Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; van Driel, Tim B.; Adachi, Shin -ichi; Bordage, Amélie; Bressler, Christian; Chabera, Pavel; Christensen, Morten; Dohn, Asmus O.; Galler, Andreas; Gawelda, Wojciech; Gosztola, David; Haldrup, Kristoffer; Harlang, Tobias; Liu, Yizhu; Møller, Klaus B.; Németh, Zoltán; Nozawa, Shunsuke; Pápai, Mátyás; Sato, Tokushi; Sato, Takahiro; Suarez-Alcantara, Karina; Togashi, Tadashi; Tono, Kensuke; Uhlig, Jens; Vithanage, Dimali A.; Wärnmark, Kenneth; Yabashi, Makina; Zhang, Jianxin; Sundström, Villy; Nielsen, Martin M.

doi:10.1038/ncomms7359

Title: Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

Journal Article · Mon Mar 02 00:00:00 EST 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms7359· OSTI ID:1225221

Canton, Sophie E. ^[1]; Kjær, Kasper S. ^[2]; Vankó, György ^[3]; van Driel, Tim B. ^[4]; Adachi, Shin -ichi ^[5]; Bordage, Amélie ^[6]; Bressler, Christian ^[7]; Chabera, Pavel ^[1]; Christensen, Morten ^[4]; Dohn, Asmus O. ^[4]; Galler, Andreas ^[8]; Gawelda, Wojciech ^[8]; Gosztola, David ^[9]; Haldrup, Kristoffer ^[4]; Harlang, Tobias ^[1]; Liu, Yizhu ^[1]; Møller, Klaus B. ^[4]; Németh, Zoltán ^[10]; Nozawa, Shunsuke ^[5]; Pápai, Mátyás ^[10] more »

Lund Univ., Lund (Sweden)
Univ. of Copenhagen, Copenhagen (Denmark); Technical Univ. of Denmark, Lyngby (Denmark)
Hungarian Academy Sciences, Budapest (Hungary)
Technical Univ. of Denmark, Lyngby (Denmark)
High Energy Accelerator Research Organization, Ibaraki (Japan)
Hungarian Academy Sciences, Budapest (Hungary); Univ. Paris-Sud, Orsay Cedex (France)
European XFEL, Hamburg (Germany); The Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
European XFEL, Hamburg (Germany)
Argonne National Lab. (ANL), Argonne, IL (United States)
Hungarian Academy of Sciences, Budapest (Hungary)
RIKEN, Hyogo (Japan)
Japan Synchrotron Radiation Research Institute, Hyogo (Japan)

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1225221

Alternate ID(s):: OSTI ID: 1392021

Journal Information:: Nature Communications, Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 117 works

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Photoinduced valence tautomerism of a cobalt-dioxolene complex revealed with femtosecond M-edge XANES Ash, Ryan; Zhang, Kaili; Vura-Weis, Josh The Journal of Chemical Physics, Vol. 151, Issue 10 https://doi.org/10.1063/1.5115227	journal	September 2019
Elucidation of the photoaquation reaction mechanism in ferrous hexacyanide using synchrotron x-rays with sub-pulse-duration sensitivity March, Anne Marie; Doumy, Gilles; Andersen, Amity The Journal of Chemical Physics, Vol. 151, Issue 14 https://doi.org/10.1063/1.5117318	journal	October 2019
Solvent-dependent complex reaction pathways of bromoform revealed by time-resolved X-ray solution scattering and X-ray transient absorption spectroscopy Kong, Qingyu; Khakhulin, Dmitry; Shkrob, Ilya A. Structural Dynamics, Vol. 6, Issue 6 https://doi.org/10.1063/1.5132968	journal	November 2019
Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole Khalili, Khadijeh; Inhester, Ludger; Arnold, Caroline Structural Dynamics, Vol. 7, Issue 4 https://doi.org/10.1063/4.0000016	journal	July 2020
Coherent control of long-range photoinduced electron transfer by stimulated X-ray Raman processes Dorfman, Konstantin E.; Zhang, Yu; Mukamel, Shaul Proceedings of the National Academy of Sciences, Vol. 113, Issue 36 https://doi.org/10.1073/pnas.1610729113	journal	August 2016
On the calculation of x-ray scattering signals from pairwise radial distribution functions Dohn, Asmus O.; Biasin, Elisa; Haldrup, Kristoffer Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 24 https://doi.org/10.1088/0953-4075/48/24/244010	journal	November 2015
Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers Wernet, Philippe Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2017.0464	journal	April 2019
Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse Nagaya, K.; Motomura, K.; Kukk, E. Physical Review X, Vol. 6, Issue 2 https://doi.org/10.1103/physrevx.6.021035	journal	June 2016
Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop Miaja-Avila, Luis; O’Neil, Galen C.; Joe, Young I. Physical Review X, Vol. 6, Issue 3 https://doi.org/10.1103/physrevx.6.031047	journal	September 2016
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Short-wavelength free-electron laser sources and science: a review Seddon, E. A.; Clarke, J. A.; Dunning, D. J. Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2018-00596	text	January 2017
Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy Khalili, Khadijeh; Inhester, Ludger; Arnold, Caroline Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2019-02799	text	January 2019
SwissFEL: The Swiss X-ray Free Electron Laser Milne, Christopher; Schietinger, Thomas; Aiba, Masamitsu Applied Sciences, Vol. 7, Issue 7 https://doi.org/10.3390/app7070720	journal	July 2017
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Initial metal–metal bond breakage detected by fs X-ray scattering in the photolysis of Ru ₃ (CO) ₁₂ in cyclohexane at 400 nm Kong, Q. Y.; Laursen, M. G.; Haldrup, K. Photochemical & Photobiological Sciences, Vol. 18, Issue 2 https://doi.org/10.1039/c8pp00420j	journal	January 2019
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Fingerprints of electronic, spin and structural dynamics from resonant inelastic soft X-ray scattering in transient photo-chemical species Norell, Jesper; Jay, Raphael M.; Hantschmann, Markus Universität Potsdam https://doi.org/10.25932/publishup-43749	text	January 2019
Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B. Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2021-00565	text	January 2020
Chemical interactions and dynamics with femtosecond X-ray spectroscopy and the role of X-ray free-electron lasers Wernet, Philippe Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2019-02735	text	January 2019
Hot Branching Dynamics in a Light‐Harvesting Iron Carbene Complex Revealed by Ultrafast X‐ray Emission Spectroscopy Tatsuno, Hideyuki; Kjær, Kasper S.; Kunnus, Kristjan Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2021-00416	text	January 2020
Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole Khalili, Khadijeh; Inhester, Ludger; Arnold, Caroline Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2020-02649	text	January 2020
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Excited-State Solvation Structure of Transition Metal Complexes from Molecular Dynamics Simulations and Assessment of Partial Atomic Charge Methods Abedi, Mostafa; Levi, Gianluca; Zederkof, Diana B. arXiv https://doi.org/10.48550/arxiv.1812.09090	text	January 2018
Atomistic characterization of the active-site solvation dynamics of a model photocatalyst van Driel, Tim B.; Kjær, Kasper S.; Hartsock, Robert W. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13678	journal	November 2016
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Femtosecond X-ray solution scattering reveals that bond formation mechanism of a gold trimer complex is independent of excitation wavelength Kim, Kyung Hwan; Kim, Jong Goo; Oang, Key Young Structural Dynamics, Vol. 3, Issue 4 https://doi.org/10.1063/1.4948516	journal	April 2016
SVD-aided pseudo principal-component analysis: A new method to speed up and improve determination of the optimum kinetic model from time-resolved data Oang, Key Young; Yang, Cheolhee; Muniyappan, Srinivasan Structural Dynamics, Vol. 4, Issue 4 https://doi.org/10.1063/1.4979854	journal	July 2017

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