Control of Exciton Spin Relaxation by Electron−Hole Decoupling in Type-II Nanocrystal Heterostructures

Abstract

The electron spin flip relaxation dynamics in type II CdSe/CdTe nanorod heterostructures are investigated by an ultrafast polarization transient grating technique. Photoexcited charge separation in the heterostructures suppresses the electron−hole exchange interaction and their recombination, which reduces the electron spin relaxation rate in CdSe nanocrystals by 1 order of magnitude compared to exciton relaxation. The electron orientation is preserved during charge transfer from CdTe to CdSe, and its relaxation time constant is found to be ∼5 ps at 293 K in the CdSe part of these nanorods. This finding suggests that hole spin relaxation determines the exciton fine structure relaxation rate and therefore control of exciton spin relaxation in semiconductor nanostructures is possible by delocalizing or translating the hole density relative to the electron.