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  Influence of pump laser fluence on ultrafast structural changes in myoglobin

Barends, T. R., Bhattacharyya, S., Gorel, A., Schiro, G., Bacellar, C., Cirelli, C., et al. (2024). Influence of pump laser fluence on ultrafast structural changes in myoglobin. Nature, 1-7. doi:10.1101/2022.11.22.517513.

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Item Permalink: https://hdl.handle.net/21.11116/0000-000B-A7B8-9 Version Permalink: https://hdl.handle.net/21.11116/0000-000E-7067-0
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 Creators:
Barends, Thomas R.M.1, Author           
Bhattacharyya, Swarnendu, Author
Gorel, Alexander1, Author           
Schiro, Giorgio, Author
Bacellar, Camila, Author
Cirelli, Claudio, Author
Colletier, Jacques-Philippe, Author
Foucar, Lutz1, Author           
Grünbein, Marie Luise1, Author           
Hartmann, Elisabeth1, Author           
Hilpert, Mario1, Author           
Johnson, Philip J.M., Author
Kloos, Marco, Author
Knopp, Gregor, Author
Marekha, Bogdan, Author
Nass, Karol, Author
Nass Kovacs, Gabriela1, Author           
Ozerov, Dmitry, Author
Stricker, Miriam, Author
Weik, Martin, Author
Doak, R. Bruce1, Author           Shoeman, Robert L.1, Author           Milne, Christopher J., AuthorHuix-Rotllant, Miquel, AuthorCammarata, Marco, AuthorSchlichting, Ilme1, Author            more..
Affiliations:
1Department of Biomolecular Mechanisms, Max Planck Institute for Medical Research, Max Planck Society, ou_1497700              

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 Abstract: High-intensity femtosecond pulses from an X-ray free-electron laser enable pump probe experiments for investigating electronic and nuclear changes during light-induced reactions. On time scales ranging from femtoseconds to milliseconds and for a variety of biological systems, time-resolved serial femtosecond crystallography (TR-SFX) has provided detailed structural data for light-induced isomerization, breakage or formation of chemical bonds and electron transfer. However, all ultra-fast TR-SFX studies to date have employed such high pump laser energies that several photons were nominally absorbed per chromophore. As multiphoton absorption may force the protein response into nonphysiological pathways, it is of great concern whether this experimental approach allows valid inferences to be drawn vis-a-vis biologically relevant single-photon-induced reactions. Here we describe ultrafast pump-probe SFX experiments on photodissociation of carboxymyoglobin, showing that different pump laser fluences yield markedly different results. In particular, the dynamics of structural changes and observed indicators of the mechanistically important coherent oscillations of the Fe-CO bond distance (predicted by recent quantum wavepacket dynamics) are seen to depend strongly on pump laser energy. Our results confirm both the feasibility and necessity of performing TR-SFX pump probe experiments in the linear photoexcitation regime. We consider this to be a starting point for reassessing design and interpretation of ultrafast TR-SFX pump probe experiments such that biologically relevant insight emerges.

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Language(s): eng - English
 Dates: 2022-11-222024-01-042024-02-14
 Publication Status: Published online
 Pages: 22
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1101/2022.11.22.517513
 Degree: -

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Title: Nature
  Abbreviation : Nature
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: 1 - 7 Identifier: ISSN: 0028-0836
CoNE: https://pure.mpg.de/cone/journals/resource/954925427238