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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References
Miller, R. D. Femtosecond crystallography with ultrabright electrons and X-rays: capturing chemistry in action. Science 343, 1108–1116 (2014).
Fletcher, L. et al. Ultrabright X-ray laser scattering for dynamic warm dense matter physics. Nature Photon. 9, 274–279 (2015).
Rousse, A. et al. Non-thermal melting in semiconductors measured at femtosecond resolution. Nature 410, 65–68 (2001).
Ditmire, T. et al. Nuclear fusion from explosions of femtosecond laser-heated deuterium clusters. Nature 398, 489–492 (1999).
Bostedt, C. et al. Ultrafast X-ray scattering from single free nanoparticles as a probe for transient states of matter. Phys. Rev. Lett. 108, 093401 (2012).
Barty, A. et al. Ultrafast single-shot diffraction imaging of nanoscale dynamics. Nature Photon. 2, 415–419 (2008).
Clark, J. et al. Ultrafast three-dimensional imaging of lattice dynamics in individual gold nanocrystals. Science 341, 56–59 (2013).
Milathianaki, D. et al. Femtosecond visualization of lattice dynamics in shock-compressed matter. Science 342, 220–223 (2013).
Arnlund, D. et al. Visualizing a protein quake with time-resolved X-ray scattering at a free-electron laser. Nature Methods 11, 923–926 (2014).
Chapman, H. N. et al. Femtosecond time-delay X-ray holography. Nature 448, 676–679 (2007).
Gorkhover, T. et al. Nanoplasma dynamics of single large xenon clusters irradiated with superintense X-ray pulses from the Linac Coherent Light Source free-electron laser. Phys. Rev. Lett. 108, 245005 (2012).
Hickstein, D. D. et al. Observation and control of shock waves in individual nanoplasmas. Phys. Rev. Lett. 112, 115004 (2014).
Zherebtsov, S. et al. Controlled near-field enhanced electron acceleration from dielectric nanospheres with intense few-cycle laser fields. Nature Phys. 7, 656–662 (2011).
Gomez, L. F. et al. Shapes and vorticities of superfluid helium nanodroplets. Science 345, 906–909 (2014).
Sellberg, J. A. et al. Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature. Nature 510, 381–384 (2014).
Emma, P. et al. First lasing and operation of an ångstrom-wavelength free-electron laser. Nature Photon. 4, 641–647 (2010).
Strüder, L. et al. Large-format, high-speed, X-ray pnCCDs combined with electron and ion imaging spectrometers in a multipurpose chamber for experiments at 4th generation light sources. Nucleic Instrum. Methods A 614, 483 (2010).
Schorb, S. et al. X-ray–optical cross-correlator for gas-phase experiments at the Linac Coherent Light Source free-electron laser. Appl. Phys. Lett. 100, 121107 (2012).
Guinier, A. & Fournet, G. Small-Angle Scattering of X-Rays (Structure of Matter series, Wiley, 1955).
Mora, P. Collisionless expansion of a Gaussian plasma into a vacuum. Phys. Plasmas 12, 112102 (2005).
Medvedev, Y. V. Expansion of a finite plasma into a vacuum. Plasma Phys. Control. Fusion 47, 1031 (2005).
Hau-Riege, S. P. & Chapman, H. N. Modeling of the damage dynamics of nanospheres exposed to X-ray free-electron-laser radiation. Phys. Rev. E 77, 041902 (2008).
Peltz, C., Varin, C., Brabec, T. & Fennel, T. Time-resolved X-ray imaging of anisotropic nanoplasma expansion. Phys. Rev. Lett. 113, 133401 (2014).
Chung, H.-K., Chen, M., Morgan, W., Ralchenko, Y. & Lee, R. FLYCHK generalized population kinetics and spectral model for rapid spectroscopic analysis for all elements. High Ener. Dens. Phys. 1, 3–12 (2005).
Aquila, A. et al. The LINAC coherent light source single particle imaging road map. Struct. Dynam. 2, 041701 (2015).
Harmand, M. et al. Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers. Nature Photon. 7, 215–218 (2013).
Hartmann, N. et al. Sub-femtosecond precision measurement of relative X-ray arrival time for free-electron lasers. Nature Photon. 8, 706–709 (2014).
Schulz, S. et al. Femtosecond all-optical synchronization of an X-ray free-electron laser. Nature Commun. 6, 5938 (2015).
Loh, N. D. et al. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight. Nature 486, 513–517 (2012).
Bryan, W. et al. Atomic excitation during recollision-free ultrafast multi-electron tunnel ionization. Nature Phys. 2, 379–383 (2006).
Rupp, D. et al. Generation and structure of extremely large clusters in pulsed jets. J. Chem. Phys. 141, 044306 (2014).
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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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.
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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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DOI: https://doi.org/10.1038/nphoton.2015.264
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