Abstract
| Original language | English |
|---|---|
| Journal | Angewandte Chemie |
| Volume | 132 |
| Issue number | 1 |
| Pages (from-to) | 372-380 |
| Number of pages | 9 |
| ISSN | 0044-8249 |
| DOIs | |
| Publication status | Published - 2020 |
Keywords
- Femtochemie
- Moleküldynamik
- Photochemie
- Photophysik
- Röntgenspektroskopie
Cite this
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Hot branching dynamics in a light‐harvesting iron carbene complex revealed by ultrafast x‐ray emission spectroscopy. / Tatsuno, Hideyuki; Kjær, Kasper Skov; Kunnus, Kristjan; Harlang, Tobias C. B.; Timm, Cornelia; Guo, Meiyuan; Chabera, Pavel; Fredin, Lisa A.; Hartsock, Robert W.; Reinhard, Marco E.; Koroidov, Sergey; Li, Lin; Cordones, Amy; Gordivska, Olga; Prakash, Om; Liu, Yizhu; Laursen, Mads; Biasin, Elisa; Hansen, Frederik Beyer Kjær; Vester, Peter; Christensen, Morten; Haldrup, Kristoffer; Németh, Zoltán; Sárosiné Szemes, Dorottya; Bajnóczi, Éva; Vankó, György; van Driel, Tim B.; Alonso-Mori, Roberto; Glownia, James; Nelson, Silke; Sikorski, Marcin; Lemke, Henrik Till; Sokaras, Dimosthenis; Canton, Sophie E.; Dohn, Asmus Ougaard; Møller, Klaus Braagaard; Nielsen, Martin Meedom; Gaffney, Kelly J.; Wärnmark, Kenneth; Sundström, Villy; Persson, Petter; Uhlig, Jens.
In: Angewandte Chemie, Vol. 132, No. 1, 2020, p. 372-380.Research output: Contribution to journal › Journal article › Research › peer-review
TY - JOUR
T1 - Hot branching dynamics in a light‐harvesting iron carbene complex revealed by ultrafast x‐ray emission spectroscopy
AU - Tatsuno, Hideyuki
AU - Kjær, Kasper Skov
AU - Kunnus, Kristjan
AU - Harlang, Tobias C. B.
AU - Timm, Cornelia
AU - Guo, Meiyuan
AU - Chabera, Pavel
AU - Fredin, Lisa A.
AU - Hartsock, Robert W.
AU - Reinhard, Marco E.
AU - Koroidov, Sergey
AU - Li, Lin
AU - Cordones, Amy
AU - Gordivska, Olga
AU - Prakash, Om
AU - Liu, Yizhu
AU - Laursen, Mads
AU - Biasin, Elisa
AU - Hansen, Frederik Beyer Kjær
AU - Vester, Peter
AU - Christensen, Morten
AU - Haldrup, Kristoffer
AU - Németh, Zoltán
AU - Sárosiné Szemes, Dorottya
AU - Bajnóczi, Éva
AU - Vankó, György
AU - van Driel, Tim B.
AU - Alonso-Mori, Roberto
AU - Glownia, James
AU - Nelson, Silke
AU - Sikorski, Marcin
AU - Lemke, Henrik Till
AU - Sokaras, Dimosthenis
AU - Canton, Sophie E.
AU - Dohn, Asmus Ougaard
AU - Møller, Klaus Braagaard
AU - Nielsen, Martin Meedom
AU - Gaffney, Kelly J.
AU - Wärnmark, Kenneth
AU - Sundström, Villy
AU - Persson, Petter
AU - Uhlig, Jens
PY - 2020
Y1 - 2020
N2 - Iron nitrogen heterocyclic carbenes (NHC) have received a great deal of attention recently, due to their growing potential as e.g light sensitizers and photocatalysts. We present a sub-ps x-ray spectroscopy study of a FeIINHC complex allowing us to identify and quantify the states involved in the deactivation cascade after light absorption. We find that excited molecules relax back to the ground state populating first the 3MLCT and then along two pathways the 3MC state. One of these pathways is ultrafast (~150 fs) for ~30% of the excited molecules, in competition with vibrational relaxation and cooling, followed by a much slower (7.6 ps) decay of the relaxed 3MLCT state. The 3MC state then rapidly (2.2 ps) decays to the ground state. The ultrafast deactivation of the 3MLCT state constitutes a loss channel from the point of view of photochemical efficiency and highlights the necessity to screen other FeNHC complexes (and perhaps other transition metal complexes) for this ultrafast decay of 3MLCT population, in order to optimize photochemical performance.
AB - Iron nitrogen heterocyclic carbenes (NHC) have received a great deal of attention recently, due to their growing potential as e.g light sensitizers and photocatalysts. We present a sub-ps x-ray spectroscopy study of a FeIINHC complex allowing us to identify and quantify the states involved in the deactivation cascade after light absorption. We find that excited molecules relax back to the ground state populating first the 3MLCT and then along two pathways the 3MC state. One of these pathways is ultrafast (~150 fs) for ~30% of the excited molecules, in competition with vibrational relaxation and cooling, followed by a much slower (7.6 ps) decay of the relaxed 3MLCT state. The 3MC state then rapidly (2.2 ps) decays to the ground state. The ultrafast deactivation of the 3MLCT state constitutes a loss channel from the point of view of photochemical efficiency and highlights the necessity to screen other FeNHC complexes (and perhaps other transition metal complexes) for this ultrafast decay of 3MLCT population, in order to optimize photochemical performance.
KW - Femtochemie
KW - Moleküldynamik
KW - Photochemie
KW - Photophysik
KW - Röntgenspektroskopie
U2 - 10.1002/ange.201908065
DO - 10.1002/ange.201908065
M3 - Journal article
VL - 132
SP - 372
EP - 380
JO - Angewandte Chemie
JF - Angewandte Chemie
SN - 0044-8249
IS - 1
ER -