Wavepacket golden rule treatment of interparticle Coulombic decay in paired quantum dots.

Abstract

The interparticle Coulombic decay process in paired quantum dots is studied by electron dynamics calculations. We consider a pair of Coulomb-coupled one-electron charged gallium arsenide quantum dots embedded in a nanowire. The two-electron decay process is approximately described by a single active electron model. Within this model, we employ the time-dependent wavepacket approach to the Fermi golden rule (introduced in the context of vibrational predissociation) to calculate autoionization rates, which are compared to exact rates obtained from fully correlated two-electron dynamics calculations. We found that the approximate decay rates agree well with the exact results in the limit of sufficiently separated quantum dots. Finally, we explore whether the short-range behavior of the new model can be further enhanced by the inclusion of local exchange effects by means of regularization of the Coulomb-potential based on a Jastrow-Slater wavefunction. The proposed method may open a route to study the interparticle Coulombic decay in more intricate systems, e.g., paired metal-nanoparticle-quantum dot systems.