4.8 Article

Illuminating Molecular Symmetries with Bicircular High-Order-Harmonic Generation

Journal

PHYSICAL REVIEW LETTERS
Volume 117, Issue 13, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.117.133902

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Funding

  1. European Research Council StG [277767-TDMET]
  2. VKR center of excellence QUSCOPE
  3. Alexander von Humboldt Foundation through the Feodor Lynen Program
  4. Villum Fonden [00007335] Funding Source: researchfish

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We present a general theory of bicircular high-order-harmonic generation from N-fold rotationally symmetric molecules. Using a rotating frame of reference we predict the complete structure of the high-order-harmonic spectra for arbitrary driving frequency ratios and show how molecular symmetries can be directly identified from the harmonic signal. Our findings reveal that a characteristic fingerprint of rotational molecular symmetries can be universally observed in the ultrafast response of molecules to strong bicircular fields.

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