Ultrafast intraband Auger process in self-doped colloidal quantum dots

Abstract

Investigating the separate dynamics of electrons and holes has been challenging, although it is critical for the fundamental understanding of semiconducting nanomaterials. n-Type self-doped colloidal quantum dots (CQDs) with excess electrons occupying the low-lying state in the conduction band (CB) have attracted a great deal of attention because of not only their potential applications to infrared optoelectronics but also their intrinsic system that offers a platform for investigating electron dynamics without elusive contributions from holes in the valence band. Here, we show an unprecedented ultrafast intraband Auger process, electron relaxation between spin orbit coupling states, and exciton-to-ligand vibrational energy transfer process that all occur exclusively in the CB of the self-doped beta-HgS CQDs. The electron dynamics obtained by femtosecond mid infrared spectroscopy will pave the way for further understanding of the blinking phenomenon, disproportionate charging in light-emitting diodes, and hot electron dynamics in higher quantum states coupled to surface states of CQDs.