Illuminating Molecular Symmetries with Bicircular High-Order-Harmonic Generation

Daniel M. Reich and Lars Bojer Madsen
Phys. Rev. Lett. 117, 133902 – Published 22 September 2016
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Abstract

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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  • Received 1 July 2016

DOI:https://doi.org/10.1103/PhysRevLett.117.133902

© 2016 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Daniel M. Reich and Lars Bojer Madsen

  • Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark

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Issue

Vol. 117, Iss. 13 — 23 September 2016

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