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Femtosecond time-delay X-ray holography


Extremely intense and ultrafast X-ray pulses from free-electron lasers offer unique opportunities to study fundamental aspects of complex transient phenomena in materials. Ultrafast time-resolved methods usually require highly synchronized pulses to initiate a transition and then probe it after a precisely defined time delay. In the X-ray regime, these methods are challenging because they require complex optical systems and diagnostics. Here we propose and apply a simple holographic measurement scheme, inspired by Newton’s ‘dusty mirror’ experiment1, to monitor the X-ray-induced explosion of microscopic objects. The sample is placed near an X-ray mirror; after the pulse traverses the sample, triggering the reaction, it is reflected back onto the sample by the mirror to probe this reaction. The delay is encoded in the resulting diffraction pattern to an accuracy of one femtosecond, and the structural change is holographically recorded with high resolution. We apply the technique to monitor the dynamics of polystyrene spheres in intense free-electron-laser pulses, and observe an explosion occurring well after the initial pulse. Our results support the notion that X-ray flash imaging2,3 can be used to achieve high resolution, beyond radiation damage limits for biological samples4. With upcoming ultrafast X-ray sources we will be able to explore the three-dimensional dynamics of materials at the timescale of atomic motion.

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Figure 1: Diagram of the apparatus, similar to Newton’s dusty-mirror experiment.
Figure 2: Time-delay X-ray holograms of 140-nm-diameter polystyrene spheres.
Figure 3: Geometry for time-delay holography.
Figure 4: Determination of the explosion of polystyrene spheres.


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Special thanks are due to the scientific and technical staff of FLASH at DESY, Hamburg, in particular to T. Tschentscher, S. Dusterer, J. Schneider, J. Feldhaus, R. L. Johnson, U. Hahn, T. Nuñez, K. Tiedtke, S. Toleikis, E. L. Saldin, E. A. Schneidmiller and M. V. Yurkov. We also thank R. Lee, R. Falcone, M. Ahmed and T. Allison for discussions, and J. Alameda, E. Gullikson, F. Dollar, T. McCarville, F. Weber, J. Crawford, C. Stockton, M. Haro, J. Robinson, H. Thomas, M. Hoener and E. Eremina for technical help with these experiments. This work was supported by the following agencies: the US Department of Energy (DOE) under contract to the University of California, Lawrence Livermore National Laboratory; the National Science Foundation Center for Biophotonics, University of California, Davis; the Advanced Light Source, Lawrence Berkeley Laboratory, under DOE contract; the Natural Sciences and Engineering Research Council of Canada (postdoctoral fellowship to M.J.B.); the Swiss National Science Foundation (fellowship to U.R.); the Sven and Lilly Lawskis Foundation (doctoral fellowship to M.M.S.); the US DOE Office of Science to the Stanford Linear Accelerator Center; the European Union (TUIXS); the Swedish Research Council; the Swedish Foundation for International Cooperation in Research and Higher Education; and The Swedish Foundation for Strategic Research.

Author Contributions H.N.C. conceived the experiment, and H.N.C., S.P.H., A.B., S.M., B.W.W., S. Boutet, M.F., R.A.L. and A.S. contributed to its design. S. Bajt, E.S. and H.N.C. designed the camera and designed and characterized the dusty-mirror optics. Samples were prepared by M.J.B., W.H.B. and M.F., and characterized by M.J.B., S.M., S. Boutet and D.A.S.; H.N.C., M.J.B., A.B., S. Boutet, S.M., M.F., B.W.W., W.H.B., U.R., T.M., C.B., D.A.S., F.B., M.B., C.C., G.H., M.M.S. and J.H. carried out the experiment. M.K., R.T. and E.P. interfaced the experiment to FLASH and developed diagnostics. H.N.C., S.P.H., M.J.B. and M.B. carried out data analysis. All authors discussed the results and contributed to the final manuscript.

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Chapman, H., Hau-Riege, S., Bogan, M. et al. Femtosecond time-delay X-ray holography. Nature 448, 676–679 (2007).

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