Probing Attosecond Electron Coherence in Molecular Charge Migration by Ultrafast X-Ray Photoelectron Imaging

Electron coherence is a fundamental quantum phenomenon in today’s ultrafast physics and chemistry research. Based on attosecond pump–probe schemes, ultrafast X-ray photoelectron imaging of molecules was used to monitor the coherent electron dynamics which is created by an XUV pulse. We performed simulations on the molecular ion H 2 + by numerically solving time-dependent Schrödinger equations. It was found that the X-ray photoelectron angular and momentum distributions depend on the time delay between the XUV pump and soft X-ray probe pulses. Varying the polarization and helicity of the soft X-ray probe pulse gave rise to a modulation of the time-resolved photoelectron distributions. The present results provide a new approach for exploring ultrafast coherent electron dynamics and charge migration in reactions of molecules on the attosecond time scale.