Biexciton Dynamics in Alloy Quantum Dots

Abstract

The biexciton Auger dynamics of alloyed Zn1–xCdxSe/ZnS and Zn1–xCdxSe/CdS core/shell nanoparticles are examined. A series of particles with increasing cadmium mole fractions are prepared by synthesizing ZnSe nanocrystals followed by cation exchange with cadmium oleate. This is followed by the low-temperature deposition of a CdS or ZnS shell to passivate surface traps. The percent composition of cadmium in the core particles is determined from the absorption spectrum upon cation exchange, and the excited-state dynamics are measured using power-dependent transient absorption spectroscopy. The biexciton lifetimes are controlled by Auger processes, and the results show that Auger recombination is faster for alloys than for either pure ZnSe or pure CdSe. The lifetimes go through a minimum at a composition that is approximately 10–40% cadmium. This behavior is assigned to partial hole localization at clusters of cadmium atoms in the alloy, which increases Auger rates through the same mechanism that is responsib...