Ultrafast X-ray photoelectron diffraction in triatomic molecules by circularly polarized attosecond light pulses

Abstract

We theoretically study ultrafast photoelectron diffraction in triatomic molecules with cyclic geometry by ultrafast circular soft X-ray attosecond pulses. Molecular frame photoelectron distributions show complex diffraction patterns, arising from molecular multiple center interference and circular charge migration. It is found that photoelectron diffraction patterns depend on the initial electronic state, encoding the information of molecular orbital symmetries. In a resonant coherent electron excitation process, time-resolved photoelectron diffraction patterns enables us to reconstruct the charge migration with highly spatiotemporal resolutions. We simulate and analyze the results from ab initio calculations of the single electron triangular hydrogen molecular ion H₃²⁺ which is used as a benchmark molecular system in combination with an ultrafast multi-center and multi-state photoionization model. This approach presents a general scheme which can be applied to explore circular charge migration from electron orbits and attosecond coherent electron dynamics in polyatomic systems by circular ultrafast laser pulses.