Ultrafast XANES Monitors Femtosecond Sequential Structural Evolution in Photoexcited Coenzyme B12
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.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2020 |
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| Erschienen: |
2020 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:124 |
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| Enthalten in: |
The journal of physical chemistry. B - 124(2020), 1 vom: 09. Jan., Seite 199-209 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Miller, Nicholas A [VerfasserIn] |
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| Links: |
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| Themen: |
Cobamamide |
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| Anmerkungen: |
Date Completed 15.01.2021 Date Revised 15.01.2021 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/acs.jpcb.9b09286 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM304515515 |
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| 500 | |a Date Revised 15.01.2021 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status MEDLINE | ||
| 520 | |a 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 | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Research Support, U.S. Gov't, Non-P.H.S. | |
| 650 | 7 | |a Cobamides |2 NLM | |
| 650 | 7 | |a Solvents |2 NLM | |
| 650 | 7 | |a cobamamide |2 NLM | |
| 650 | 7 | |a F0R1QK73KB |2 NLM | |
| 700 | 1 | |a Michocki, Lindsay B |e verfasserin |4 aut | |
| 700 | 1 | |a Konar, Arkaprabha |e verfasserin |4 aut | |
| 700 | 1 | |a Alonso-Mori, Roberto |e verfasserin |4 aut | |
| 700 | 1 | |a Deb, Aniruddha |e verfasserin |4 aut | |
| 700 | 1 | |a Glownia, James M |e verfasserin |4 aut | |
| 700 | 1 | |a Sofferman, Danielle L |e verfasserin |4 aut | |
| 700 | 1 | |a Song, Sanghoon |e verfasserin |4 aut | |
| 700 | 1 | |a Kozlowski, Pawel M |e verfasserin |4 aut | |
| 700 | 1 | |a Kubarych, Kevin J |e verfasserin |4 aut | |
| 700 | 1 | |a Penner-Hahn, James E |e verfasserin |4 aut | |
| 700 | 1 | |a Sension, Roseanne J |e verfasserin |4 aut | |
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