dc.contributor |
Háskóli Íslands |
dc.contributor |
University of Iceland |
dc.contributor.author |
Kjær, Kasper S. |
dc.contributor.author |
Van Driel, Tim B. |
dc.contributor.author |
Harlang, Tobias C. B. |
dc.contributor.author |
Kunnus, Kristjan |
dc.contributor.author |
Biasin, Elisa |
dc.contributor.author |
Ledbetter, Kathryn |
dc.contributor.author |
Hartsock, Robert W. |
dc.contributor.author |
Reinhard, Marco E. |
dc.contributor.author |
Koroidov, Sergey |
dc.contributor.author |
Li, Lin |
dc.contributor.author |
Laursen, Mads G. |
dc.contributor.author |
Hansen, Frederik B. |
dc.contributor.author |
Vester, Peter |
dc.contributor.author |
Christensen, Morten |
dc.contributor.author |
Haldrup, Kristoffer |
dc.contributor.author |
Nielsen, Martin M. |
dc.contributor.author |
Ougaard Dohn, Asmus |
dc.contributor.author |
Pápai, Mátyás I. |
dc.contributor.author |
Møller, Klaus Braagaard |
dc.contributor.author |
Chabera, Pavel |
dc.contributor.author |
Liu, Yizhu |
dc.contributor.author |
Tatsuno, Hideyuki |
dc.contributor.author |
Timm, Cornelia |
dc.contributor.author |
Jarenmark, Martin |
dc.contributor.author |
Uhlig, Jens |
dc.contributor.author |
Sundstöm, Villy |
dc.contributor.author |
Wärnmark, Kenneth |
dc.contributor.author |
Persson, Petter |
dc.contributor.author |
Németh, Zoltán |
dc.contributor.author |
Szemes, Dorottya Sárosiné |
dc.contributor.author |
Bajnóczi, Éva |
dc.contributor.author |
Vankó, György |
dc.contributor.author |
Alonso-Mori, Roberto |
dc.contributor.author |
Glownia, James M. |
dc.contributor.author |
Nelson, Silke |
dc.contributor.author |
Sikorski, Marcin |
dc.contributor.author |
Sokaras, Dimosthenis |
dc.contributor.author |
Canton, Sophie E. |
dc.contributor.author |
Lemke, Henrik T. |
dc.contributor.author |
Gaffney, Kelly J. |
dc.date.accessioned |
2020-09-08T15:17:55Z |
dc.date.available |
2020-09-08T15:17:55Z |
dc.date.issued |
2019-04-22 |
dc.identifier.citation |
Kjær, K. S., Van Driel, T. B., Harlang, T. C. B., Kunnus, K., Biasin, E., Ledbetter, K., . . . Gaffney, K. J. (2019). Finding intersections between electronic excited state potential energy surfaces with simultaneous ultrafast X-ray scattering and spectroscopy. Chemical Science, 10(22), 5749-5760. doi:10.1039/C8SC04023K |
dc.identifier.issn |
2041-6520 |
dc.identifier.issn |
2041-6539 (eISSN) |
dc.identifier.uri |
https://hdl.handle.net/20.500.11815/2052 |
dc.description |
Publisher's version (útgefin grein) |
dc.description.abstract |
Light-driven molecular reactions are dictated by the excited state potential energy landscape, depending critically on the location of conical intersections and intersystem crossing points between potential surfaces where non-adiabatic effects govern transition probabilities between distinct electronic states. While ultrafast studies have provided significant insight into electronic excited state reaction dynamics, experimental approaches for identifying and characterizing intersections and seams between electronic states remain highly system dependent. Here we show that for 3d transition metal systems simultaneously recorded X-ray diffuse scattering and X-ray emission spectroscopy at sub-70 femtosecond time-resolution provide a solid experimental foundation for determining the mechanistic details of excited state reactions. In modeling the mechanistic information retrieved from such experiments, it becomes possible to identify the dominant trajectory followed during the excited state cascade and to determine the relevant loci of intersections between states. We illustrate our approach by explicitly mapping parts of the potential energy landscape dictating the light driven low-to-high spin-state transition (spin crossover) of [Fe(2,2′-bipyridine)3]2+, where the strongly coupled nuclear and electronic dynamics have been a source of interest and controversy. We anticipate that simultaneous X-ray diffuse scattering and X-ray emission spectroscopy will provide a valuable approach for mapping the reactive trajectories of light-triggered molecular systems involving 3d transition metals. |
dc.description.sponsorship |
Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Work by KK, MER, and KJG was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. KL acknowledges a Melvin and Joan Lane Stanford Graduate Fellowship. KSK, KH, MMN, MGL, PV, EB, FBH, MC gratefully acknowledge DANSCATT support for the beamtime efforts. TCBH, EB, MGL, MIP, KBM, and MMN gratefully acknowledge support by the Danish Council for Independent Research under grant no. DFF-4002-00272B. MIP, MMN, and KBM acknowledge support by the Danish Council for Independent Research under grant no. DFF-8021-00347B. KSK gratefully acknowledge the support of the Carlsberg Foundation and the Danish Council for Independent Research. MIP, DSS, EB, and GV acknowledge support from the ‘Lendület’ (Momentum) Program of the Hungarian Academy of Sciences (LP2013-59), the Government of Hungary and the European Regional Development Fund under grant No. VEKOP-2.3.2-16-2017-00015, the European Research Council via contract ERC-StG-259709 (X-cited!), the Hungarian Scientific Research Fund (OTKA) under contract K 109257, and the National Research, Development and Innovation Fund (NKFIH FK 124460). ZN acknowledges support from the Bolyai Fellowship of the Hungarian Academy of Sciences. SC acknowledges the ELI-ALPS project (GINOP-2.3.6-15-2015-00001) which is supported by the European Union and co-financed by the European Regional Development Fund. VS, JU, and PP acknowledge support from the Knut and Alice Wallenberg Foundation (KAW). SK acknowledges the support from Knut & Alice Wallenberg foundation (KAW 2014.0370). AOD acknowledges support by the Icelandic Research Fund (Grant# 196279-051). |
dc.format.extent |
5749-5760 |
dc.language.iso |
en |
dc.publisher |
Royal Society of Chemistry (RSC) |
dc.relation.ispartofseries |
Chemical Science;10(22) |
dc.rights |
info:eu-repo/semantics/openAccess |
dc.subject |
X-ray |
dc.subject |
Spectroscopy |
dc.subject |
Molecular reactions |
dc.subject |
Energy surfaces |
dc.subject |
Röntgentækni |
dc.subject |
Litrófsgreining |
dc.title |
Finding intersections between electronic excited state potential energy surfaces with simultaneous ultrafast X-ray scattering and spectroscopy |
dc.type |
info:eu-repo/semantics/article |
dcterms.license |
Open Access Article. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. |
dc.description.version |
Peer Reviewed |
dc.identifier.journal |
Chemical Science |
dc.identifier.doi |
10.1039/c8sc04023k |
dc.contributor.department |
Raunvísindastofnun (HÍ) |
dc.contributor.department |
Science Institute (UI) |
dc.contributor.school |
Verkfræði- og náttúruvísindasvið (HÍ) |
dc.contributor.school |
School of Engineering and Natural Sciences (UI) |