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Linked attosecond phase interferometry for molecular frame measurements

Nature Physics volume 9, pages 174–178 (2013)Cite this article

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Abstract

High-harmonic spectroscopy uses attosecond techniques to measure single-atom or molecule photorecombination cross-sections. Whereas the amplitude of the extreme-ultraviolet light is easily measurable, the phase is more challenging to access. However, the phase contains information necessary for tomographic imaging of the molecular orbital wavefunction with attosecond–ångström resolution. Present techniques cannot simultaneously measure the phase as a function of molecular angle and photon frequency, which is necessary for a full reconstruction of the wavefunction. We overcome this limitation with an all-optical method that does not require any ad hoc assumptions about the phase. We apply it to record the full phase map of aligned bromine molecules relative to reference xenon atoms. It allows us to resolve, both spectrally and angularly, the participation of multiple molecular orbitals, and infer a phase of ionization. This method opens a path to time-resolved molecular orbital tomography.

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Figure 1: In aligned molecules, the high-harmonic spectral phase ϕMol(q,θ) is a function of both harmonic order q and molecular alignment angle θ with respect to the driving laser field polarization axis (linear).
Figure 2: Spectral harmonic phase interferometry of aligned Br2 molecules.
Figure 3: Mixed-gases interferometry results.
Figure 4: Experimentally determined relative phase ΔϕMix(q,θ) between the molecule and reference atom.
Figure 5: Experimentally determined molecular frame amplitude and phase compared with model calculations.

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Acknowledgements

The authors gratefully acknowledge financial support from NSERC, CIPI, AFOSR and the NRC-CEA agreement.

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Authors and Affiliations

  1. Joint Attosecond Science Laboratory, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa K1A 0R6, Canada

    J. B. Bertrand, D. M. Villeneuve & P. B. Corkum

  2. Laboratorium für physikalische Chemie, ETH Zürich, Wolfgang-Pauli-Strasse 10, 8093 Zürich, Switzerland

    H. J. Wörner

  3. CEA-Saclay, DSM, Service des Photons, Atomes et Molécules, 91191 Gif sur Yvette, France

    P. Salières

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  1. J. B. Bertrand
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Contributions

J.B.B., H.J.W., P.S., D.M.V. and P.B.C. conceived the experiment and helped prepare the manuscript. J.B.B. and H.J.W. performed all experiments. J.B.B. and D.M.V. developed the LAPIN algorithm. J.B.B. did all data analysis and calculations, prepared all figures and led the writing of the manuscript.

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Correspondence to D. M. Villeneuve.

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Bertrand, J., Wörner, H., Salières, P. et al. Linked attosecond phase interferometry for molecular frame measurements. Nature Phys 9, 174–178 (2013). https://doi.org/10.1038/nphys2540

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