A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids
Type
ArticleAuthors
Voznyy, Oleksandr
Zhitomirsky, David
Stadler, Philipp
Ning, Zhijun
Hoogland, Sjoerd
Sargent, Edward H.

KAUST Grant Number
KUS-11-009-21Date
2012-09-07Online Publication Date
2012-09-07Print Publication Date
2012-09-25Permanent link to this record
http://hdl.handle.net/10754/597229
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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.Citation
Voznyy O, Zhitomirsky D, Stadler P, Ning Z, Hoogland S, et al. (2012) A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids. ACS Nano 6: 8448–8455. Available: http://dx.doi.org/10.1021/nn303364d.Sponsors
This publication is based in part on work supported by Award KUS-11-009-21, made by King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, and by the Natural Sciences and Engineering Research Council (NSERC) of Canada. David Zhitomirsky would like to acknowledge his NSERC CGS D scholarship. We thank Angstrom Engineering, Inc. and Innovative Technology, Inc. for useful discussions regarding material deposition methods and control of the glovebox environment, respectively. We thank Lyudmila Goncharova for help in RBS measurements and Mark Greiner for help in XPS measurements. We thank Larissa Levina for PbS COD synthesis and Melissa Furukawa for FET measurements. Computations were performed on the GPC supercomputer at the SciNet<SUP>49</SUP> HPC Consortium. SciNet is funded by the Canada Foundation for Innovation under the auspices of Compute Canada, the Government of Ontario, Ontario Research Fund-Research Excellence, and the University of Toronto.Publisher
American Chemical Society (ACS)Journal
ACS NanoPubMed ID
22928602ae974a485f413a2113503eed53cd6c53
10.1021/nn303364d
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