Ultrafast X-ray Absorption Near Edge Structure Reveals Ballistic Excited State Structural Dynamics

Miller, Nicholas A.; Deb, Aniruddha; Alonso-Mori, Roberto; Glownia, James M.; Kiefer, Laura M.; Konar, Arkaprabha; Michocki, Lindsay B.; Sikorski, Marcin; Sofferman, Danielle L.; Song, Sanghoon; Toda, Megan J.; Wiley, Theodore E.; Zhu, Diling; Kozlowski, Pawel M.; Kubarych, Kevin J.; Penner-Hahn, James E.; Sension, Roseanne J.

doi:10.1021/acs.jpca.8b04223

Title: Ultrafast X-ray Absorption Near Edge Structure Reveals Ballistic Excited State Structural Dynamics

Journal Article · Fri May 25 00:00:00 EDT 2018 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.8b04223· OSTI ID:1470935

Miller, Nicholas A. ^[1];

^[1]; Alonso-Mori, Roberto ^[2]; Glownia, James M. ^[2]; Kiefer, Laura M. ^[1];

^[1]; Michocki, Lindsay B. ^[1]; Sikorski, Marcin ^[3]; Sofferman, Danielle L. ^[1]; Song, Sanghoon ^[2]; Toda, Megan J. ^[4]; Wiley, Theodore E. ^[1]; Zhu, Diling ^[2]; Kozlowski, Pawel M. ^[5];

^[1]; Penner-Hahn, James E. ^[1];

^[1]

Univ. of Michigan, Ann Arbor, MI (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); European XFEL GmbH, Schenefeld (Germany)
Univ. of Louisville, Louisville, KY (United States)
Univ. of Louisville, Louisville, KY (United States); Univ. of Gdansk, Gdansk (Poland)

Here, polarized ultrafast time-resolved X-ray absorption near edge structure (XANES) allows characterization of excited state dynamics following excitation. Excitation of vitamin B₁₂, cyanocobalamin (CNCbl), in the αβ-band at 550 nm and the γ-band at 365 nm was used to uniquely resolve axial and equatorial contributions to the excited state dynamics. The structural evolution of the excited molecule is best described by a coherent ballistic trajectory on the excited state potential energy surface. Prompt expansion of the Co cavity by ca. 0.03 Å is followed by significant elongation of the axial bonds (>0.25 Å) over the first 190 fs. Subsequent contraction of the Co cavity in both axial and equatorial directions results in the relaxed S₁ excited state structure within 500 fs of excitation.

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

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

Grant/Contract Number:: CHE 1428479; CHE 1565795; CHE-1464584; AC02-76SF00515; UMO-2015/17/B/ST4/ 03733

OSTI ID:: 1470935

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 122, Issue 22; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 26 works

Citation information provided by
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Cited By (5)

Pump–probe experimental methodology at the Linac Coherent Light Source Glownia, James M.; Gumerlock, Karl; Lemke, Henrik T. Journal of Synchrotron Radiation, Vol. 26, Issue 3 https://doi.org/10.1107/s160057751900225x	journal	April 2019
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
Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering Kunnus, Kristjan; Vacher, Morgane; Harlang, Tobias C. B. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14468-w	journal	January 2020
The restricted active space followed by second-order perturbation theory method: Theory and application to the study of CuO2 and Cu2O2 systems Malmqvist, Per Åke; Pierloot, Kristine; Shahi, Abdul Rehaman Moughal The Journal of Chemical Physics, Vol. 128, Issue 20 https://doi.org/10.1063/1.2920188	journal	May 2008
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

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