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Attosecond coherent control of electronic wave packets in two-colour photoionization using a novel timing tool for seeded free-electron laser

Nature Photonics volume 17, pages 200–207 (2023)Cite this article

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Abstract

In ultrafast spectroscopy, the temporal resolution of time-resolved experiments depends on the duration of the pump and probe pulses, and on the control and characterization of their relative synchronization. Free-electron lasers operating in the extreme ultraviolet and X-ray spectral regions deliver pulses with femtosecond and attosecond duration in a broad array of pump–probe configurations to study a wide range of physical processes. However, this flexibility, together with the large dimensions and high complexity of the experimental set-ups, limits control of the temporal delay to the femtosecond domain, thus precluding a time resolution below the optical cycle. Here we demonstrate a novel single-shot technique able to determine the relative synchronization between an attosecond pulse train—generated by a seeded free-electron laser—and the optical oscillations of a near-infrared field, with a resolution of one atomic unit (24 as). Using this attosecond timing tool, we report the first example of attosecond coherent control of photoionization in a two-colour field by manipulating the phase of high-order near-infrared transitions.

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Fig. 1: Principle of the attosecond timing tool.
Fig. 2: Experimental reconstruction of sideband oscillations.
Fig. 3: Intensity dependence of multi-NIR-photon transitions on sideband oscillations.
Fig. 4: Attosecond coherent control of two-colour photoionization for different sidebands.
Fig. 5: Coherent control through manipulation of high-order NIR pathways.

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Data availability

Experimental data were generated at the FERMI large-scale facility. The experimental and simulations data included in this work are available on the open repository: https://zenodo.org/record/7015967#.YwQTS-xBxQJ. Additional derived data supporting the findings of this study are available from the corresponding author on reasonable request.

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Acknowledgements

We acknowledge the contribution of N. Pal in the preparation of the magnetic bottle electron spectrometer used in the experiment. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 641789 MEDEA. K.U. acknowledges support from the X-ray Free Electron Laser Utilization Research Project and the X-ray Free Electron Laser Priority Strategy Program of the Ministry of Education, Culture, Sports, Science and Technology of Japan (MEXT); from the Cooperative Research Program of ‘Network Joint Research Center for Materials and Devices: Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials’; from the bilateral project CNR-JSPS ‘Ultrafast science with XUV Free Electron Lasers’; and from the IMRAM project for the international co-operation. R.F. and J.M. thank the Swedish Research Council (VR) and the Knut and Alice Wallenberg Foundation for financial support. D.B. acknowledges support from the Swedish Research Council grant 2020-06384. Research at Louisiana State University was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, under contract no. de-sc0010431. Portions of this research were conducted with high-performance computing resources provided by Louisiana State University (http://www.hpc.lsu.edu) and Louisiana Optical Network Infrastructure (http://hpc.loni.org). P.K.M, B.M., R.S. and G.S. acknowledge financial support from the Deutsche Forschungsgemeinschaft Research Training Group DynCAM (RTG 2717), Priority Program 1840 (QUTIF) and grant 429805582 (project SA 3470/4-1). P.K.M acknowledges financial support from Wissenschaftliche Gesellschaft Freiburg im Breisgau. I.M. and G.S. acknowledge financial support from the BMBF project 05K19VF1.

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Authors and Affiliations

  1. Physikalisches Institut, Albert-Ludwigs-Universität Freiburg, Freiburg, Germany

    Praveen Kumar Maroju, Barbara Merzuk, David Busto, Ioannis Makos, Marvin Schmoll, Ronak Shah & Giuseppe Sansone

  2. Elettra-Sincrotrone Trieste, Basovizza, Trieste, Italy

    Michele Di Fraia, Oksana Plekan, Primož Rebernik Ribič, Luca Giannessi, Giovanni De Ninno, Carlo Spezzani, Giuseppe Penco, Alexander Demidovich, Miltcho Danailov, Marcello Coreno, Marco Zangrando, Alberto Simoncig, Michele Manfredda, Kevin C. Prince & Carlo Callegari

  3. Dipartimento di Fisica Politecnico, Milan, Italy

    Matteo Bonanomi

  4. Istituto di Fotonica e Nanotecnologie CNR-IFN, Milan, Italy

    Matteo Bonanomi

  5. Department of Physics, Lund University, Lund, Sweden

    David Busto, Samuel Bengtsson, Emma Rose Simpson & Johan Mauritsson

  6. INFN Laboratori Nazionali di Frascati, Frascati, Italy

    Luca Giannessi & Marcello Coreno

  7. Laboratory of Quantum Optics, University of Nova Gorica, Nova Gorica, Slovenia

    Giovanni De Ninno & Carlo Spezzani

  8. ISM-CNR, Istituto Struttura della Materia, Trieste, Italy

    Marcello Coreno

  9. Department of Physics, University of Gothenburg, Gothenburg, Sweden

    Richard J. Squibb & Raimund Feifel

  10. ELI ALPS, ELI-HU Non-Profit, Szeged, Hungary

    Tamás Csizmadia, Mathieu Dumergue & Sergei Kühn

  11. Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai, Japan

    Kiyoshi Ueda

  12. Department of Physics and Astronomy, Louisiana State University, Baton Rouge, LA, USA

    Jianxiong Li & Kenneth J. Schafer

  13. Istituto di Fotonica e Nanotecnologie, CNR, Padova, Italy

    Fabio Frassetto & Luca Poletto

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  1. Praveen Kumar Maroju
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Contributions

P.K.M., M.D.F., O.P., M.B., B.M., D.B., I.M., M.S., R.S., S.B., E.R.S., T.C., M.D., S.K., K.U., F.F., L.P., K.C.P., J.M., C.C. and G.S. contributed to data acquisition. P.R.R., L.G., G.D.N, C.S. and G.P. operated the machine and designed the three- and four-harmonic generation scheme. M.Z. and A.S. optimized the transport and focusing of the FEL pulses to the end station. M.M. analysed the spatial properties of the phase profile of the XUV beam. A.D. and M. Danailov. designed the set-up for the NIR pulse delivery. M.D.F., O.P., M.B., C.C. prepared the end station. J.L. and K.J.S. contributed with simulations. R.J.S. and R.F. constructed and operated the magnetic bottle electron spectrometer, where parts of its operation mode were conceptually devised for this experiment. P.K.M., C.C. and G.S. conceived the idea of the experiment. P.K.M. performed the data analysis. P.K.M. and G.S. performed the simulations. G.S. supervised the work and wrote the manuscript, which was discussed and agreed by all co-authors.

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Correspondence to Giuseppe Sansone.

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Nature Photonics thanks Zenghu Chang, Fernando Martín, Predrag Ranitovic and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Methods, Figs. 1–7, Tables 1 and 2, equations and experimental information.

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Maroju, P.K., Di Fraia, M., Plekan, O. et al. Attosecond coherent control of electronic wave packets in two-colour photoionization using a novel timing tool for seeded free-electron laser. Nat. Photon. 17, 200–207 (2023). https://doi.org/10.1038/s41566-022-01127-3

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