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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; [...]

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

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  • Media type: E-Article
  • Title: Hot Branching Dynamics in a Light‐Harvesting Iron Carbene Complex Revealed by Ultrafast X‐ray Emission Spectroscopy
  • Contributor: 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; [...]
  • imprint: Wiley, 2020
  • Published in: Angewandte Chemie
  • Language: English
  • DOI: 10.1002/ange.201908065
  • ISSN: 0044-8249; 1521-3757
  • Keywords: General Medicine
  • Origination:
  • Footnote:
  • Description: <jats:title>Abstract</jats:title><jats:p>Iron N‐heterocyclic carbene (NHC) complexes have received a great deal of attention recently because of their growing potential as light sensitizers or photocatalysts. We present a sub‐ps X‐ray spectroscopy study of an Fe<jats:sup>II</jats:sup>NHC complex that identifies and quantifies the states involved in the deactivation cascade after light absorption. Excited molecules relax back to the ground state along two pathways: After population of a hot <jats:sup>3</jats:sup>MLCT state, from the initially excited <jats:sup>1</jats:sup>MLCT state, 30 % of the molecules undergo ultrafast (150 fs) relaxation to the <jats:sup>3</jats:sup>MC state, in competition with vibrational relaxation and cooling to the relaxed <jats:sup>3</jats:sup>MLCT state. The relaxed <jats:sup>3</jats:sup>MLCT state then decays much more slowly (7.6 ps) to the <jats:sup>3</jats:sup>MC state. The <jats:sup>3</jats:sup>MC state is rapidly (2.2 ps) deactivated to the ground state. The <jats:sup>5</jats:sup>MC state is not involved in the deactivation pathway. The ultrafast partial deactivation of the <jats:sup>3</jats:sup>MLCT 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.</jats:p>