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Coherent control of ultrafast extreme ultraviolet transient absorption

Nature Photonics volume 16, pages 45–51 (2022)Cite this article

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Abstract

Ultrafast extreme ultraviolet (XUV) transient absorption is the process by which atoms and molecules absorb light on a timescale faster than the lifetime of the states involved. Coherent control uses quantum coherences to manipulate quantum pathways in light–matter interactions. Here we combine the two. We show that we can control the absorption spectral lineshape, changing it from Lorentzian to Fano to inverted Lorentzian and back again. The control is achieved by creating quantum coherence in the ground electronic state of hydrogen molecules, long before the arrival of the ultrafast XUV pulse. We show that the absorption can become negative at 12 eV, which is the optical gain. These observations provide new insights into the control of spectral lineshapes and open the way for achieving lasing without inversion in the XUV spectral range.

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Fig. 1: Absorption lineshape change induced by rotational coherence.
Fig. 2: XUV transient absorption in aligned H2.
Fig. 3: Absorption lineshape of an individual rotational transition in aligned H2.
Fig. 4: XUV transient absorption in aligned D2.
Fig. 5: Optical gain in aligned D2.
Fig. 6: Calculated FID of a three-level system based on H2.

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Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

Code availability

The code used in this study is available from the corresponding authors upon reasonable request.

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Acknowledgements

We thank D. Crane and R. Kroeker for technical support. We acknowledge fruitful discussions with A. Korobenko, G. Xin, A. Stolow, M. Spanner, B. Bernhardt and V. Schuster. This research is supported by the NSERC Discovery Grant program (RGPIN-327147-2012; D.M.V.), and by the US Army Research Office through award W911NF-14-1-0383 (D.M.V.). We acknowledge support of the Joint Centre for Extreme Photonics (P.B.C. and D.M.V.), the DFG (grant no. MI 2434/1-1; Y.M.), and the start-up grant of ShanghaiTech University (P.P.).

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Authors and Affiliations

  1. Joint Attosecond Science Laboratory, National Research Council and University of Ottawa, Ottawa, Ontario, Canada

    Peng Peng, Yonghao Mi, Xiaoyan Ding, A. Yu. Naumov, P. B. Corkum & D. M. Villeneuve

  2. Department of Physics, University of Ottawa, Ottawa, Ontario, Canada

    Peng Peng, Marianna Lytova, Mathew Britton, Xiaoyan Ding, P. B. Corkum & D. M. Villeneuve

  3. School of Physical Science and Technology, ShanghaiTech University, Shanghai, China

    Peng Peng

  4. Center for Transformative Science, ShanghaiTech University, Shanghai, China

    Peng Peng

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Contributions

P.P. and D.M.V. conceived and planned the experiment. P.P., Y.M. and X.D. conducted the measurements. P.P. and D.M.V. analysed and interpreted the data. M.L. and M.B. provided the theoretical supporting calculations. A.Y.N., P.B.C. and D.M.V. supervised the project. P.P. wrote the manuscript, with inputs from all the authors.

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Correspondence to Peng Peng or D. M. Villeneuve.

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Peng, P., Mi, Y., Lytova, M. et al. Coherent control of ultrafast extreme ultraviolet transient absorption. Nat. Photon. 16, 45–51 (2022). https://doi.org/10.1038/s41566-021-00907-7

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