Ultrafast XANES Monitors Femtosecond Sequential Structural Evolution in Photoexcited Coenzyme B12

Miller, Nicholas A.; Michocki, Lindsay B.; Konar, Arkaprabha; Alonso-Mori, Roberto; Deb, Aniruddha; Glownia, James M.; Sofferman, Danielle L.; Song, Sanghoon; Kozlowski, Pawel M.; Kubarych, Kevin J.; Penner-Hahn, James E.; Sension, Roseanne J.

doi:10.1021/acs.jpcb.9b09286

Title: Ultrafast XANES Monitors Femtosecond Sequential Structural Evolution in Photoexcited Coenzyme B₁₂

Journal Article · Wed Dec 18 00:00:00 EST 2019 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.9b09286· OSTI ID:1605287

^[1]; Michocki, Lindsay B. ^[1];

^[2]; Alonso-Mori, Roberto ^[3];

^[4]; Glownia, James M. ^[3]; Sofferman, Danielle L. ^[5]; Song, Sanghoon ^[3];

^[6];

^[4];

^[7]

Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemistry
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemistry and Dept. of Biophysics
Univ. of Michigan, Ann Arbor, MI (United States). Applied Physics Program
Univ. of Louisville, KY (United States). Dept. of Chemistry
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemistry, Dept. of Physics, and Dept. of Biophysics

Polarized X-ray absorption near-edge structure (XANES) at the Co K-edge and broadband UV-vis transient absorption are used to monitor the sequential evolution of the excited-state structure of coenzyme B₁₂ (adenosylcobalamin) over the first picosecond following excitation. The initial state is characterized by sub-100 fs sequential changes around the central cobalt. These are polarized first in the y-direction orthogonal to the transition dipole and 50 fs later in the x-direction along the transition dipole. Expansion of the axial bonds follows on a ca. 200 fs time scale as the molecule moves out of the Franck-Condon active region of the potential energy surface. On the same 200 fs time scale there are electronic changes that result in the loss of stimulated emission and the appearance of a strong absorption at 340 nm. These measurements provide a cobalt-centered movie of the excited molecule as it evolves to the local excited-state minimum.

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515; 1464584; 1565795; 1836435

OSTI ID:: 1605287

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 124, Issue 1; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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X-ray absorption near edge spectroscopy
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Light absorption
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