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Attosecond imaging of molecular electronic wavepackets

Abstract

A strong laser field may tunnel ionize a molecule from several orbitals simultaneously, forming an attosecond electron–hole wavepacket. Both temporal and spatial information on this wavepacket can be obtained through the coherent soft X-ray emission resulting from the laser-driven recollision of the liberated electron with the core. By characterizing the emission from aligned N2 molecules, we demonstrate the attosecond contributions of the two highest occupied molecular orbitals. We determine conditions where they are disentangled in the real and imaginary parts of the emission dipole moment. This allows us to carry out a tomographic reconstruction of both orbitals with angstrom spatial resolution. Their coherent superposition provides experimental images of the attosecond wavepacket created in the ionization process. Our results open the prospect of imaging ultrafast intramolecular dynamics combining attosecond and angstrom resolutions.

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Figure 1: Attosecond emission of aligned N2 molecules.
Figure 2: Experimental recombination dipole for N2 molecules.
Figure 3: Phase of the harmonic emission.
Figure 4: Orbital tomographic reconstructions.
Figure 5: Reconstructions of the dynamic hole.

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Acknowledgements

We thank O. Smirnova, M. Ivanov and Y. Mairesse for fruitful discussions. Financial support from the LASERLAB2 programme and from the ANR-09-BLAN-0031-01 ATTO-WAVE is acknowledged. Parts of the computations have been carried out at the Institut du Développement et des Ressources en Informatique Scientifique IDRIS.

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Contributions

P.S. with B.C. planned the project. W.B., P.B., B.C. and P.S. designed and installed the experiment. S.H. with assistance from W.B., P.B. and P.S. carried out the measurements. S.H. and J.C. with assistance from W.B.,T.R., Z.D. and P.S. analysed the data. J.C., C.G.-T., T.A., A.M. and R.T. carried out the calculations. All authors discussed the results and contributed to the final manuscript.

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Correspondence to P. Salières.

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Haessler, S., Caillat, J., Boutu, W. et al. Attosecond imaging of molecular electronic wavepackets. Nature Phys 6, 200–206 (2010). https://doi.org/10.1038/nphys1511

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