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Generalized molecular orbital tomography

Nature Physics volume 7, pages 822–826 (2011)Cite this article

Abstract

The emission of coherent XUV radiation from atomic or molecular gases exposed to intense infrared laser pulses, known as high harmonic generation, is of paramount interest in atomic and molecular physics as well as in attosecond science. The emitted radiation contains a wealth of information about the structure of its generating medium, which inspired vigorous efforts to tomographically image the valence orbital of atoms and molecules. The orbital retrieval is nevertheless seriously hindered by the complexity of the harmonic emission process, as recently demonstrated by several theoretical and experimental works. Here we present a novel approach for molecular orbital tomography that contributes to overcome those difficulties, opening intriguing perspectives on coherent XUV imaging of complex species by high-order harmonic generation.

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Figure 1: High-order harmonic spectra measured in CO2 molecules as a function of the delay between the aligning and generating pulses.
Figure 2: Single-molecule contribution to high-order harmonic generation in CO2, retrieved with a self-referencing approach.
Figure 3: High-order harmonic spectra measured in aligned CO2 molecules for different pulse intensities and wavelengths.
Figure 4: HOMO reconstruction in CO2.

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Acknowledgements

We acknowledge the partial financial support from the Cariplo Foundation through the project 2009-2562 and from the European Union within the contract n. 228334 JRA-ALADIN (Laserlab Europe II). We gratefully acknowledge the contributions of F. Frassetto, L. Poletto and P. Villoresi in the development of the XUV spectrometer. We thank C. Altucci, P. Corkum, P. Hockett, M. Ivanov, J. Marangos, A. Staudte, C. Smeenk, R. Torres, R. Velotta and D. Villeneuve for useful discussions.

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Authors and Affiliations

  1. Istituto di Fotonica e Nanotecnologie—CNR, Milan 20133, Italy

    C. Vozzi

  2. Dipartimento di Fisica, Politecnico di Milano, Milan 20133, Italy

    M. Negro, F. Calegari, G. Sansone, M. Nisoli, S. De Silvestri & S. Stagira

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  1. C. Vozzi
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  3. F. Calegari
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Contributions

S.S. and C.V. planned the experiment. F.C., M. Negro, S.S. and C.V. designed and realized the experimental set-up. S.D.S., M. Nisoli and G.S. contributed to the development of the experimental set-up. M. Negro and C.V. carried out the measurements and analysed the data. S.S. developed the algorithms for the self-referenced HOMO reconstruction and performed the numerical simulations. All the authors discussed the results and contributed to the final manuscript.

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Correspondence to S. Stagira.

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The authors declare no competing financial interests.

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Vozzi, C., Negro, M., Calegari, F. et al. Generalized molecular orbital tomography. Nature Phys 7, 822–826 (2011). https://doi.org/10.1038/nphys2029

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