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Résumé |
The past two decades have witnessed a revolution in nonlinear optical spectroscopy in condensed matter [1], with the advent of new ultrafast optical and X-ray domain methodologies enabled by new instrumentation, which extends and allows the investigation of dynamical processes in Biology. In particular, multidimensional spectroscopy allows new insights into inter-chromophoric energy or electron transfer phenomena [2], while X-ray spectroscopies deliver insights into the electronic and spin structure of specific elements and the geometric structure of their environment [3]. In this presentation, I will present some results on the 2-Dimensional deep-UV spectroscopy of electron transfer processes in proteins [4,5] and deep-UV Circular dichroism studies of molecular chirality [6,7], which promise applications for biological systems. Finally, I will present recent ultrafast X-ray spectroscopic studies of respiratory and non-respiratory haem proteins [8–10].
[1] S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford University Press, New York, 1995
[2] S. Mukamel, Y. Tanimura, and P. Hamm, Coherent Multidimensional Optical Spectroscopy, Accounts Chem Res Accounts Chem Res 42, 9 (2009).
[3] C. J. Milne, T. J. Penfold, and M. Chergui, Recent Experimental and Theoretical Developments in Time-Resolved X-Ray Spectroscopies, Coordin Chem Rev 277, 44 (2014).
[4] C. Consani, G. Aubock, F. van Mourik, and M. Chergui, Ultrafast Tryptophan-to-Haem Electron Transfer in Myoglobins Revealed by UV 2D Spectroscopy, Science 339, 1586 (2013).
[5] R. Monni, A. Al Haddad, F. van Mourik, G. Auböck, and M. Chergui, Tryptophan-to-Heme Electron Transfer in Ferrous Myoglobins, Proceedings of the National Academy of Sciences 112, 18 (2015).
[6] M. Oppermann, B. Bauer, T. Rossi, F. Zinna, J. Helbing, J. Lacour, and M. Chergui, Ultrafast Broadband Circular Dichroism in the Deep Ultraviolet, Optica, OPTICA 6, 56 (2019).
[7] M. Oppermann, F. Zinna, J. Lacour, and M. Chergui, Chiral Control of Spin-Crossover Dynamics in Fe(II) Complexes, Nat. Chem. (2022).
[8] D. Kinschel et al., Femtosecond X-Ray Emission Study of the Spin Cross-over Dynamics in Haem Proteins, Nature Communications 11, 1 (2020).
[9] C. Bacellar et al., Spin Cascade and Doming in Ferric Hemes: Femtosecond X-Ray Absorption and X-Ray Emission Studies, PNAS 117, 36 (2020).
[10] C. Bacellar et al., Femtosecond X-Ray Spectroscopy of Haem Proteins, Faraday Discuss. 228, 312 (2021). |
