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Sub-femtosecond precision measurement of relative X-ray arrival time for free-electron lasers

Abstract

Today's brightest coherent X-ray sources, X-ray free-electron lasers, produce ultrafast X-ray pulses for which full-width at half-maximum durations as short as 3 fs have been measured1. There has been a marked increase in the popularity of such short pulses now that optical timing techniques have begun to report an X-ray/optical delay below 10 fs r.m.s. errors. As a result, sub-10 fs optical pulses have been implemented at the Linac Coherent Light Source (LCLS) X-ray beamlines, thus warranting a push to reduce the error in X-ray/optical delay measurements to the 1 fs level. Here, we report a unique two-dimensional spectrogram measurement of the relative X-ray/optical delay. This easily scalable relative delay measurement already surpasses previous techniques by an order of magnitude with its sub-1 fs temporal resolution and opens up the prospect of time-resolved X-ray measurements to the attosecond community.

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Figure 1: Schematic of the single-shot geometry for measurement of the spectrogram.
Figure 2: Edge finding.
Figure 3: Results for timing precision.

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References

  1. Ding, Y. et al. Femtosecond X-ray pulse characterization in free-electron lasers using a cross-correlation technique. Phys. Rev. Lett. 109, 254802 (2012).

    Article  ADS  Google Scholar 

  2. Fritz, D. M. et al. Ultrafast bond softening in bismuth: mapping a solid's interatomic potential with X-rays. Science 315, 633–636 (2007).

    Article  ADS  Google Scholar 

  3. Glownia, J. M. et al. Time-resolved pump–probe experiments at the LCLS. Opt. Express 18, 17620–17630 (2010).

    Article  ADS  Google Scholar 

  4. Sato, T. et al. Development of ultrafast pump and probe experimental system at SACLA. J. Phys. Conf. Ser. 425, 092009 (2013).

    Article  Google Scholar 

  5. Ding, Y. et al. Femtosecond X-ray pulse temporal characterization in free-electron lasers using a transverse deflector. Phys. Rev. ST Accel. Beams 14, 120701 (2011).

    Article  ADS  Google Scholar 

  6. Grguraš, I. et al. Ultrafast X-ray pulse characterization at free-electron lasers. Nature Photon. 6, 852–857 (2012).

    Article  ADS  Google Scholar 

  7. Hoffmann, M. C. & Turner, J. J. Ultrafast X-ray experiments using terahertz excitation. Synchrotron Radiat. News 25, 17–24 (2012).

    Article  Google Scholar 

  8. Cunovic, S. et al. Time-to-space mapping in a gas medium for the temporal characterization of vacuum-ultraviolet pulses. Appl. Phys. Lett. 90, 121112 (2007).

    Article  ADS  Google Scholar 

  9. Bionta, M. R. et al. Spectral encoding of X-ray/optical relative delay. Opt. Express 19, 21855–21865 (2011).

    Article  ADS  Google Scholar 

  10. 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).

    Article  ADS  Google Scholar 

  11. Krupin, O. et al. Temporal cross-correlation of X-ray free electron and optical lasers using soft X-ray pulse induced transient reflectivity. Opt. Express 20, 11396–11406 (2012).

    Article  ADS  Google Scholar 

  12. Harmand, M. et al. Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers. Nature Photon. 7, 215–218 (2013).

    Article  ADS  Google Scholar 

  13. Riedel, R. et al. Single-shot pulse duration monitor for extreme ultraviolet and X-ray free-electron lasers. Nature Commun. 4, 1731 (2013).

    Article  ADS  Google Scholar 

  14. Mukamel, S., Healion, D., Zhang, Y. & Biggs, J. D. Multidimensional attosecond resonant X-ray spectroscopy of molecules: lessons from the optical regime. Annu. Rev. Phys. Chem. 64, 101–127 (2013).

    Article  ADS  Google Scholar 

  15. Biggs, J. D., Zhang, Y., Healion, D. & Mukamel, S. Two-dimensional stimulated resonance Raman spectroscopy of molecules with broadband X-ray pulses. J. Chem. Phys 136, 174117 (2012).

    Article  ADS  Google Scholar 

  16. Gahl, C. et al. A femtosecond X-ray/optical cross-correlator. Nature Photon. 2, 165–169 (2008).

    Article  ADS  Google Scholar 

  17. Beye, M. et al. X-ray pulse preserving single-shot optical cross-correlation method for improved experimental temporal resolution. Appl. Phys. Lett. 100, 121108 (2012).

    Article  ADS  Google Scholar 

  18. Sokolowski-Tinten, K., Cavalleri, A. & von der Linde, D. Single-pulse time- and fluence-resolved optical measurements at femtosecond excited surfaces. Appl. Phys. A 69, 577–579 (1999).

    Article  ADS  Google Scholar 

  19. Bionta, M. R. et al. Spectral encoding based measurement of X-ray/optical relative delay to 10 fs rms. Proc. SPIE 8504, 85040M 10.1117/12.929097(2012).

    Article  Google Scholar 

  20. Kane, D. J. & Trebino, R. Characterization of arbitrary femtosecond pulses using frequency-resolved optical gating. IEEE J. Quantum Electron. 29, 571–579 (1993).

    Article  ADS  Google Scholar 

  21. Ziaja, B., London, R. A. & Hajdu, J. Unified model of secondary electron cascades in diamond. J. Appl. Phys. 97, 064905 (2005).

    Article  ADS  Google Scholar 

  22. Medvedev, N., Jeschke, H. O. & Ziaja, B. Nonthermal phase transitions in semiconductors induced by a femtosecond extreme ultraviolet laser pulse. New J. Phys. 15, 015016 (2013).

    Article  ADS  Google Scholar 

  23. Sundaram, S. K. & Mazur, E. Inducing and probing non-thermal transitions in semiconductors using femtosecond laser pulses. Nature Mater. 1, 217–224 (2002).

    Article  ADS  Google Scholar 

  24. Cohen, L. Time-frequency distributions—a review. Proc. IEEE 77, 941–981 (1989).

    Article  ADS  Google Scholar 

  25. Gu, X. et al. Generation of carrier-envelope-phase-stable 2-cycle 740-μJ pulses at 2.1-μm carrier wavelength. Opt. Express 17, 62–69 (2009).

    Article  ADS  Google Scholar 

  26. Linden, S., Giessen, H. & Kuhl, J. XFROG—a new method for amplitude and phase characterization of weak ultrashort pulses. Phys. Status Solidi B 206, 119–124 (1998).

    Article  ADS  Google Scholar 

  27. Hauri, C. P. et al. Generation of intense, carrier-envelope phase-locked few-cycle laser pulses through filamentation. Appl. Phys. B 79, 673–677 (2004).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

The authors thank S. Durbin, D. Reis, A. Lindahl and R. Schoenlein for discussions of bulk material X-ray interactions. W.H. acknowledges financial support from a Marie Curie fellowship. T.F. acknowledges financial support from National Center of Competence in Research, Molecular Ultrafast Science and Technology. This research was 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.

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Contributions

N.H. and R.N.C conceived and coordinated the experiment. M.R.B., J.G. and R.N.C. carried out sample preparation. N.H., W.H., A.G., J.M.G., D.J.K. and R.N.C. built the optical set-up. M.R.B., K.R.F., S.S., M.L.S., S.C., C.B., J.-C.C. and J.B. carried out instrument control and integration. N.H. and D.J.K. performed data analysis. N.H., R.N.C., T.F., C.P.H. and W.H. interpreted data. R.N.C., T.F., C.P.H., A.R.F., W.E.W. and S.L.M. oversaw manuscript production. N.H. wrote the paper with extensive suggestions from R.N.C., T.F., C.P.H., W.H. and D.J.K. and contributions from all other authors.

Corresponding authors

Correspondence to N. Hartmann or R. N. Coffee.

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Competing interests

D.J.K., head of Mesa Photonics, has referenced some of the results herein for SBIR proposals regarding the development of temporal X-ray diagnostics.

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Hartmann, N., Helml, W., Galler, A. et al. Sub-femtosecond precision measurement of relative X-ray arrival time for free-electron lasers. Nature Photon 8, 706–709 (2014). https://doi.org/10.1038/nphoton.2014.164

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