state. The 3MC state is rapidly (2.2 ps) deactivated to the ground state. The 5MC state is not involved in the deactivation pathway. The ultrafast partial deactivation of the 3MLCT state constitutes a loss channel from the point of view of photochemical efficiency and highlights the necessity to screen transition-metal complexes for similar ultrafast decays to optimize photochemical performance.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4];  [3]; ORCiD logo [3] more »; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [6];  [6]; ORCiD logo [6]; ORCiD logo [6];  [6]; ORCiD logo [7];  [8]; ORCiD logo [9]; ORCiD logo [10]; ORCiD logo [3]; ORCiD logo [3];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Lund Univ. (Sweden)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  3. Technical Univ. of Denmark, Lyngby (Denmark)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Technical Univ. of Denmark, Lyngby (Denmark)
  5. Hungarian Academy of Sciences, Budapest (Hungary)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  9. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); ELI-HU Non-Profit Ltd., Szeged (Hungary)
  10. Technical Univ. of Denmark, Lyngby (Denmark); Univ. of Iceland, Reykjavik (Iceland)
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). Chemical Sciences, Geosciences & Biosciences Division; Independent Research Fund Denmark; Icelandic Research Fund; European Union (EU); European Regional Development Fund; Hungarian Academy of Sciences; Government of Hungary; National Research, Development and Innovation Fund; Knut and Alice Wallenberg Foundation
OSTI Identifier:
1633958
Alternate Identifier(s):
OSTI ID: 1572578
Grant/Contract Number:  
AC02-76SF00515; DFF‐4002‐00272; DFF‐8021‐00347B; 196279‐051; GINOP‐2.3.6‐15‐2015‐00001; LP2013‐59; VEKOP‐2.3.2–16–2017‐00015; NKFIH-FK-124460; KAW2014.0370
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 1; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; femtochemistry molecular dynamics; photochemistry; photophysics; X-ray spectroscopy

Citation Formats

Tatsuno, Hideyuki, Kjær, Kasper S., Kunnus, Kristjan, Harlang, Tobias C. B., Timm, Cornelia, Guo, Meiyuan, Chàbera, Pavel, Fredin, Lisa A., Hartsock, Robert W., Reinhard, Marco E., Koroidov, Sergey, Li, Lin, Cordones, Amy A., Gordivska, Olga, Prakash, Om, Liu, Yizhu, Laursen, Mads G., Biasin, Elisa, Hansen, Frederik B., Vester, Peter, Christensen, Morten, Haldrup, Kristoffer, Németh, Zoltán, Sárosiné Szemes, Dorottya, Bajnóczi, Éva, Vankó, György, Van Driel, Tim B., Alonso‐Mori, Roberto, Glownia, James M., Nelson, Silke, Sikorski, Marcin, Lemke, Henrik T., Sokaras, Dimosthenis, Canton, Sophie E., Dohn, Asmus O., Møller, Klaus B., Nielsen, Martin M., Gaffney, Kelly J., Wärnmark, Kenneth, Sundström, Villy, Persson, Petter, and Uhlig, Jens. Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy. United States: N. p., 2019. Web. doi:10.1002/anie.201908065.
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Tatsuno, Hideyuki, Kjær, Kasper S., Kunnus, Kristjan, Harlang, Tobias C. B., Timm, Cornelia, Guo, Meiyuan, Chàbera, Pavel, Fredin, Lisa A., Hartsock, Robert W., Reinhard, Marco E., Koroidov, Sergey, Li, Lin, Cordones, Amy A., Gordivska, Olga, Prakash, Om, Liu, Yizhu, Laursen, Mads G., Biasin, Elisa, Hansen, Frederik B., Vester, Peter, Christensen, Morten, Haldrup, Kristoffer, Németh, Zoltán, Sárosiné Szemes, Dorottya, Bajnóczi, Éva, Vankó, György, Van Driel, Tim B., Alonso‐Mori, Roberto, Glownia, James M., Nelson, Silke, Sikorski, Marcin, Lemke, Henrik T., Sokaras, Dimosthenis, Canton, Sophie E., Dohn, Asmus O., Møller, Klaus B., Nielsen, Martin M., Gaffney, Kelly J., Wärnmark, Kenneth, Sundström, Villy, Persson, Petter, & Uhlig, Jens. Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy. United States. https://doi.org/10.1002/anie.201908065
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Tatsuno, Hideyuki, Kjær, Kasper S., Kunnus, Kristjan, Harlang, Tobias C. B., Timm, Cornelia, Guo, Meiyuan, Chàbera, Pavel, Fredin, Lisa A., Hartsock, Robert W., Reinhard, Marco E., Koroidov, Sergey, Li, Lin, Cordones, Amy A., Gordivska, Olga, Prakash, Om, Liu, Yizhu, Laursen, Mads G., Biasin, Elisa, Hansen, Frederik B., Vester, Peter, Christensen, Morten, Haldrup, Kristoffer, Németh, Zoltán, Sárosiné Szemes, Dorottya, Bajnóczi, Éva, Vankó, György, Van Driel, Tim B., Alonso‐Mori, Roberto, Glownia, James M., Nelson, Silke, Sikorski, Marcin, Lemke, Henrik T., Sokaras, Dimosthenis, Canton, Sophie E., Dohn, Asmus O., Møller, Klaus B., Nielsen, Martin M., Gaffney, Kelly J., Wärnmark, Kenneth, Sundström, Villy, Persson, Petter, and Uhlig, Jens. Thu . "Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy". United States. https://doi.org/10.1002/anie.201908065. https://www.osti.gov/servlets/purl/1633958.
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@article{osti_1633958,
title = {Hot Branching Dynamics in a Light-Harvesting Iron Carbene Complex Revealed by Ultrafast X-ray Emission Spectroscopy},
author = {Tatsuno, Hideyuki and Kjær, Kasper S. and Kunnus, Kristjan and Harlang, Tobias C. B. and Timm, Cornelia and Guo, Meiyuan and Chàbera, Pavel and Fredin, Lisa A. and Hartsock, Robert W. and Reinhard, Marco E. and Koroidov, Sergey and Li, Lin and Cordones, Amy A. and Gordivska, Olga and Prakash, Om and Liu, Yizhu and Laursen, Mads G. and Biasin, Elisa and Hansen, Frederik B. and Vester, Peter and Christensen, Morten and Haldrup, Kristoffer and Németh, Zoltán and Sárosiné Szemes, Dorottya and Bajnóczi, Éva and Vankó, György and Van Driel, Tim B. and Alonso‐Mori, Roberto and Glownia, James M. and Nelson, Silke and Sikorski, Marcin and Lemke, Henrik T. and Sokaras, Dimosthenis and Canton, Sophie E. and Dohn, Asmus O. and Møller, Klaus B. and Nielsen, Martin M. and Gaffney, Kelly J. and Wärnmark, Kenneth and Sundström, Villy and Persson, Petter and Uhlig, Jens},
abstractNote = {Iron N-heterocyclic carbene (NHC) complexes have received a great deal of attention recently because of their growing potential as light sensitizers or photocatalysts. Here, we present a sub-ps X-ray spectroscopy study of an FeIINHC complex that identifies absorption. Excited molecules relax back to the ground state along two pathways: After population of a hot 3MLCT state, from the initially excited 1MLCT state, 30 % of the molecules undergo ultrafast (150 fs) relaxation to the 3MC state, in comand quantifies the states involved in the deactivation cascade after light petition with vibrational relaxation and cooling to the relaxed 3MLCT state. The relaxed 3MLCT state then decays much more slowly (7.6 ps) to the 3MC state. The 3MC state is rapidly (2.2 ps) deactivated to the ground state. The 5MC state is not involved in the deactivation pathway. The ultrafast partial deactivation of the 3MLCT state constitutes a loss channel from the point of view of photochemical efficiency and highlights the necessity to screen transition-metal complexes for similar ultrafast decays to optimize photochemical performance.},
doi = {10.1002/anie.201908065},
journal = {Angewandte Chemie (International Edition)},
number = 1,
volume = 59,
place = {United States},
year = {Thu Oct 10 00:00:00 EDT 2019},
month = {Thu Oct 10 00:00:00 EDT 2019}
}
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https://doi.org/10.1002/anie.201908065
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Figure 1 Figure 1: The bidentate FeII complex studied in this paper. Hydrogen atoms omitted for clarity.
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    Works referencing / citing this record:

    Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
    text, January 2020

    • Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B.
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
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    Design and Synthesis of Photoactive Iron N-Heterocyclic Carbene Complexes
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    Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
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    • Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B.
    • Nature Communications, Vol. 11, Issue 1
    • DOI: 10.1038/s41467-020-14468-w

    Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
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    • Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B.
    • Nature Communications, Vol. 11, Issue 1
    • DOI: 10.1038/s41467-020-14468-w
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