ACS Nano, volume 6, issue 9, pages 8448-8455

A charge-orbital balance picture of doping in colloidal quantum dot solids.

Publication typeJournal Article
Publication date2012-09-07
Journal: ACS Nano
scimago Q1
SJR4.593
CiteScore26.0
Impact factor15.8
ISSN19360851, 1936086X
PubMed ID:  22928602
General Physics and Astronomy
General Materials Science
General Engineering
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.
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