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Ultrafast single-shot diffraction imaging of nanoscale dynamics

A Corrigendum to this article was published on 01 September 2008


The transient nanoscale dynamics of materials on femtosecond to picosecond timescales is of great interest in the study of condensed phase dynamics such as crack formation, phase separation and nucleation, and rapid fluctuations in the liquid state or in biologically relevant environments. The ability to take images in a single shot is the key to studying non-repetitive behaviour mechanisms, a capability that is of great importance in many of these problems. Using coherent diffraction imaging with femtosecond X-ray free-electron-laser pulses we capture time-series snapshots of a solid as it evolves on the ultrafast timescale. Artificial structures imprinted on a Si3N4 window are excited with an optical laser and undergo laser ablation, which is imaged with a spatial resolution of 50 nm and a temporal resolution of 10 ps. By using the shortest available free-electron-laser wavelengths1 and proven synchronization methods2 this technique could be extended to spatial resolutions of a few nanometres and temporal resolutions of a few tens of femtoseconds. This experiment opens the door to a new regime of time-resolved experiments in mesoscopic dynamics.

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Figure 1: X-ray dynamic diffraction imaging.
Figure 2: Sample evolution revealed by coherent X-ray diffraction.
Figure 3: Correlation between diffraction patterns quantify the loss of mesoscale order.
Figure 4: Reference object and objects retrieved using phase retrieval.


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Special thanks are given to the scientific and technical staff of FLASH at DESY, Hamburg, in particular to T. Tschentscher, J. Schneider, J. Feldhaus, R.L. Johnson, U. Hahn, T. Nũnez, K. Tiedtke, H. Redlin, S. Toleikis, E.L. Saldin, E.A. Schneidmiller and M.V. Yurkov. We also thank J. Alameda, E. Spiller, E. Gullikson, A. Aquila, F. Dollar, T. McCarville, F. Weber, J. Crawford, C. Stockton, M. Haro, J. Robinson, H. Thomas and E. Eremina for technical help with these experiments. This work was supported by the following agencies: The US Department of Energy (DOE) Lawrence Livermore National Laboratory; The National Science Foundation Center for Biophotonics, University of California, Davis; The Advanced Light Source and National Centre for Electron Microscopy, Lawrence Berkeley Laboratory, under contract DE-AC03-76SF00098; Natural Sciences and Engineering Research Council of Canada (NSERC Postdoctoral Fellowship to M.J.B.); Sven and Lilly Lawskis Foundation (doctoral fellowship to M.M.S.); the US Department of Energy Office of Science to the Stanford Linear Accelerator Center; the European Union (TUIXS); the German Federal Ministry of Education and Research (FSP 301); The Swedish Research Council; The Swedish Foundation for International Cooperation in Research and Higher Education; and The Swedish Foundation for Strategic Research. This work was performed under the auspices of the US DOE by Lawrence Livermore National Laboratory in part under contract W-7405-Eng-48 and in part under contract DE-AC52- 07NA27344.

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H.N.C., A.B., S.Boutet and K.S.T. conceived the experiment, and A.B., H.N.C., S.Boutet, M.J.B., S.M., B.W.W., M.F. and S.Bajt contributed to its design. Samples were prepared by S.Boutet, M.J.B. and S.Bajt. A.B., S.Boutet, M.J.B., S.M., K.S.T., N.S., R.T., H.E., A.C., S.D., M.F., B.W.W., M.M.S., R.T., and J.H. carried out the experiment, in addition to K.S.T., N.S., R.T., H.E., A.C. and S.D., who were responsible for the ablation laser pulse and synchronization. A.B., H.N.C., S.M. and K.S.T. analysed the data. S.P.H.R. performed hydrodynamic modelling of sample ablation. All authors discussed the results and contributed to the final manuscript.

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Correspondence to Anton Barty or Henry N. Chapman.

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Barty, A., Boutet, S., Bogan, M. et al. Ultrafast single-shot diffraction imaging of nanoscale dynamics. Nature Photon 2, 415–419 (2008).

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