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Ultrafast formation dynamics of D3+ from the light-driven bimolecular reaction of the D2–D2 dimer

Nature Chemistry volume 15, pages 1229–1235 (2023)Cite this article

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Abstract

The light-driven formation of trihydrogen cation has been attracting considerable attention because of its important role as an initiator of chemical reactions in interstellar clouds. To understand the formation dynamics, most previous studies focused on creating H3+ or D3+ from unimolecular reactions of various organic molecules. Here we observe and characterize the ultrafast formation dynamics of D3+ from a bimolecular reaction, using pump–probe experiments that employ ultrashort laser pulses to probe its formation from a D2–D2 dimer. Our molecular dynamics simulations provide an intuitive representation of the reaction dynamics, which agree well with the experimental observation. We also show that the emission direction of D3+ can be controlled using a tailored two-colour femtosecond laser field. The underlying control mechanism is in line with what is known from the light control of electron localization in the bond breaking of single molecules.

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Fig. 1: Schematic of the experiments.
Fig. 2: Results of single-colour pump–probe experiments.
Fig. 3: Potential energy surface of the T-type cationic (D2–D2)+ dimer.
Fig. 4: Molecular dynamics simulation results.
Fig. 5: Asymmetric emission of D3+ and D+ in the (D3+, D+) channel.

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Data availability

The data that support the plots within this article are available from the Zenodo database at https://doi.org/10.5281/zenodo.7807812.

Code availability

The code that supports the plots within this article is available from the corresponding authors upon reasonable request.

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Acknowledgements

This work was supported by the National Key R&D Program of China (grant number 2018YFA0306303 to J. Wu), National Natural Science Fund (grants numbers 11834004, 12241407 and 12227807 to J. Wu, 12174109 to P.L., 92050105 to K.L., 92150105 to H.N. and 22173017 to J. Wen) and Science and Technology Commission of Shanghai Municipality (20JC1414900 to M.Z. and 21ZR1420100 to H.N.). K.L. acknowledges support from the Alexander Von Humboldt Foundation. R.D. acknowledges support from the Deutsche Forschungsgemeinschaft.

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Authors and Affiliations

  1. State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, China

    Lianrong Zhou, Hongcheng Ni, Zhejun Jiang, Junjie Qiang, Wenyu Jiang, Wenbin Zhang, Peifen Lu & Jian Wu

  2. Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, China

    Hongcheng Ni & Jian Wu

  3. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, China

    Jin Wen & Meifang Zhu

  4. Institut für Kernphysik, Goethe-Universität Frankfurt am Main, Frankfurt, Germany

    Kang Lin & Reinhard Dörner

  5. Chongqing Key Laboratory of Precision Optics, Chongqing Institute of East China Normal University, Chongqing, China

    Jian Wu

  6. CAS Center for Excellence in Ultra-intense Laser Science, Shanghai, China

    Jian Wu

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  1. Lianrong Zhou
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Contributions

L.Z., Z.J., J.Q., W.J., P.L., K.L. and J. Wu contributed to the experiments. H.N., J. Wen and M.Z. performed the simulation. L.Z., Z.J., W.Z., P.L., K.L., R.D. and J. Wu analysed the data. All authors contributed to writing the manuscript. K.L. and J. Wu supervised the project.

Corresponding authors

Correspondence to Jin Wen, Kang Lin or Jian Wu.

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Nature Chemistry thanks Marcos Dantus and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Video 1

Molecular dynamics: structural evolution of the T shape (D2–D2)+ to form (D3+, D).

Supplementary Video 2

Molecular dynamics: structural evolution of the L shape (D2–D2)+ to form (D3+, D).

Supplementary Video 3

Molecular dynamics: structural evolution of the H shape (D2–D2)+ to form (D3+, D).

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Zhou, L., Ni, H., Jiang, Z. et al. Ultrafast formation dynamics of D3+ from the light-driven bimolecular reaction of the D2–D2 dimer. Nat. Chem. 15, 1229–1235 (2023). https://doi.org/10.1038/s41557-023-01230-0

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