Asymmetric Attosecond Photoionization in Molecular Shape Resonance

Abstract

A shape resonance emerges during the light absorption in many molecules with a gigantic burst amplitude and a lifetime of hundreds of attoseconds. Recent advances in attosecond metrology revealed the attosecond lifetime of the shape resonance. For a heteronuclear molecule, the asymmetric initial state and landscape of the molecular potential would lead to an asymmetric shape resonance, whose effect, however, has not been characterized yet. Here, we employ an attosecond interferometer to investigate the molecular-frame photoionization time delay in the vicinity of the shape resonance of the NO molecule. Driven by photons with energy ranging from 23.8 eV to 36.5 eV, a 150 attosecond difference in the time delay is observed between photoemission from the N/O end. Our quantum scattering theoretical simulations reproduce well our experimental findings. It illustrates that the asymmetric time delay originates from the interference between resonant and nonresonant photoionization pathways.