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Direct observation of coherent femtosecond solvent reorganization coupled to intramolecular electron transfer

Nature Chemistry volume 13, pages 343–349 (2021)Cite this article

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Abstract

It is well known that the solvent plays a critical role in ultrafast electron-transfer reactions. However, solvent reorganization occurs on multiple length scales, and selectively measuring short-range solute–solvent interactions at the atomic level with femtosecond time resolution remains a challenge. Here we report femtosecond X-ray scattering and emission measurements following photoinduced charge-transfer excitation in a mixed-valence bimetallic (FeiiRuiii) complex in water, and their interpretation using non-equilibrium molecular dynamics simulations. Combined experimental and computational analysis reveals that the charge-transfer excited state has a lifetime of 62 fs and that coherent translational motions of the first solvation shell are coupled to the back electron transfer. Our molecular dynamics simulations identify that the observed coherent translational motions arise from hydrogen bonding changes between the solute and nearby water molecules upon photoexcitation, and have an amplitude of tenths of ångströms, 120–200 cm−1 frequency and ~100 fs relaxation time. This study provides an atomistic view of coherent solvent reorganization mediating ultrafast intramolecular electron transfer.

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Fig. 1: Mixed-valence complex under study and experimental set-up.
Fig. 2: Fe Kβ XES tracks the MMCT excited-state population.
Fig. 3: The XSS signal.
Fig. 4: Difference scattering signals calculated from equilibrium MD simulations of the GS and MMCT state of FeRu in water.
Fig. 5: Non-equilibrium MD simulations describe the measured solvation dynamics.
Fig. 6: Results of non-equilibrium MD simulations.

Data availability

The experimental data and the simulation results that support the findings of this study are available in Figshare with the identifier https://doi.org/10.6084/m9.figshare.13322975 (ref. 59).

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Acknowledgements

This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division under award nos DE-SC0012450 (Z.W.F., J.M.C., J.D.G., Y.Z., S.M. and M.K.), DE-SC0019277 (C.L.-S. and M.K.), DE-FG02-04ER15571 (S.M.), KC-030105066418 (N.G.), KC-030105172685 (N.G.), DE-AC02-76SF00515 (E.B., K.L., K.S.K, K.H., J.H.L., M.R., K.J.G., R.W.S. and A.A.C) and DE-AC02-06CH11357 (G.D., A.M.M. and S.H.S.). J.D.G. acknowledges support by the National Science Foundation Graduate Research Fellowship Program (no. DGE-1256082). Use of the Linac Coherent Light Source, SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. This research used resources of the Advanced Photon Source, a US Department of Energy Office of Science User Facility operated for the US Department of Energy Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. This research benefited from computational resources provided by the Environmental Molecular Sciences Laboratory, a US Department of Energy Office of Science User Facility sponsored by the Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory. The Pacific Northwest National Laboratory is operated by Battelle Memorial Institute for the US Department of Energy under US Department of Energy contract no. DE-AC05-76RL1830. This research also used resources from the National Energy Research Scientific Computing Center, a US Department of Energy Office of Science User Facility operated under contract no. DE-AC02-05CH11231.

Author information

Author notes

  1. Julia M. Carlstad & James D. Gaynor

    Present address: Department of Chemistry, University of California, Berkeley, CA, USA

  2. Kiryong Hong

    Present address: Gas Metrology Group, Division of Chemical and Biological Metrology, Korea Research Institute of Standards and Science, Daejeon, Republic of Korea

  3. Jae Hyuk Lee

    Present address: Pohang Accelerator Laboratory, Pohang, Republic of Korea

  4. Yu Zhang

    Present address: Q-Chem, Pleasanton, CA, USA

Authors and Affiliations

  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Elisa Biasin, Kathryn Ledbetter, Kasper S. Kjær, Marco Reinhard, Kelly J. Gaffney, Robert W. Schoenlein & Amy A. Cordones

  2. Department of Chemistry, University of Washington, Seattle, WA, USA

    Zachary W. Fox, Julia M. Carlstad, James D. Gaynor, Chelsea Liekhus-Schmaltz & Munira Khalil

  3. Environmental Molecular Sciences Division, Earth and Biological Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, USA

    Amity Andersen

  4. Department of Physics, Technical University of Denmark, Kongens Lyngby, Denmark

    Kasper S. Kjær

  5. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Roberto Alonso-Mori, Matthieu Chollet, James M. Glownia, Thomas Kroll, Dimosthenis Sokaras & Robert W. Schoenlein

  6. Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Kiryong Hong & Jae Hyuk Lee

  7. Department of Chemistry, Physics, and Astronomy, University of California, Irvine, CA, USA

    Yu Zhang & Shaul Mukamel

  8. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

    Gilles Doumy, Anne Marie March & Stephen H. Southworth

  9. Physical Sciences Division, Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, USA

    Niranjan Govind

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Contributions

Z.W.F., K.S.K., R.A.-M., M.C., J.D.G., J.M.G., K.H., T.K., J.H.L., M.R., D.S., R.W.S., N.G., A.A.C. and M.K. prepared and conducted the experiment at the Linac Coherent Light Source. Z.W.F., K.H., J.H.L., G.D., A.M.M., S.H.S. and A.A.C. measured the reference iron spectra at the Advanced Photon Source. J.M.C. synthesized the sample. E.B. analysed the experimental data and performed the MD simulations. E.B and K.L. analysed the results from the MD simulations. A.A., Y.Z., S.M. and N.G. performed the quantum-mechanics/molecular-mechanics, density functional theory and TDDFT calculations. E.B., K.L., C.L.-S., K.J.G., R.W.S., N.G., A.A.C. and M.K. interpreted the results. E.B. and A.A.C. wrote the article with contributions from all authors.

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Correspondence to Elisa Biasin, Niranjan Govind, Amy A. Cordones or Munira Khalil.

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Supplementary Discussions 1–9, Figs. 1–24 and Tables 1–2.

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Biasin, E., Fox, Z.W., Andersen, A. et al. Direct observation of coherent femtosecond solvent reorganization coupled to intramolecular electron transfer. Nat. Chem. 13, 343–349 (2021). https://doi.org/10.1038/s41557-020-00629-3

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