Illuminating Molecular Symmetries with Bicircular High-Order-Harmonic Generation

Abstract

We present a complete theory of bicircular high-order-harmonic emission 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.