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Ultrafast dynamics of correlation bands following XUV molecular photoionization

Abstract

Modern ultrashort X-ray/XUV (extreme ultraviolet) sources provide unique opportunities to investigate the primary reactions of matter upon energetic excitation. Understanding these processes in molecules on ultrafast timescales is required to improve bespoke high-energy radiation detectors, nanomedicine schemes or to study the molecular composition of interstellar media. However, current experiments struggle to provide a general framework because of the uniqueness and complexity of each system. Here we show the universal role of correlation bands—features created by electron correlation. This is done by studying ultrafast energy relaxation of size-scalable two-dimensional molecules following ionization by an ultrashort XUV pulse. We observed long lifetimes that nonlinearly increase with the number of valence electrons. A general law based on solid-like electron–phonon scattering is proposed, which explains both our results and previously reported measurements. This offers new opportunities in attosecond science and high-energy photophysics.

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Fig. 1: Dynamics in correlation bands.
Fig. 2: Scaling law in the relaxation of CBs for 2D and 3D structures.
Fig. 3: Analogy between CBs and solid-like band structures.

Data availability

Data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.

Code availability

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

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Acknowledgements

We thank C. Dujardin and L.S. Cederbaum for fruitful discussions. We acknowledge financial support from CNRS, ANR Circé (ANR-16-CE30-0012). V.D. acknowledges financial support from the DFG through the QUTIF priority programme. A.I.K. thanks US ARO for financial support under grant no. W911NF-14-1-0383. Studies of interstellar PAHs at Leiden Observatory are supported through a grant by the Netherlands Organisation for Scientific Research (NWO) as part of the Dutch Astrochemistry Network and through the Spinozapremie.

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Contributions

M.H., A.G.G.M.T. and F.L. conceived the project. M.H., P.C.N., V.L., A.B., A.S., G.K., R.B., E.C. and F.L. conducted the experiments. M.H., V.L. and A.B. performed the data analysis. M.H., V.D., A.I.K. and F.L. conceived the theoretical model. V.D. and A.I.K. performed the calculations. M.H. and F.L. wrote the manuscript, with inputs from all the authors. F.L. led the project.

Corresponding author

Correspondence to F. Lépine.

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The authors declare no competing interests.

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Peer review information Nature Physics thanks Laura Cattaneo, Mette Gaarde and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–10, Discussion and Table 1.

Source data

Source Data Fig. 1

Source data of Fig. 1b (raw data, fit, cross-correlation) and of Fig. 1c.

Source Data Fig. 2

Source data of Fig. 2a–j, including fits in Fig. 2j.

Source Data Fig. 3

Source data of Fig. 3a–c (raw ADC data and extracted DOS).

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Hervé, M., Despré, V., Castellanos Nash, P. et al. Ultrafast dynamics of correlation bands following XUV molecular photoionization. Nat. Phys. 17, 327–331 (2021). https://doi.org/10.1038/s41567-020-01073-3

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