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

Handle URI:
http://hdl.handle.net/10754/597229
Title:
A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids
Authors:
Voznyy, Oleksandr; Zhitomirsky, David; Stadler, Philipp; Ning, Zhijun; Hoogland, Sjoerd; Sargent, Edward H.
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.
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.
Publisher:
American Chemical Society (ACS)
Journal:
ACS Nano
KAUST Grant Number:
KUS-11-009-21
Issue Date:
25-Sep-2012
DOI:
10.1021/nn303364d
PubMed ID:
22928602
Type:
Article
ISSN:
1936-0851; 1936-086X
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.
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Full metadata record

DC FieldValue Language
dc.contributor.authorVoznyy, Oleksandren
dc.contributor.authorZhitomirsky, Daviden
dc.contributor.authorStadler, Philippen
dc.contributor.authorNing, Zhijunen
dc.contributor.authorHoogland, Sjoerden
dc.contributor.authorSargent, Edward H.en
dc.date.accessioned2016-02-25T12:28:28Zen
dc.date.available2016-02-25T12:28:28Zen
dc.date.issued2012-09-25en
dc.identifier.citationVoznyy 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.en
dc.identifier.issn1936-0851en
dc.identifier.issn1936-086Xen
dc.identifier.pmid22928602en
dc.identifier.doi10.1021/nn303364den
dc.identifier.urihttp://hdl.handle.net/10754/597229en
dc.description.abstractWe 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.en
dc.description.sponsorshipThis 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.en
dc.publisherAmerican Chemical Society (ACS)en
dc.subjectcolloidal quantum dotsen
dc.subjectDFTen
dc.subjectdopingen
dc.subjectFETen
dc.subjectPbS nanocrystalsen
dc.subjectRBSen
dc.titleA Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solidsen
dc.typeArticleen
dc.identifier.journalACS Nanoen
dc.contributor.institutionUniversity of Toronto, Toronto, Canadaen
kaust.grant.numberKUS-11-009-21en

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