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High harmonic interferometry of multi-electron dynamics in molecules

Author

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  • Olga Smirnova

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
    Max-Born Institute, 2a Max-Born-Strasse, Berlin D-12489, Germany)

  • Yann Mairesse

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
    CELIA, Université Bordeaux I, UMR 5107 (CNRS, Bordeaux 1, CEA), 351 Cours de la Libération, 33405 Talence cedex, France)

  • Serguei Patchkovskii

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada)

  • Nirit Dudovich

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
    Weizmann Institute of Science)

  • David Villeneuve

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada)

  • Paul Corkum

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada)

  • Misha Yu. Ivanov

    (National Research Council of Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
    Imperial College London, South Kensington Campus)

Abstract

High harmonic emission occurs when an electron, liberated from a molecule by an incident intense laser field, gains energy from the field and recombines with the parent molecular ion. The emission provides a snapshot of the structure and dynamics of the recombining system, encoded in the amplitudes, phases and polarization of the harmonic light. Here we show with CO2 molecules that high harmonic interferometry can retrieve this structural and dynamic information: by measuring the phases and amplitudes of the harmonic emission, we reveal ‘fingerprints’ of multiple molecular orbitals participating in the process and decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Ångström spatial resolution arising from the de Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event.

Suggested Citation

  • Olga Smirnova & Yann Mairesse & Serguei Patchkovskii & Nirit Dudovich & David Villeneuve & Paul Corkum & Misha Yu. Ivanov, 2009. "High harmonic interferometry of multi-electron dynamics in molecules," Nature, Nature, vol. 460(7258), pages 972-977, August.
    • Handle: RePEc:nat:nature:v:460:y:2009:i:7258:d:10.1038_nature08253
    DOI: 10.1038/nature08253
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    Cited by:

    1. Álvaro Jiménez-Galán & Chandler Bossaer & Guilmot Ernotte & Andrew M. Parks & Rui E. F. Silva & David M. Villeneuve & André Staudte & Thomas Brabec & Adina Luican-Mayer & Giulio Vampa, 2023. "Orbital perspective on high-harmonic generation from solids," Nature Communications, Nature, vol. 14(1), pages 1-6, December.
    2. Peipei Ge & Yankun Dou & Meng Han & Yiqi Fang & Yongkai Deng & Chengyin Wu & Qihuang Gong & Yunquan Liu, 2024. "Spatiotemporal imaging and shaping of electron wave functions using novel attoclock interferometry," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Lixin He & Siqi Sun & Pengfei Lan & Yanqing He & Bincheng Wang & Pu Wang & Xiaosong Zhu & Liang Li & Wei Cao & Peixiang Lu & C. D. Lin, 2022. "Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Li Wang & Guangru Bai & Xiaowei Wang & Jing Zhao & Cheng Gao & Jiacan Wang & Fan Xiao & Wenkai Tao & Pan Song & Qianyu Qiu & Jinlei Liu & Zengxiu Zhao, 2024. "Raman time-delay in attosecond transient absorption of strong-field created krypton vacancy," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    5. Pengcheng Chen & Dingxin Fan & Annabella Selloni & Emily A. Carter & Craig B. Arnold & Yunlong Zhang & Adam S. Gross & James R. Chelikowsky & Nan Yao, 2023. "Observation of electron orbital signatures of single atoms within metal-phthalocyanines using atomic force microscopy," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    6. Hongbin Lei & Jinping Yao & Jing Zhao & Hongqiang Xie & Fangbo Zhang & He Zhang & Ning Zhang & Guihua Li & Qian Zhang & Xiaowei Wang & Yan Yang & Luqi Yuan & Ya Cheng & Zengxiu Zhao, 2022. "Ultraviolet supercontinuum generation driven by ionic coherence in a strong laser field," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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