Control and analysis of coherence in ultrafast X-ray crystallography

by Prof. Jasper Van Thor (Imperial College, London, UK)

Tuesday 12 Nov 2024, 13:00 → 14:00 Europe/Berlin

XHQ/E1.173 (European XFEL )

 We have demonstrated a first example of a coherent control experiment of vibrational coherence with ultrafast X-ray crystallographic observation [1]. Using a two-colour, two-pulse excitation scheme, a ‘Tannor-Rice’ coherent control mechanism strongly modified the nuclear coherences seen on ultrafast time-scale with X-ray crystallography measurements of a fluorescent protein. We apply the analysis of impulsive stimulated Raman spectroscopy and coherent control methodology to the real-space observation of low frequency vibrational dynamics and displacements [1,2].  Calculation and analysis of the coherence transfer mechanism is demonstrated with quantum dynamics theory, which add the phase space analysis through Wigner transformation [2]. The results show that in these experiments the ground state coherences dominate the crystallographic dynamics on short time scale [1]. I will additionally discuss new and future classes of optical control experiments with the ability to reveal coherences, and consider the optical instrumentation that would be required [3].

[1]. Christopher D.M. Hutchison, et al. Optical control of ultrafast structural dynamics in a fluorescent protein. (2023) Nature Chemistry. 15, 1607–1615 

[2] Samuel Perrett et al. Application of Density Matrix Wigner Transforms for Ultrafast Macromolecular and Chemical X-ray Crystallography. (2024) J. Chem. Phys.160, 100901.

[3] Christopher D. M. Hutchison, Samuel Perrett and Jasper J. van Thor. XFEL Beamline Optical Instrumentation for Ultrafast Science. (2024) J. Phys. Chem. B https://doi.org/10.1021/acs.jpcb.4c01492

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