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Femtosecond and nanometre visualization of structural dynamics in superheated nanoparticles

Abstract

The ability to observe ultrafast structural changes in nanoscopic samples is essential for understanding non-equilibrium phenomena such as chemical reactions1, matter under extreme conditions2, ultrafast phase transitions3 and intense light–matter interactions4. Established imaging techniques are limited either in time or spatial resolution and typically require samples to be deposited on a substrate, which interferes with the dynamics. Here, we show that coherent X-ray diffraction images from isolated single samples can be used to visualize femtosecond electron density dynamics. We recorded X-ray snapshot images from a nanoplasma expansion, a prototypical non-equilibrium phenomenon4,5. Single Xe clusters are superheated using an intense optical laser pulse and the structural evolution of the sample is imaged with a single X-ray pulse. We resolved ultrafast surface softening on the nanometre scale at the plasma/vacuum interface within 100 fs of the heating pulse. Our study is the first time-resolved visualization of irreversible femtosecond processes in free, individual nanometre-sized samples.

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Figure 1: Experimental set-up.
Figure 2: Time-dependent diffraction patterns.
Figure 3: Simulation of diffraction patterns.

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Acknowledgements

T.G. acknowledges a Peter Ewald fellowship from the Volkswagen Foundation. Parts of this research were carried out at the Linac Coherent Light Source (LCLS) at the SLAC National Accelerator Laboratory. LCLS is an Office of Science User Facility operated for the US Department of Energy Office of Science by Stanford University. This work is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical, Geological and Biological Sciences (contract nos. DE-AC02-06CH11357 (C.B.), DE-AC02-76SF00515 (C.B. and R.C.) and DE-FG02-86ER13491 (D.Ro. and A.R.)). T.M. acknowledges financial support from BMBF projects 05K10KT2 and 05K13KT2 as well as DFG BO3169/2-2. P.J. acknowledges support from the Swedish Research Council and the Swedish Foundation for Strategic Research. M.M. acknowledges support from the National Science Foundation (award no. 1231306). The authors acknowledge the Max Planck Society for funding the development and operation of the CAMP instrument within the ASG at CFEL. The authors thank T. Fennel for discussions, and M. Swiggers, J.-C. Castagna and all LCLS staff for their help in setting up and performing the experiments.

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Contributions

C.B. conceived the idea and coordinated the project together with T.G., S.Sc., R.C., D.Ro., A.Ru. and T.M. The experimental setup was designed by all authors. The laser system was prepared by R.C., T.G., L.H., P.J., J.K., A.Ro. and B.W. The pnCCD detectors were developed and operated by A.H., R.H., G.H., P.H., N.K., C.R., G.W., H.S. and L.S. The experiment was performed by T.G., S.Ss., R.C., M.A., L.F., A.A., J.D.B., B.E., R.H., P.H., N.K., K.-U.K., C.R., B.R., J.S., G.W., J.U., D.Ro., A.Ru., T.M. and C.B. The CASS online and offline data analysis software was developed by L.F. The data were analysed by T.G. The results were interpreted by T.G., T.M. and C.B. The manuscript was written by T.G. and C.B. with contributions from T.M. and I.S. as well as input from all authors.

Corresponding authors

Correspondence to Tais Gorkhover or Christoph Bostedt.

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The authors declare no competing financial interests.

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Gorkhover, T., Schorb, S., Coffee, R. et al. Femtosecond and nanometre visualization of structural dynamics in superheated nanoparticles. Nature Photon 10, 93–97 (2016). https://doi.org/10.1038/nphoton.2015.264

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