Ultrafast x-ray pump x-ray probe transient absorption spectroscopy: A computational study and proposed experiment probing core-valence electronic correlations in solvated complexes

Liekhus-Schmaltz, Chelsea E.; Ho, Phay J.; Weakly, Robert B.; Aquila, Andrew; Schoenlein, Robert W.; Khalil, Munira; Govind, Niranjan

doi:10.1063/5.0047381

Title: Ultrafast x-ray pump x-ray probe transient absorption spectroscopy: A computational study and proposed experiment probing core-valence electronic correlations in solvated complexes

Journal Article · 01 June 2021 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0047381 · OSTI ID:1785528

^[1];

^[2];

^[1];

^[3];

^[4];

^[1];

^[5]

Univ. of Washington, Seattle, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Institute
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Femtosecond X-ray pump X-ray probe experiments are currently possible at free electron lasers such as the linac coherent light source (LCLS), which opens new opportunities for studying solvated transition metal-ligand complexes. In order to make the most effective use of these kinds of experiments, it is necessary to determine which chemical properties an X-ray pump pulse will measure. In this paper, we have combined electron cascade calculations and excited-state time-dependent density functional theory calculations to predict the initial state prepared by an X-ray pump and the subsequent X-ray probe spectra at the Fe K-edge in the solvated model transition metal complex, K₄Fe^II(CN)₆. We find several key spectral features that report on the ligand-field splitting, solvent-solute interactions, and the 3p and 3d electron interactions. We then show how these features could be measured in an experiment.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; AC05-76RL01830; SC0019277

OSTI ID:: 1785528

Report Number(s):: PNNL-SA--160027

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 154; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (52)

X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 Henke, B. L.; Gullikson, E. M.; Davis, J. C. Atomic Data and Nuclear Data Tables, Vol. 54, Issue 2, p. 181-342 https://doi.org/10.1006/adnd.1993.1013	journal	July 1993
Segmented contracted basis sets for atoms H through Xe: Sapporo-(DK)-nZP sets (n = D, T, Q) Noro, Takeshi; Sekiya, Masahiro; Koga, Toshikatsu Theoretical Chemistry Accounts, Vol. 131, Issue 2 https://doi.org/10.1007/s00214-012-1124-z	journal	February 2012
Ultrafast photophysics and photochemistry of iron hexacyanides in solution: Infrared to X-ray spectroscopic studies Chergui, M. Coordination Chemistry Reviews, Vol. 372 https://doi.org/10.1016/j.ccr.2018.05.021	journal	October 2018
Auger electron cascades in water and ice Tı̂mneanu, Nicuşor; Caleman, Carl; Hajdu, Janos Chemical Physics, Vol. 299, Issue 2-3 https://doi.org/10.1016/j.chemphys.2003.10.011	journal	April 2004
NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations Valiev, M.; Bylaska, E. J.; Govind, N. Computer Physics Communications, Vol. 181, Issue 9, p. 1477-1489 https://doi.org/10.1016/j.cpc.2010.04.018	journal	September 2010
Chemical analysis: Double core-hole spectroscopy with free-electron lasers Berrah, N.; Fang, L. Journal of Electron Spectroscopy and Related Phenomena, Vol. 204 https://doi.org/10.1016/j.elspec.2015.05.020	journal	October 2015
Time-resolved studies with FELs Rudenko, Artem; Rolles, Daniel Journal of Electron Spectroscopy and Related Phenomena, Vol. 204 https://doi.org/10.1016/j.elspec.2015.07.010	journal	October 2015
Simulating Valence-to-Core X-ray Emission Spectroscopy of Transition Metal Complexes with Time-Dependent Density Functional Theory Zhang, Yu; Mukamel, Shaul; Khalil, Munira Journal of Chemical Theory and Computation, Vol. 11, Issue 12 https://doi.org/10.1021/acs.jctc.5b00763	journal	November 2015
Comprehensive Experimental and Computational Spectroscopic Study of Hexacyanoferrate Complexes in Water: From Infrared to X-ray Wavelengths Ross, Matthew; Andersen, Amity; Fox, Zachary W. The Journal of Physical Chemistry B, Vol. 122, Issue 19 https://doi.org/10.1021/acs.jpcb.7b12532	journal	April 2018
Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy) ₂ ] ²⁺ Vankó, György; Bordage, Amélie; Pápai, Mátyás The Journal of Physical Chemistry C, Vol. 119, Issue 11 https://doi.org/10.1021/acs.jpcc.5b00557	journal	March 2015
Stimulated X-ray Raman Imaging of Conical Intersections Cho, Daeheum; Mukamel, Shaul The Journal of Physical Chemistry Letters, Vol. 11, Issue 1 https://doi.org/10.1021/acs.jpclett.9b03020	journal	November 2019
Linear-Response and Real-Time Time-Dependent Density Functional Theory Studies of Core-Level Near-Edge X-Ray Absorption Lopata, K.; Van Kuiken, B. E.; Khalil, M. Journal of Chemical Theory and Computation, Vol. 8, Issue 9 https://doi.org/10.1021/ct3005613	journal	August 2012
Ultrafast Excited State Relaxation of a Metalloporphyrin Revealed by Femtosecond X-ray Absorption Spectroscopy Shelby, Megan L.; Lestrange, Patrick J.; Jackson, Nicholas E. Journal of the American Chemical Society, Vol. 138, Issue 28 https://doi.org/10.1021/jacs.6b02176	journal	July 2016
Polarized XANES Monitors Femtosecond Structural Evolution of Photoexcited Vitamin B ₁₂ Miller, Nicholas A.; Deb, Aniruddha; Alonso-Mori, Roberto Journal of the American Chemical Society, Vol. 139, Issue 5 https://doi.org/10.1021/jacs.6b11295	journal	January 2017
Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics Lemke, Henrik T.; Bressler, Christian; Chen, Lin X. The Journal of Physical Chemistry A, Vol. 117, Issue 4 https://doi.org/10.1021/jp312559h	journal	January 2013
Simulating Ru L ₃ -Edge X-ray Absorption Spectroscopy with Time-Dependent Density Functional Theory: Model Complexes and Electron Localization in Mixed-Valence Metal Dimers Van Kuiken, Benjamin E.; Valiev, Marat; Daifuku, Stephanie L. The Journal of Physical Chemistry A, Vol. 117, Issue 21 https://doi.org/10.1021/jp401020j	journal	May 2013
A Smooth Solvation Potential Based on the Conductor-Like Screening Model York, Darrin M.; Karplus, Martin The Journal of Physical Chemistry A, Vol. 103, Issue 50 https://doi.org/10.1021/jp992097l	journal	December 1999
High-intensity double-pulse X-ray free-electron laser Marinelli, A.; Ratner, D.; Lutman, A. A. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7369	journal	March 2015
Ultrafast isomerization initiated by X-ray core ionization Liekhus-Schmaltz, Chelsea E.; Tenney, Ian; Osipov, Timur Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9199	journal	September 2015
Direct observation of coherent femtosecond solvent reorganization coupled to intramolecular electron transfer Biasin, Elisa; Fox, Zachary W.; Andersen, Amity Nature Chemistry, Vol. 13, Issue 4 https://doi.org/10.1038/s41557-020-00629-3	journal	February 2021
Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser Duris, Joseph; Li, Siqi; Driver, Taran Nature Photonics https://doi.org/10.1038/s41566-019-0549-5	journal	December 2019
Double-pulse speckle contrast correlations with near Fourier transform limited free-electron laser light using hard X-ray split-and-delay Roseker, Wojciech; Lee, Sooheyong; Walther, Michael Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-61926-y	journal	March 2020
Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy Driver, Taran; Li, Siqi; Champenois, Elio G. Physical Chemistry Chemical Physics, Vol. 22, Issue 5 https://doi.org/10.1039/c9cp03951a	journal	January 2020
Revealing the bonding of solvated Ru complexes with valence-to-core resonant inelastic X-ray scattering Biasin, Elisa; Nascimento, Daniel R.; Poulter, Benjamin I. Chemical Science, Vol. 12, Issue 10 https://doi.org/10.1039/d0sc06227h	journal	January 2021
COSMO: a new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient Klamt, A.; Schüürmann, G. J. Chem. Soc., Perkin Trans. 2, Issue 5 https://doi.org/10.1039/p29930000799	journal	January 1993
Self‐consistent molecular orbital methods. XX. A basis set for correlated wave functions Krishnan, R.; Binkley, J. S.; Seeger, R. The Journal of Chemical Physics, Vol. 72, Issue 1 https://doi.org/10.1063/1.438955	journal	January 1980
Contracted Gaussian basis sets for molecular calculations. I. Second row atoms, Z=11–18 McLean, A. D.; Chandler, G. S. The Journal of Chemical Physics, Vol. 72, Issue 10, p. 5639-5648 https://doi.org/10.1063/1.438980	journal	May 1980
A single-shot transmissive spectrometer for hard x-ray free electron lasers Zhu, Diling; Cammarata, Marco; Feldkamp, Jan M. Applied Physics Letters, Vol. 101, Issue 3 https://doi.org/10.1063/1.4736725	journal	July 2012
Toward reliable density functional methods without adjustable parameters: The PBE0 model Adamo, Carlo; Barone, Vincenzo The Journal of Chemical Physics, Vol. 110, Issue 13 https://doi.org/10.1063/1.478522	journal	April 1999
Ultraviolet photochemical reaction of [Fe(III)(C2O4)3]3− in aqueous solutions studied by femtosecond time-resolved X-ray absorption spectroscopy using an X-ray free electron laser Ogi, Y.; Obara, Y.; Katayama, T. Structural Dynamics, Vol. 2, Issue 3 https://doi.org/10.1063/1.4918803	journal	April 2015
Generating femtosecond X-ray pulses using an emittance-spoiling foil in free-electron lasers Ding, Y.; Behrens, C.; Coffee, R. Applied Physics Letters, Vol. 107, Issue 19 https://doi.org/10.1063/1.4935429	journal	November 2015
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
NWChem: Past, present, and future Aprà, E.; Bylaska, E. J.; de Jong, W. A. The Journal of Chemical Physics, Vol. 152, Issue 18 https://doi.org/10.1063/5.0004997	journal	May 2020
Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme Inoue, Ichiro; Inubushi, Yuichi; Sato, Takahiro Proceedings of the National Academy of Sciences, Vol. 113, Issue 6 https://doi.org/10.1073/pnas.1516426113	journal	January 2016
X-ray-excited Auger and photoelectron spectroscopy Weightman, P. Reports on Progress in Physics, Vol. 45, Issue 7 https://doi.org/10.1088/0034-4885/45/7/002	journal	July 1982
Direct Hartree-Fock calculation of multiple Xe ⁱ⁺ ion production through inner shell vacancy de-excitations Kochur, A. G.; Dudenko, A. I.; Sukhorukov, V. L. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 27, Issue 9 https://doi.org/10.1088/0953-4075/27/9/011	journal	May 1994
Direct Hartree-Fock calculation of the cascade decay production of multiply charged ions following inner-shell ionization of Ne, Ar, Kr and Xe Kochur, A. G.; Sukhorukov, V. L.; Dudenko, A. J. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 28, Issue 3 https://doi.org/10.1088/0953-4075/28/3/010	journal	February 1995
Probing ultrafast electronic and molecular dynamics with free-electron lasers Fang, L.; Osipov, T.; Murphy, B. F. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 47, Issue 12 https://doi.org/10.1088/0953-4075/47/12/124006	journal	June 2014
Resonant x-ray absorption of strong-field-ionized CF ₃ Br Fouda, A. E. A.; Ho, P. J.; Dunford, R. W. Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 53, Issue 24 https://doi.org/10.1088/1361-6455/abc49a	journal	November 2020
Stimulated Raman adiabatic passage with two-color x-ray pulses Picón, Antonio; Mompart, Jordi; Southworth, Stephen H. New Journal of Physics, Vol. 17, Issue 8 https://doi.org/10.1088/1367-2630/17/8/083038	journal	August 2015
X-ray split and delay system for soft x-rays at LCLS Castagna, J. C.; Murphy, B.; Bozek, J. Journal of Physics: Conference Series, Vol. 425, Issue 15 https://doi.org/10.1088/1742-6596/425/15/152021	journal	March 2013
Development of ultrafast capabilities for X-ray free-electron lasers at the linac coherent light source Coffee, Ryan N.; Cryan, James P.; Duris, Joseph Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2018.0386	journal	April 2019
Resonance-mediated atomic ionization dynamics induced by ultraintense x-ray pulses Ho, Phay J.; Kanter, E. P.; Young, L. Physical Review A, Vol. 92, Issue 6 https://doi.org/10.1103/physreva.92.063430	journal	December 2015
Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy Lehmann, C. S.; Picón, A.; Bostedt, C. Physical Review A, Vol. 94, Issue 1 https://doi.org/10.1103/physreva.94.013426	journal	July 2016
Experimental Demonstration of Femtosecond Two-Color X-Ray Free-Electron Lasers Lutman, A. A.; Coffee, R.; Ding, Y. Physical Review Letters, Vol. 110, Issue 13 https://doi.org/10.1103/physrevlett.110.134801	journal	March 2013
Theoretical Tracking of Resonance-Enhanced Multiple Ionization Pathways in X-ray Free-Electron Laser Pulses Ho, Phay J.; Bostedt, Christoph; Schorb, Sebastian Physical Review Letters, Vol. 113, Issue 25 https://doi.org/10.1103/physrevlett.113.253001	journal	December 2014
Delayed Onset of Nonthermal Melting in Single-Crystal Silicon Pumped with Hard X Rays Pardini, T.; Alameda, J.; Aquila, A. Physical Review Letters, Vol. 120, Issue 26 https://doi.org/10.1103/physrevlett.120.265701	journal	June 2018
Observation of Seeded Mn K β Stimulated X-Ray Emission Using Two-Color X-Ray Free-Electron Laser Pulses Kroll, Thomas; Weninger, Clemens; Fuller, Franklin D. Physical Review Letters, Vol. 125, Issue 3 https://doi.org/10.1103/physrevlett.125.037404	journal	July 2020
Observation of shock-induced protein crystal damage during megahertz serial femtosecond crystallography Grünbein, Marie L.; Foucar, Lutz; Gorel, Alexander Physical Review Research, Vol. 3, Issue 1 https://doi.org/10.1103/physrevresearch.3.013046	journal	January 2021
The Coherent X-ray Imaging instrument at the Linac Coherent Light Source Liang, Mengning; Williams, Garth J.; Messerschmidt, Marc Journal of Synchrotron Radiation, Vol. 22, Issue 3 https://doi.org/10.1107/s160057751500449x	journal	April 2015
The X-ray Pump–Probe instrument at the Linac Coherent Light Source Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco Journal of Synchrotron Radiation, Vol. 22, Issue 3 https://doi.org/10.1107/s1600577515005135	journal	April 2015
Two-color X-ray free-electron laser consisting of broadband and narrowband beams Inoue, Ichiro; Osaka, Taito; Hara, Toru Journal of Synchrotron Radiation, Vol. 27, Issue 6 https://doi.org/10.1107/s1600577520011716	journal	October 2020

Similar Records

Ultrafast tabletop laser-pump-x-ray probe measurement of solvated Fe(CN){sub 6}{sup 4-}

Journal Article · 2005 · Journal of Chemical Physics · OSTI ID:20662312

Lee, Taewoo; Yan, Jiang; Rose-Petruck, Christoph G; +1 more

Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy

Journal Article · 2023 · Nature Communications · OSTI ID:1984540

Weakly, Robert B.; Liekhus-Schmaltz, Chelsea E.; Poulter, Benjamin I.; +14 more

Probing Ultrafast Electron (De)localization Dynamics in Mixed Valence Complexes Using Femtosecond X-ray Spectroscopy (Final Report)

Technical Report · 2019 · OSTI ID:1576203

Khalil, Munira; Govind, Niranjan; Mukamel, Shaul; +1 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Ultrafast x-ray pump x-ray probe transient absorption spectroscopy: A computational study and proposed experiment probing core-valence electronic correlations in solvated complexes

Citation Formats

References (52)

Similar Records

Related Subjects