Energy-dispersive X-ray emission spectroscopy using an X-ray free-electron laser in a shot-by-shot mode. Alonso-Mori, R., Kern, J., Gildea, R. J., Sokaras, D., Weng, T., Lassalle-Kaiser, B., Tran, R., Hattne, J., Laksmono, H., Hellmich, J., Glöckner, C., Echols, N., Sierra, R. G., Schafer, D. W., Sellberg, J., Kenney, C., Herbst, R., Pines, J., Hart, P., Herrmann, S., Grosse-Kunstleve, R. W., Latimer, M. J., Fry, A. R., Messerschmidt, M. M., Miahnahri, A., Seibert, M. M., Zwart, P. H., White, W. E., Adams, P. D., Bogan, M. J., Boutet, S., Williams, G. J., Zouni, A., Messinger, J., Glatzel, P., Sauter, N. K., Yachandra, V. K., Yano, J., & Bergmann, U. Proceedings of the National Academy of Sciences, 109(47):19103–19107, November, 2012. Publisher: Proceedings of the National Academy of Sciences
Energy-dispersive X-ray emission spectroscopy using an X-ray free-electron laser in a shot-by-shot mode [link]Paper  doi  abstract   bibtex   
The ultrabright femtosecond X-ray pulses provided by X-ray free-electron lasers open capabilities for studying the structure and dynamics of a wide variety of systems beyond what is possible with synchrotron sources. Recently, this “probe-before-destroy” approach has been demonstrated for atomic structure determination by serial X-ray diffraction of microcrystals. There has been the question whether a similar approach can be extended to probe the local electronic structure by X-ray spectroscopy. To address this, we have carried out femtosecond X-ray emission spectroscopy (XES) at the Linac Coherent Light Source using redox-active Mn complexes. XES probes the charge and spin states as well as the ligand environment, critical for understanding the functional role of redox-active metal sites. Kβ1,3 XES spectra of MnII and Mn2III,IV complexes at room temperature were collected using a wavelength dispersive spectrometer and femtosecond X-ray pulses with an individual dose of up to \textgreater100 MGy. The spectra were found in agreement with undamaged spectra collected at low dose using synchrotron radiation. Our results demonstrate that the intact electronic structure of redox active transition metal compounds in different oxidation states can be characterized with this shot-by-shot method. This opens the door for studying the chemical dynamics of metal catalytic sites by following reactions under functional conditions. The technique can be combined with X-ray diffraction to simultaneously obtain the geometric structure of the overall protein and the local chemistry of active metal sites and is expected to prove valuable for understanding the mechanism of important metalloproteins, such as photosystem II.
@article{alonso-mori_energy-dispersive_2012,
	title = {Energy-dispersive {X}-ray emission spectroscopy using an {X}-ray free-electron laser in a shot-by-shot mode},
	volume = {109},
	url = {https://www.pnas.org/doi/10.1073/pnas.1211384109},
	doi = {10.1073/pnas.1211384109},
	abstract = {The ultrabright femtosecond X-ray pulses provided by X-ray free-electron lasers open capabilities for studying the structure and dynamics of a wide variety of systems beyond what is possible with synchrotron sources. Recently, this “probe-before-destroy” approach has been demonstrated for atomic structure determination by serial X-ray diffraction of microcrystals. There has been the question whether a similar approach can be extended to probe the local electronic structure by X-ray spectroscopy. To address this, we have carried out femtosecond X-ray emission spectroscopy (XES) at the Linac Coherent Light Source using redox-active Mn complexes. XES probes the charge and spin states as well as the ligand environment, critical for understanding the functional role of redox-active metal sites. Kβ1,3 XES spectra of MnII and Mn2III,IV complexes at room temperature were collected using a wavelength dispersive spectrometer and femtosecond X-ray pulses with an individual dose of up to {\textgreater}100 MGy. The spectra were found in agreement with undamaged spectra collected at low dose using synchrotron radiation. Our results demonstrate that the intact electronic structure of redox active transition metal compounds in different oxidation states can be characterized with this shot-by-shot method. This opens the door for studying the chemical dynamics of metal catalytic sites by following reactions under functional conditions. The technique can be combined with X-ray diffraction to simultaneously obtain the geometric structure of the overall protein and the local chemistry of active metal sites and is expected to prove valuable for understanding the mechanism of important metalloproteins, such as photosystem II.},
	number = {47},
	urldate = {2024-12-10},
	journal = {Proceedings of the National Academy of Sciences},
	author = {Alonso-Mori, Roberto and Kern, Jan and Gildea, Richard J. and Sokaras, Dimosthenis and Weng, Tsu-Chien and Lassalle-Kaiser, Benedikt and Tran, Rosalie and Hattne, Johan and Laksmono, Hartawan and Hellmich, Julia and Glöckner, Carina and Echols, Nathaniel and Sierra, Raymond G. and Schafer, Donald W. and Sellberg, Jonas and Kenney, Christopher and Herbst, Ryan and Pines, Jack and Hart, Philip and Herrmann, Sven and Grosse-Kunstleve, Ralf W. and Latimer, Matthew J. and Fry, Alan R. and Messerschmidt, Marc M. and Miahnahri, Alan and Seibert, M. Marvin and Zwart, Petrus H. and White, William E. and Adams, Paul D. and Bogan, Michael J. and Boutet, Sébastien and Williams, Garth J. and Zouni, Athina and Messinger, Johannes and Glatzel, Pieter and Sauter, Nicholas K. and Yachandra, Vittal K. and Yano, Junko and Bergmann, Uwe},
	month = nov,
	year = {2012},
	note = {Publisher: Proceedings of the National Academy of Sciences},
	pages = {19103--19107},
}
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