Ultrafast isomerization initiated by X-ray core ionization
Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-r...
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| Other Authors: | |
| Format: | Article |
| Language: | en_US |
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Nature Publishing Group
2015
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| Online Access: | http://hdl.handle.net/1721.1/100524 https://orcid.org/0000-0002-7609-4205 |
| _version_ | 1826194123951964160 |
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| author | Field, Robert W. |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Field, Robert W. |
| author_sort | Field, Robert W. |
| collection | MIT |
| description | Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a ‘molecular movie’ of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy. |
| first_indexed | 2024-09-23T09:51:20Z |
| format | Article |
| id | mit-1721.1/100524 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T09:51:20Z |
| publishDate | 2015 |
| publisher | Nature Publishing Group |
| record_format | dspace |
| spelling | mit-1721.1/1005242022-09-26T14:08:09Z Ultrafast isomerization initiated by X-ray core ionization Field, Robert W. Massachusetts Institute of Technology. Department of Chemistry Field, Robert W. Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a ‘molecular movie’ of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy. United States. Dept. of Energy. Office of Basic Energy Sciences 2015-12-28T12:51:30Z 2015-12-28T12:51:30Z 2015-09 2014-10 Article http://purl.org/eprint/type/JournalArticle 2041-1723 http://hdl.handle.net/1721.1/100524 Liekhus-Schmaltz, Chelsea E., Ian Tenney, Timur Osipov, Alvaro Sanchez-Gonzalez, Nora Berrah, Rebecca Boll, Cedric Bomme, et al. “Ultrafast Isomerization Initiated by X-Ray Core Ionization.” Nat Comms 6 (September 10, 2015): 8199. © 2015 Macmillan Publishers Limited https://orcid.org/0000-0002-7609-4205 en_US http://dx.doi.org/10.1038/ncomms9199 Nature Communications Creative Commons Attribution http://creativecommons.org/licenses/by/4.0/ application/pdf Nature Publishing Group Nature Publishing Group |
| spellingShingle | Field, Robert W. Ultrafast isomerization initiated by X-ray core ionization |
| title | Ultrafast isomerization initiated by X-ray core ionization |
| title_full | Ultrafast isomerization initiated by X-ray core ionization |
| title_fullStr | Ultrafast isomerization initiated by X-ray core ionization |
| title_full_unstemmed | Ultrafast isomerization initiated by X-ray core ionization |
| title_short | Ultrafast isomerization initiated by X-ray core ionization |
| title_sort | ultrafast isomerization initiated by x ray core ionization |
| url | http://hdl.handle.net/1721.1/100524 https://orcid.org/0000-0002-7609-4205 |
| work_keys_str_mv | AT fieldrobertw ultrafastisomerizationinitiatedbyxraycoreionization |