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Title:
Microscopic Theory of Cation Exchange in CdSe Nanocrystals
Authors:
Ott, Florian D.; Spiegel, Leo L.; Norris, David J.; Erwin, Steven C.
Affiliation:
AA(Optical Materials Engineering Laboratory, ETH Zurich, 8092 Zurich, Switzerland), AB(Optical Materials Engineering Laboratory, ETH Zurich, 8092 Zurich, Switzerland), AC(Optical Materials Engineering Laboratory, ETH Zurich, 8092 Zurich, Switzerland), AD(Center for Computational Materials Science, Naval Research Laboratory, Washington, D.C. 20375, USA)
Publication:
Physical Review Letters, Volume 113, Issue 15, id.156803 (PhRvL Homepage)
Publication Date:
10/2014
Origin:
APS
PACS Keywords:
Electronic structure of nanoscale materials: clusters nanoparticles nanotubes and nanocrystals, Defects and impurities in crystals, microstructure, Quantum dots
Abstract Copyright:
(c) 2014: American Physical Society
DOI:
10.1103/PhysRevLett.113.156803
Bibliographic Code:
2014PhRvL.113o6803O

Abstract

Although poorly understood, cation-exchange reactions are increasingly used to dope or transform colloidal semiconductor nanocrystals (quantum dots). We use density-functional theory and kinetic Monte Carlo simulations to develop a microscopic theory that explains structural, optical, and electronic changes observed experimentally in Ag-cation-exchanged CdSe nanocrystals. We find that Coulomb interactions, both between ionized impurities and with the polarized nanocrystal surface, play a key role in cation exchange. Our theory also resolves several experimental puzzles related to photoluminescence and electrical behavior in CdSe nanocrystals doped with Ag.
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