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.

doi:10.1038/s41467-020-14468-w

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

Journal Article · Fri Jan 31 00:00:00 EST 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-14468-w· OSTI ID:1619477

; ; Harlang, Tobias C. B.; Kjær, Kasper S.; ; Biasin, Elisa; van Driel, Tim B.; ; ; Liu, Yizhu; Tatsuno, Hideyuki; Timm, Cornelia; Källman, Erik; Delcey, Mickaël; Hartsock, Robert W.; ; Koroidov, Sergey; Laursen, Mads G.; Hansen, Frederik B.; more »

Abstract

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 ( ³ MC) excited state surface. This ³ MC state is populated with a 110 fs time constant by 40% of the excited molecules while the rest relax to a ³ MLCT 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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Danish Council for Independent Research; Independent Research Fund Denmark; Knut and Alice Wallenberg Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1619477

Alternate ID(s):: OSTI ID: 1605173

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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