Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

Abstract

Ultrafast X-ray imaging on individual fragile specimens such as aerosols1, metastable particles2, superfluid quantum systems3 and live biospecimens4 provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined4,5. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.

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Fig. 1: Principles of in-flight holography.
Fig. 2: Experimental setup.
Fig. 3: Hologram and reconstructions.
Fig. 4: 3D reconstruction.
Fig. 5: Holograms of deformed specimen recorded with small reference clusters.

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Acknowledgements

We would like to thank J. Geilhufe, E. Guehrs, A. Schropp and S. Eisebitt for many helpful discussions. T.G. acknowledges the P. Ewald fellowship from the Volkswagen Foundation and the Panofsky fellowship from SLAC National Accelerator Laboratory. We would like to thank J. Segal and A. Tomada from SLAC for providing high-resistivity Si wafers. 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 Sciences, Geosciences, and Biosciences under contract no. DE-AC02-06CH11357 and contract no. DE-AC02-76SF00515. T.M. acknowledges financial support from BMBF (German Federal Ministry of Education and Research) projects 05K10KT2 and 05K13KT2 as well as DFG (German Research Foundation) BO3169/2-2. This work was supported by the Swedish Research Council, the Knut and Alice Wallenberg Foundation, the European Research Council, the Röntgen-Angström Cluster, ELI Extreme Light Infrastructure Phase 2 (CZ.02.1.01/0.0/0.0/15 008/0000162), ELIBIO (CZ.02.1.01/0.0/0.0/15 003/0000447) from the European Regional Development Fund, Material science and the Chalmers Area of Advance. F.R.N.C.M. acknowledges the Swedish Foundation for Strategic Research. Portions of this research were carried out at Brookhaven National Laboratory, operated under contract no. DE-SC0012704 from the US Department of Energy Office of Science. G.F. acknowledges the support of NKFIH K115504.

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Contributions

T.G. conceived the concept of 'in-flight' holography with two sources with support from C.B., T.M. and J.H. The project was led by T.G., C.B., F.R.N.C.M. and J.H. The experimental setup was designed and the experiment was performed by all authors. The bioparticle injector was operated by J.B., M.Sei. and K.M.. The cluster source was operated by K.F., M.B., C.B. and T.G. The biological samples were prepared by D.H., D.S.D.L., K.O. and M.Sve. The online and offline data analysis was carried out by F.M., T.E., M.F.H., B.J.D., C.N., A.M., G.v.S., M.B. and K.F. The images were analysed and processed by A.U. and T.G. The results were interpreted by A.U. and T.G. with input from C.B., G.F., T.M., F.R.N.C.M. and J.H. The manuscript was written by T.G. and A.U. with contributions from C.B., G.F., T.M., F.M. and J.H. and input from all authors.

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Correspondence to Tais Gorkhover.

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Gorkhover, T., Ulmer, A., Ferguson, K. et al. Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles. Nature Photon 12, 150–153 (2018). https://doi.org/10.1038/s41566-018-0110-y

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