Time-Domain ab Initio Study of Auger and Phonon-Assisted Auger Processes in a Semiconductor Quantum Dot

We developed time-domain ab initio simulation of Auger, phenomena, including multiple exciton generation (MEG) and recombination (MER). It is the first approach,. describing phonon assisted processes and early dynamics. MEG starts below the electronic threshold, strongly accelerating with energy. Ligands are particularly important to phonon assisted MEG, which therefore can be probed with infrared spectroscopy. Short-time Gaussian component gives 5-10% of MEG, justifying rate theories that assume exponential dynamics. MER is preceded by electron-phonon relaxation to low energies.