Tracing ultrafast interatomic electronic decay processes in real time and space

Abstract

Tremendous advances in laser pump-probe techniques open the door for the observation in real time of ultrafast \textit{electronic} processes. Particularly attractive is the visualization of interatomic processes where one can follow the process of energy transfer from one atom to another. The interatomic Coulombic decay (ICD) provides such a process which is abundant in nature. A multielectron wavepacket propagation method enables now to trace fully ab initio the electron dynamics of the process in real time and in space taking into account all electrons of the system and their correlations. The evolution of the electronic cloud throughout the ICD process in the rare gas cluster NeAr following Ne2s ionization is computed and analyzed. The process takes place on a femtosecond timescale, and a surprisingly strong response is found at a much shorter attosecond timescale.