A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids
Sargent, Edward H.
KAUST Grant NumberKUS-11-009-21
Online Publication Date2012-09-07
Print Publication Date2012-09-25
Permanent link to this recordhttp://hdl.handle.net/10754/597229
MetadataShow full item record
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.
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.
SponsorsThis 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.
PublisherAmerican Chemical Society (ACS)
CollectionsPublications Acknowledging KAUST Support
- Measuring charge carrier diffusion in coupled colloidal quantum dot solids.
- Authors: Zhitomirsky D, Voznyy O, Hoogland S, Sargent EH
- Issue date: 2013 Jun 25
- Joint mapping of mobility and trap density in colloidal quantum dot solids.
- Authors: Stadler P, Sutherland BR, Ren Y, Ning Z, Simchi A, Thon SM, Hoogland S, Sargent EH
- Issue date: 2013 Jul 23
- Role of bond adaptability in the passivation of colloidal quantum dot solids.
- Authors: Thon SM, Ip AH, Voznyy O, Levina L, Kemp KW, Carey GH, Masala S, Sargent EH
- Issue date: 2013 Sep 24
- Depleted-heterojunction colloidal quantum dot solar cells.
- Authors: Pattantyus-Abraham AG, Kramer IJ, Barkhouse AR, Wang X, Konstantatos G, Debnath R, Levina L, Raabe I, Nazeeruddin MK, Grätzel M, Sargent EH
- Issue date: 2010 Jun 22
- Hybrid passivated colloidal quantum dot solids.
- Authors: Ip AH, Thon SM, Hoogland S, Voznyy O, Zhitomirsky D, Debnath R, Levina L, Rollny LR, Carey GH, Fischer A, Kemp KW, Kramer IJ, Ning Z, Labelle AJ, Chou KW, Amassian A, Sargent EH
- Issue date: 2012 Sep