Two-photon photoemission study of competing Auger and surface-mediated relaxation of hot electrons in CdSe quantum dot solids

Nano Lett. 2013 Apr 10;13(4):1655-61. doi: 10.1021/nl400113t. Epub 2013 Mar 22.

Abstract

Solids composed of colloidal quantum dots hold promise for third generation highly efficient thin-film photovoltaic cells. The presence of well-separated conduction electron states opens the possibility for an energy-selective collection of hot and equilibrated carriers, pushing the efficiency above the one-band gap limit. However, in order to reach this goal the decay of hot carriers within a band must be better understood and prevented, eventually. Here, we present a two-photon photoemission study of the 1Pe→1Se intraband relaxation dynamics in a CdSe quantum dot solid that mimics the active layer in a photovoltaic cell. We observe fast hot electron relaxation from the 1Pe to the 1Se state on a femtosecond-scale by Auger-type energy donation to the hole. However, if the oleic acid capping is exchanged for hexanedithiol capping, fast deep hole trapping competes efficiently with this relaxation pathway, blocking the Auger-type electron-hole energy exchange. A slower decay becomes then visible; we provide evidence that this is a multistep process involving the surface.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cadmium Compounds / chemistry*
  • Electrons
  • Hot Temperature
  • Nanotechnology*
  • Photoelectron Spectroscopy
  • Photons
  • Quantum Dots / chemistry*
  • Selenium Compounds / chemistry*
  • Surface Properties

Substances

  • Cadmium Compounds
  • Selenium Compounds
  • cadmium selenide