Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
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Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering. / Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C B; Kjær, Kasper S; Haldrup, Kristoffer; Biasin, Elisa; van Driel, Tim B; Pápai, Mátyás; Chabera, Pavel; Liu, Yizhu; Tatsuno, Hideyuki; Timm, Cornelia; Källman, Erik; Delcey, Mickaël; Hartsock, Robert W; Reinhard, Marco E; Koroidov, Sergey; Laursen, Mads G; Hansen, Frederik B; Vester, Peter; Christensen, Morten; Sandberg, Lise; Németh, Zoltán; Szemes, Dorottya Sárosiné; Bajnóczi, Éva; Alonso-Mori, Roberto; Glownia, James M; Nelson, Silke; Sikorski, Marcin; Sokaras, Dimosthenis; Lemke, Henrik T; Canton, Sophie E; Møller, Klaus B; Nielsen, Martin M; Vankó, György; Wärnmark, Kenneth; Sundström, Villy; Persson, Petter; Lundberg, Marcus; Uhlig, Jens; Gaffney, Kelly J.
In: Nature Communications, Vol. 11, No. 1, 634, 31.01.2020.Research output: Contribution to journal › Journal article › Research › peer-review
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TY - JOUR
T1 - Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering
AU - Kunnus, Kristjan
AU - Vacher, Morgane
AU - Harlang, Tobias C B
AU - Kjær, Kasper S
AU - Haldrup, Kristoffer
AU - Biasin, Elisa
AU - van Driel, Tim B
AU - Pápai, Mátyás
AU - Chabera, Pavel
AU - Liu, Yizhu
AU - Tatsuno, Hideyuki
AU - Timm, Cornelia
AU - Källman, Erik
AU - Delcey, Mickaël
AU - Hartsock, Robert W
AU - Reinhard, Marco E
AU - Koroidov, Sergey
AU - Laursen, Mads G
AU - Hansen, Frederik B
AU - Vester, Peter
AU - Christensen, Morten
AU - Sandberg, Lise
AU - Németh, Zoltán
AU - Szemes, Dorottya Sárosiné
AU - Bajnóczi, Éva
AU - Alonso-Mori, Roberto
AU - Glownia, James M
AU - Nelson, Silke
AU - Sikorski, Marcin
AU - Sokaras, Dimosthenis
AU - Lemke, Henrik T
AU - Canton, Sophie E
AU - Møller, Klaus B
AU - Nielsen, Martin M
AU - Vankó, György
AU - Wärnmark, Kenneth
AU - Sundström, Villy
AU - Persson, Petter
AU - Lundberg, Marcus
AU - Uhlig, Jens
AU - Gaffney, Kelly J
PY - 2020/1/31
Y1 - 2020/1/31
N2 - The non-equilibrium dynamics of electrons and nuclei govern the function of photoactive materials. Disentangling these dynamics remains a critical goal for understanding photoactive materials. Here we investigate the photoinduced dynamics of the [Fe(bmip)2]2+ photosensitizer, where bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine, with simultaneous femtosecond-resolution Fe Kα and Kβ X-ray emission spectroscopy (XES) and X-ray solution scattering (XSS). This measurement shows temporal oscillations in the XES and XSS difference signals with the same 278 fs period oscillation. These oscillations originate from an Fe-ligand stretching vibrational wavepacket on a triplet metal-centered (3MC) excited state surface. This 3MC state is populated with a 110 fs time constant by 40% of the excited molecules while the rest relax to a 3MLCT excited state. The sensitivity of the Kα XES to molecular structure results from a 0.7% average Fe-ligand bond length shift between the 1 s and 2p core-ionized states surfaces.
AB - The non-equilibrium dynamics of electrons and nuclei govern the function of photoactive materials. Disentangling these dynamics remains a critical goal for understanding photoactive materials. Here we investigate the photoinduced dynamics of the [Fe(bmip)2]2+ photosensitizer, where bmip = 2,6-bis(3-methyl-imidazole-1-ylidine)-pyridine, with simultaneous femtosecond-resolution Fe Kα and Kβ X-ray emission spectroscopy (XES) and X-ray solution scattering (XSS). This measurement shows temporal oscillations in the XES and XSS difference signals with the same 278 fs period oscillation. These oscillations originate from an Fe-ligand stretching vibrational wavepacket on a triplet metal-centered (3MC) excited state surface. This 3MC state is populated with a 110 fs time constant by 40% of the excited molecules while the rest relax to a 3MLCT excited state. The sensitivity of the Kα XES to molecular structure results from a 0.7% average Fe-ligand bond length shift between the 1 s and 2p core-ionized states surfaces.
U2 - 10.1038/s41467-020-14468-w
DO - 10.1038/s41467-020-14468-w
M3 - Journal article
C2 - 32005815
VL - 11
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 634
ER -
ID: 243197672