Influence of pump laser fluence on ultrafast myoglobin structural dynamics

Thomas R. M. Barends (), Alexander Gorel, Swarnendu Bhattacharyya, Giorgio Schirò, Camila Bacellar, Claudio Cirelli, Jacques-Philippe Colletier, Lutz Foucar, Marie Luise Grünbein, Elisabeth Hartmann, Mario Hilpert, James M. Holton, Philip J. M. Johnson, Marco Kloos, Gregor Knopp, Bogdan Marekha, Karol Nass, Gabriela Nass Kovacs, Dmitry Ozerov, Miriam Stricker, Martin Weik, R. Bruce Doak, Robert L. Shoeman, Christopher J. Milne, Miquel Huix-Rotllant (), Marco Cammarata and Ilme Schlichting ()
Additional contact information
Thomas R. M. Barends: Max Planck Institute for Medical Research
Alexander Gorel: Max Planck Institute for Medical Research
Swarnendu Bhattacharyya: Institut de Chimie Radicalaire, CNRS, Aix Marseille Univ
Giorgio Schirò: Université Grenoble Alpes, CEA, CNRS
Camila Bacellar: Paul Scherrer Institute
Claudio Cirelli: Paul Scherrer Institute
Jacques-Philippe Colletier: Université Grenoble Alpes, CEA, CNRS
Lutz Foucar: Max Planck Institute for Medical Research
Marie Luise Grünbein: Max Planck Institute for Medical Research
Elisabeth Hartmann: Max Planck Institute for Medical Research
Mario Hilpert: Max Planck Institute for Medical Research
James M. Holton: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory
Philip J. M. Johnson: Paul Scherrer Institute
Marco Kloos: European XFEL GmbH
Gregor Knopp: Paul Scherrer Institute
Bogdan Marekha: ENSL, CNRS, Laboratoire de Chimie UMR 5182
Karol Nass: Paul Scherrer Institute
Gabriela Nass Kovacs: Max Planck Institute for Medical Research
Dmitry Ozerov: Paul Scherrer Institute
Miriam Stricker: University of Oxford
Martin Weik: Université Grenoble Alpes, CEA, CNRS
R. Bruce Doak: Max Planck Institute for Medical Research
Robert L. Shoeman: Max Planck Institute for Medical Research
Christopher J. Milne: Paul Scherrer Institute
Miquel Huix-Rotllant: Institut de Chimie Radicalaire, CNRS, Aix Marseille Univ
Marco Cammarata: ESRF
Ilme Schlichting: Max Planck Institute for Medical Research

Nature, 2024, vol. 626, issue 8000, 905-911

Abstract: Abstract High-intensity femtosecond pulses from an X-ray free-electron laser enable pump–probe experiments for the investigation of electronic and nuclear changes during light-induced reactions. On timescales 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 transfer1,2. However, all ultrafast TR-SFX studies to date have employed such high pump laser energies that nominally several photons were absorbed per chromophore3–17. As multiphoton absorption may force the protein response into non-physiological pathways, it is of great concern18,19 whether this experimental approach20 allows valid conclusions to be drawn vis-à-vis biologically relevant single-photon-induced reactions18,19. Here we describe ultrafast pump–probe SFX experiments on the 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 dynamics21) are seen to depend strongly on pump laser energy, in line with quantum chemical analysis. Our results confirm both the feasibility and necessity of performing ultrafast TR-SFX pump–probe experiments in the linear photoexcitation regime. We consider this to be a starting point for reassessing both the design and the interpretation of ultrafast TR-SFX pump–probe experiments20 such that mechanistically relevant insight emerges.

Date: 2024
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DOI: 10.1038/s41586-024-07032-9

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