Single-shot molecular orbital tomography with orthogonal two-color fields.

Molecular orbital tomography (MOT) based on high-order-harmonic generation opens a way to track the molecular electron dynamics or even follow a chemical reaction. However, the real-time imaging of the evolution of electron orbitals is hampered by the multi-shot measurement of high-order harmonics. Here, we report a single-shot MOT scheme with orthogonal two-color (OTC) fields. This scheme enables the tomographic imaging of molecular orbital with single-shot measurement in experiment, owing to the two-dimensional manipulation of the electron motion in OTC fields. Our work paves the way towards tracking the molecular electron dynamics with combined attosecond temporal and sub-Ångström spatial resolutions.