Multiexciton spectroscopy of semiconductor nanocrystals under quasi-continuous-wave optical pumping

Abstract

We present a method for performing multiexciton spectroscopy in colloidal semiconductor nanocrystals. In this regime multiexcitonic states are generated sequentially via a “ladder-climbing” mechanism. The distribution of multiexcitonic states, determined by a steady-state rate equation, adiabatically follows the illumination intensity, allowing for “slow” detection of multiexcitonic spectra. Emission spectra of multiexcitonic states with a small number of excitons are obtained without passing through states with a large number of excitons. This is in contrast with impulsive excitation schemes utilizing picosecond pulses, where in order to significantly populate a given multiexcitonic state, many of the dots necessarily pass through states with a larger number of excitons due to the Poissonian distribution of the number of absorbed photons. In particular, we observe directly the order of appearance of the various multiexcitonic peaks. This enables us to determine the threshold conditions for Auger ionization, shedding more light on the nature of this process. We are also able to observe the short-lived excitations at higher energies than triexcitons in CdSe quantum dots. Finally, we demonstrate bi- and triexcitonic optical gain in a close-packed film under quasi-continuous-wave pumping.