Extreme ultraviolet and X-ray free-electron lasers (FELs) produce short-wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilized for many experiments previously possible only at long wavelengths: multiphoton ionization1, pumping an atomic laser2 and four-wave mixing spectroscopy3. However one important optical technique, coherent control, has not yet been demonstrated, because self-amplified spontaneous emission FELs have limited longitudinal coherence4,5,6,7. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent8,9, and two-colour emission is predicted to be coherent. Here, we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5 nm ionized neon, and we controlled the asymmetry of the photoelectron angular distribution10,11 by adjusting the phase, with a temporal resolution of 3 as. This opens the door to new short-wavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity.
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Young, L. et al. Femtosecond electronic response of atoms to ultra-intense X-rays. Nature 466, 56–61 (2010).
Rohringer, N. et al. Atomic inner-shell X-ray laser at 1.46 nanometres pumped by an X-ray free-electron laser. Nature 481, 488–491 (2012).
Bencivenga, F. et al. Four wave mixing experiments with extreme ultraviolet transient gratings. Nature 520, 205–208 (2015).
Singer, A. et al. Hanbury Brown–Twiss interferometry at a free-electron laser. Phys. Rev. Lett. 111, 034802 (2013).
Lehmkühler, F. et al. Single shot coherence properties of the free-electron laser SACLA in the hard X-ray regime. Sci. Rep. 4, 5234 (2014).
Alaimo, M. D. et al. Mapping the transverse coherence of the self amplified spontaneous emission of a free-electron laser with the heterodyne speckle method. Opt. Express 22, 30013 (2014).
Bachelard, R. et al. Wavefront analysis of nonlinear self-amplified spontaneous-emission free-electron laser harmonics in the single-shot regime. Phys. Rev. Lett. 106, 234801 (2011).
Allaria, E. et al. Highly coherent and stable pulses from the FERMI seeded free-electron laser in the extreme ultraviolet. Nature Photon. 6, 699–704 (2012).
Allaria, E. et al. Control of the polarization of a vacuum-ultraviolet, high-gain, free-electron laser. Phys. Rev. X 4, 041040 (2014).
Brumer, P. & Shapiro, M. Principles of the Quantum Control of Molecular Processes (Wiley, 2003).
Brumer, P. & Shapiro, M. Control of unimolecular reactions using coherent light. Chem. Phys. Lett. 126, 541–546 (1986).
Brif, C., Chakrabarti, R. & Rabitz, H. Control of quantum phenomena: past, present and future. New J. Phys. 12, 075008 (2010).
Ehlotzky, F. Atomic phenomena in bichromatic laser fields. Phys. Reports 345, 175–264 (2001).
Yin, Y.-Y., Chen, C., Elliott, D. S. & Smith, A. V. Asymmetric photoelectron angular distributions from interfering photoionization processes. Phys. Rev. Lett. 69, 2353 (1992).
Baranova, N. B. et al. Observation of an interference of one- and two-photon ionization of the sodium 4s state. JETP Lett. 55, 439–444 (1992).
Wang, Z.-M. & Elliott, D. S. Determination of the phase difference between even and odd continuum wave functions in atoms through quantum interference measurements. Phys. Rev. Lett. 87, 173001 (2001).
Baranova, N. B. & Zel'dovich, B. Ya. Physical effects in optical fields with non-zero average cube, <E3> ≠ 0. J. Opt. Soc. Am. 8, 27–32 (1991).
Sorgenfrei, F. et al. The extreme ultraviolet split and femtosecond delay unit at the plane grating monochromator beamline PG2 at FLASH. Rev. Sci. Instrum. 81, 043107 (2010).
Tzallas, P., Charalambidis, D., Papadogiannis, N. A., Witte, K. & Tsakiris, G. D. Direct observation of attosecond light bunching. Nature 426, 267–271 (2003).
Mauritsson, J. et al. Attosecond pulse trains generated using two color laser fields. Phys. Rev. Lett. 97, 013001 (2006).
Paul, P. M. et al. Observation of a train of attosecond pulses from high harmonic generation. Science 292, 1689–1692 (2001).
Ranitovic, P. et al. Attosecond vacuum UV coherent control of molecular dynamics. Proc. Natl Acad. Sci. USA 111, 912–917 (2014).
Johnsson, P., Mauritsson, J., Remetter, T., L'Huillier, A. & Schafer, K. J. Attosecond control of ionization by wave-packet interference. Phys. Rev. Lett. 99, 233001 (2007).
Schumacher, D. W., Weihe, F., Muller, H. G. & Bucksbaum, P. H. Phase dependence of intense field ionization a study using two colors. Phys. Rev. Lett. 73, 1344 (1994).
Sasaki, S. Analyses for a planar variably-polarizing undulator. Nucl. Instrum. Meth. A 347, 83–86 (1994).
Diviacco, B., Bracco, R., Millo, D. & Musardo, M. Phase shifters for the FERMI@Elettra undulators. In Proc. IPAC 2011 3278–3280 (IPAC, 2011).
Zangrando, M. et al. Recent results of PADReS, the Photon Analysis Delivery and REduction System, from the FERMI FEL commissioning and user operations. J. Synch. Rad. 22, 565–570 (2015).
Franco, I. & Brumer, P. Minimum requirements for laser-induced symmetry breaking in quantum and classical mechanics. J. Phys. B: At. Mol. Opt. Phys. 41, 074003 (2008).
Garcia, G. A., Nahon, L. & Powis, I. Two-Dimensional charged particle image inversion using a polar basis function Expansion. Rev. Sci. Instrum. 75, 4989–4996 (2004).
Grum-Grzhimailo, A. N., Gryzlova, E. V., Staroselskaya, E. I., Venzke, J. & Bartschat, K. Phys. Rev. A 91, 063418 (2015).
Lyamayev, V. et al. A modular end-station for atomic, molecular, and cluster science at the Low Density Matter beamline of FERMI@Elettra. J. Phys. B 46, 164007 (2013).
Svetina, C. et al. The Low Density Matter (LDM) beamline at FERMI: optical layout and first commissioning. J. Synch. Rad. 22, 538–543 (2015).
Fawley, W. M. An enhanced GINGER simulation code with harmonic emission and HDF5 IO capabilities. In Proc. FEL (eds Abo-Bakr, M. et al.) 218, abstract MOPPH07 (BESSY, 2006); http://accelconf.web.cern.ch/AccelConf/f06/PAPERS/MOPPH073.PDF
NIST Atomic Spectra Database (NIST, accessed 31 January 2016); http://www.nist.gov/pml/data/asd.cfm
Svetina, C. et al. Characterization of the FERMI@Elettra's on-line photon energy spectrometer. In Proc. SPIE Vol. 8139 (eds Morawe, C. et al.) 81390J (SPIE, 2011).
Mazza, T. et al. Determining the polarization state of a short-wavelength free-electron laser beam using atomic circular dichroism. Nature Commun. 5, 3648 (2014).
Raimondi, L. et al. Microfocusing of the FERMI@Elettra FEL beam with a K-B active optics system: spot size predictions by application of the WISE code. Nucl. Instrum. Meth. A 710, 131–138 (2013).
We acknowledge the project CENILS (funded by the Central Europe Programme 2007–2013), which provided the wavefront sensor. We acknowledge the support of the Alexander von Humboldt Foundation (Project Tirinto), the Italian Ministry of Research (Project FIRB No. RBID08CRXK and PRIN 2010ERFKXL_006), and funding from the European Union Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No. 641789 MEDEA (Molecular Electron Dynamics investigated by IntensE Fields and Attosecond Pulses). K.B., N.D. and J.V. acknowledge support from the US National Science Foundation under grants No. PHY-1430245 and XSEDE-090031. D.I., Y.K. and K.U. are grateful for support from the X-ray Free Electron Laser Priority Strategy Program of MEXT. D.I., K.U. and T.T. are grateful for support from IMRAM, Tohoku University. T.M. and M.M. acknowledge support by the Deutsche Forschungsgemeinschaft (DFG) under grant nos. SFB 925/A1 and A3. A.N.G.G. acknowledges support from the European XFEL. M.N. acknowledges the ERC Starting Research Grant UDYNI, grant agreement no. 307964, EC Seventh Framework Programme.
The authors declare no competing financial interests.
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Prince, K., Allaria, E., Callegari, C. et al. Coherent control with a short-wavelength free-electron laser. Nature Photon 10, 176–179 (2016). https://doi.org/10.1038/nphoton.2016.13
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