Nano-engineered electron-hole exchange interaction controls exciton dynamics in core-shell semiconductor nanocrystals

Nat Commun. 2011:2:280. doi: 10.1038/ncomms1281.

Abstract

A strong electron-hole exchange interaction (EI) in semiconductor nanocrystals (NCs) gives rise to a large (up to tens of meV) splitting between optically active ('bright') and optically passive ('dark') excitons. This dark-bright splitting has a significant effect on the optical properties of band-edge excitons and leads to a pronounced temperature and magnetic field dependence of radiative decay. Here we demonstrate a nanoengineering-based approach that provides control over EI while maintaining nearly constant emission energy. We show that the dark-bright splitting can be widely tuned by controlling the electron-hole spatial overlap in core-shell CdSe/CdS NCs with a variable shell width. In thick-shell samples, the EI energy reduces to <250 μeV, which yields a material that emits with a nearly constant rate over temperatures from 1.5 to 300 K and magnetic fields up to 7 T. The EI-manipulation strategies demonstrated here are general and can be applied to other nanostructures with variable electron-hole overlap.

Publication types

  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Cadmium Compounds / chemistry
  • Chemical Engineering / methods
  • Electromagnetic Fields
  • Electrons*
  • Fluorescence
  • Microscopy, Electron, Transmission
  • Models, Theoretical*
  • Nanoparticles / chemistry*
  • Nanotechnology / methods*
  • Quantum Dots*
  • Selenium Compounds / chemistry
  • Sulfides / chemistry
  • Temperature

Substances

  • Cadmium Compounds
  • Selenium Compounds
  • Sulfides
  • cadmium sulfide
  • cadmium selenide