L-edge X-ray absorption spectroscopy of dilute systems relevant to 
metalloproteins using an X-ray free-electron laser.

Mitzner, R.; Rehanek, J.; Kern, J.; Gul, S.; Hattne, J.; Taguchi, T.; Alonso-Mori, R.; Tran, R.; Weniger, C.; Schröder, H.; Quevedo, W.; Laksmono, H.; Sierra, R. G.; Han, G.; Lasalle-Kaiser, B.; Koroidov, S.; Kubicek, K.; Schreck, S.; Kunnus, K.; Brzhezinskaya, M.; Firsov, A.; Minitti, M. P.; Turner, J. J.; Moseller, S.; Sauter, N. K.; Bogan, M. J.; Nordlund, D.; Schlotter, W. F.; Messinger, J.; Borovik, A.; Techert, S.; de Groot, F. M. F.; Föhlisch, A.; Erko, A.; Bergmann, U.; Yachandra, V. K.; Wernet, P.; Yano, J.

doi:10.1021/jz401837f

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L-edge X-ray absorption spectroscopy of dilute systems relevant to metalloproteins using an X-ray free-electron laser.

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Techert, S.
Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for biophysical chemistry, Max Planck Society;

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Citation

Mitzner, R., Rehanek, J., Kern, J., Gul, S., Hattne, J., Taguchi, T., et al. (2013). L-edge X-ray absorption spectroscopy of dilute systems relevant to metalloproteins using an X-ray free-electron laser. The Journal of Physical Chemistry Letters, 4(21), 3641-3647. doi:10.1021/jz401837f.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0014-A0D8-3

Abstract

L-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS). The spectrometer has been optimized for discriminating the Mn L-edge signal from the overwhelming O K-edge background that arises from water and protein itself, and the ultrashort LCLS X-ray pulses can outrun X-ray induced damage. We show that the deviations of the partial-fluorescence yield-detected spectra from the true absorption can be well modeled using the state-dependence of the fluorescence yield, and discuss implications for the application of our concept to biological samples.