A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids

Oleksandr Voznyy, David Zhitomirsky, Philipp Stadler, Zhijun Ning, Sjoerd Hoogland, Edward H. Sargent

Research output: Contribution to journalArticlepeer-review

158 Scopus citations

Abstract

We present a framework-validated using both modeling and experiment-to predict doping in CQD films. In the ionic semiconductors widely deployed in CQD films, the framework reduces to a simple accounting of the contributions of the oxidation state of each constituent, including both inorganic species and organic ligands. We use density functional theory simulations to confirm that the type of doping can be reliably predicted based on the overall stoichiometry of the CQDs, largely independent of microscopic geometrical bonding configurations. Studies employing field-effect transistors constructed from CQDs that have undergone various chemical treatments, coupled with Rutherford backscattering and X-ray photoelectron spectroscopy to provide compositional analysis, allow us to test and confirm the proposed model in an experimental framework. We investigate both p- and n-type electronic doping spanning a wide range of carrier concentrations from 10 16 cm -3 to over 10 18 cm -3, and demonstrate reversible switching between p- and n-type doping by changing the CQD stoichiometry. We show that the summation of the contributions from all cations and anions within the film can be used to predict accurately the majority carrier type. The findings enable predictable control over majority carrier concentration via tuning of the overall stoichiometry. © 2012 American Chemical Society.
Original languageEnglish (US)
Pages (from-to)8448-8455
Number of pages8
JournalACS Nano
Volume6
Issue number9
DOIs
StatePublished - Sep 7 2012
Externally publishedYes

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