Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Quantum imaging with incoherently scattered light from a free-electron laser

Abstract

The advent of accelerator-driven free-electron lasers (FEL) has opened new avenues for high-resolution structure determination via diffraction methods that go far beyond conventional X-ray crystallography methods1,2,3,4,5,6,7,8,9,10. These techniques rely on coherent scattering processes that require the maintenance of first-order coherence of the radiation field throughout the imaging procedure. Here we show that higher-order degrees of coherence, displayed in the intensity correlations of incoherently scattered X-rays from an FEL, can be used to image two-dimensional objects with a spatial resolution close to or even below the Abbe limit. This constitutes a new approach towards structure determination based on incoherent processes11,12, including fluorescence emission or wavefront distortions, generally considered detrimental for imaging applications. Our method is an extension of the landmark intensity correlation measurements of Hanbury Brown and Twiss13 to higher than second order, paving the way towards determination of structure and dynamics of matter in regimes where coherent imaging methods have intrinsic limitations14.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Scheme of the experiment.
Figure 2: Single-shot speckle pattern and experimentally derived fourth-order intensity correlation function g(4)(r1; MPx).
Figure 3: Geometry of the artificial benzene molecule.

Similar content being viewed by others

References

  1. Chapman, H. N. et al. Femtosecond diffractive imaging with a soft-X-ray free-electron laser. Nat. Phys. 2, 839–843 (2006).

    Article  Google Scholar 

  2. Chapman, H. N. et al. Femtosecond X-ray protein nanocrystallography. Nature 470, 73–77 (2011).

    Article  ADS  Google Scholar 

  3. Seibert, M. et al. Single mimivirus particles intercepted and imaged with an X-ray laser. Nature 470, 78–81 (2011).

    Article  ADS  Google Scholar 

  4. Loh, N. D. et al. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight. Nature 486, 513–517 (2012).

    Article  ADS  Google Scholar 

  5. Kupitz, C. et al. Serial time-resolved crystallography of photosystem II using a femtosecond X-ray laser. Nature 513, 261–265 (2014).

    Article  ADS  Google Scholar 

  6. Takahashi, Y. et al. Coherent diffraction imaging analysis of shape-controlled nanoparticles with focused hard X-ray free-electron laser pulses. Nano Lett. 13, 6028–6032 (2013).

    Article  ADS  Google Scholar 

  7. Barke, I. et al. The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering. Nat. Commun. 6, 6187 (2015).

    Article  ADS  Google Scholar 

  8. Neutze, R., Wouts, R., van der Spoel, D., Weckert, E. & Hajdu, H. Potential for biomolecular imaging with femtosecond X-ray pulses. Nature 406, 752–757 (2000).

    Article  ADS  Google Scholar 

  9. Aquila, A. et al. The linac coherent light source single particle imaging road map. Struct. Dyn. 2, 041701 (2015).

    Article  Google Scholar 

  10. Barty, A., Küpper, J. & Chapman, H. N. Molecular imaging using X-ray free-electron lasers. Annu. Rev. Phys. Chem. 64, 415–435 (2013).

    Article  ADS  Google Scholar 

  11. Slovik, J. M., Son, S.-K., Dixit, G., Jurek, Z. & Santra, R. Incoherent X-ray scattering in single molecule imaging. New J. Phys. 16, 073042 (2014).

    Article  ADS  Google Scholar 

  12. Gorobtsov, O. Y., Lorenz, U., Kabachnik, N. M. & Vartanyants, I. A. Theoretical study of electronic damage in single-particle imaging experiments at X-ray free-electron lasers for pulse durations from 0.1 to 10 fs. Phys. Rev. E 91, 062712 (2015).

    Article  ADS  Google Scholar 

  13. Hanbury Brown, R. & Twiss, R. Q. A test of a new type of stellar interferometer on Sirius. Nature 178, 1046–1048 (1956).

    Article  ADS  Google Scholar 

  14. Chapman, H. N. & Nugent, K. A. Coherent lensless X-ray imaging. Nat. Photon. 4, 833–839 (2010).

    Article  ADS  Google Scholar 

  15. Hanbury Brown, R. & Twiss, R. Q. Correlation between photons in two coherent beams of light. Nature 177, 27–29 (1956).

    Article  ADS  Google Scholar 

  16. Glauber, R. J. Nobel lecture: one hundred years of light quanta. Rev. Mod. Phys. 78, 1267–1278 (2006).

    Article  ADS  Google Scholar 

  17. Glauber, R. J. The quantum theory of optical coherence. Phys. Rev. 130, 2529–2539 (1963).

    Article  ADS  MathSciNet  Google Scholar 

  18. Goodman, J. W. Statistical Optics (John Wiley & Sons, 1985).

    Google Scholar 

  19. Baym, G. The physics of Hanbury Brown-Twiss intensity interferometry: from stars to nuclear collisions. Acta Phys. Pol. B 29, 1839–1884 (1998).

    ADS  Google Scholar 

  20. Singer, A. et al. Hanbury Brown-Twiss interferometry at a free-electron laser. Phys. Rev. Lett. 111, 034802 (2013).

    Article  ADS  Google Scholar 

  21. Gorobtsov, O. Y. et al. Statistical properties of a free-electron laser revealed by Hanbury Brown-Twiss interferometry. Phys. Rev. A 95, 023843 (2017).

    Article  ADS  Google Scholar 

  22. Thiel, C. et al. Quantum imaging with incoherent photons. Phys. Rev. Lett. 99, 133603 (2007).

    Article  ADS  Google Scholar 

  23. Oppel, S., Büttner, T., Kok, P. & von Zanthier, J. Superresolving multiphoton interferences with independent light sources. Phys. Rev. Lett. 109, 233603 (2012).

    Article  ADS  Google Scholar 

  24. Classen, A. et al. Superresolving imaging of irregular arrays of thermal light sources using multiphoton interferences. Phys. Rev. Lett. 117, 253601 (2016).

    Article  ADS  Google Scholar 

  25. Ackermann, W. et al. Operation of a free-electron laser from the extreme ultraviolet to the water window. Nat. Photon. 1, 336–342 (2007).

    Article  ADS  Google Scholar 

  26. Goodman, J. W. Speckle Phenomena in Optics: Theory and Applications (Roberts and Company, 2007).

    Google Scholar 

  27. Ayyer, K. et al. Macromolecular diffractive imaging using imperfect crystals. Nature 530, 202–206 (2016).

    Article  ADS  Google Scholar 

Download references

Acknowledgements

R.S., T.M., A.C., D.B. and J.v.Z. gratefully acknowledge funding by the Erlangen Graduate School in Advanced Optical Technologies (SAOT) by the German Research Foundation (DFG) in the framework of the German excellence initiative. A.C. and D.B. gratefully acknowledge financial support by the Staedtler Foundation and the Cusanuswerk, Bischöfliche Studienförderung, respectively. We acknowledge support of the Helmholtz Association through project oriented funds. I.V. acknowledges the support of the Virtual Institute VH-VI-403 of the Helmholtz Association. Y.O. and S.W. acknowledge support by the Partnership for Innovation, Education and Research (PIER) between DESY and the University of Hamburg. We are grateful to the FLASH machine operators, to the technical staff at FLASH for excellent FEL conditions, and to Holger Meyer for his contributions to the design of the experimental set-up. We appreciate fruitful discussions with E. Weckert and H. N. Chapman.

Author information

Authors and Affiliations

Authors

Contributions

J.v.Z., R.R. and I.A.V. conceived the experiment and coordinated the experimental efforts. R.S. and T.M. designed the experimental layout and provided post-measurement analysis and evaluation of experimental data. G.M. designed and built the experimental set-up. G.M., L.W., R.S., T.M., O.G., S.L., P.S. and I.Z. carried out the experiment at FLASH/DESY. A.C. and F.W. developed the idea of sequential spatial frequency filtering in 1D and 2D using higher-order intensity correlations. A.C. and D.B. developed quantum path analysis of the method and mathematical explanation for sub-Abbe resolution. A.B. installed the motor control of the diffusor stage. L.B. coordinated efforts to characterize diffusors and samples. B.F. provided silica particles for production of diffusors. K.S. prepared diffusors and thin film coatings. J.W. prepared the hole mask of the artificial benzene molecule used as sample. S.W. participated in preparation and characterization of diffusors. G.B. provided the operation of the beamline PG2 at FLASH. Y.O. participated in discussion of the theoretical basis of quantum imaging. W.W. provided the end station for measurements at the PG2 beamline. R.S., T.M., J.v.Z., R.R. and I.A.V. wrote the manuscript with contributions and improvements from all authors.

Corresponding author

Correspondence to Joachim von Zanthier.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary information

Supplementary information (PDF 309 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Schneider, R., Mehringer, T., Mercurio, G. et al. Quantum imaging with incoherently scattered light from a free-electron laser. Nature Phys 14, 126–129 (2018). https://doi.org/10.1038/nphys4301

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue date:

  • DOI: https://doi.org/10.1038/nphys4301

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing