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Aliovalent Doping in Colloidal Quantum Dots and Its Manifestation on Their Optical Properties: Surface Attachment versus Structural Incorporation

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ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels (Barcelona), Spain
Department of Physics and Astronomy, University of Bologna, Bologna, Italy
§ Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche, c/o ESRF, Grenoble, France
Laboratorio de Microscopías Avanzadas (LMA), Instituto de Nanociencia de Aragon (INA)—ARAID and Departamento de Fisica de la Materia Condensada, Universidad de Zaragoza, 50018 Zaragoza, Spain
ICREA—Institució Catalana de Recerca i Estudis Avançats, Passeig Lluís Companys 23, 08010 Barcelona, Spain
Cite this: Chem. Mater. 2016, 28, 15, 5384–5393
Publication Date (Web):July 12, 2016
https://doi.org/10.1021/acs.chemmater.6b01445
Copyright © 2016 American Chemical Society

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    Abstract

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    Doping colloidal quantum dots (CQDs) with aliovalent cations is a promising, yet underexplored, approach to control the optoelectronic properties in CQDs. In CQD doping, kinetics determine whether a dopant element will incorporate into the host crystal structure, while thermodynamics dictate the mechanism of dopant incorporation. Here, we show that those mechanisms can be readily monitored by simple optical measurements and XRD studies in CQD ensembles. Based on this, we outline the critical role of dopant solubility limit in CQD doping, bridging the gap between nanocrystalline and bulk semiconductors. Finally, we present a combined simulation and X-ray absorption fine structure (XAFS) data study to shed new insights on the origin of charge compensation upon doping in CQD materials that has, thus far, limited high doping efficacy, even under efficient dopant incorporation schemes.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.6b01445.

    • Supplementary figures with XRD spectra and related peak fitting examples, additional optical absorption and PL spectra, TEM and HAADF micrographs and CQD size analysis, FFT of XAFS spectra, XANES spectra, fits of the first-shell XAFS signal, supplementary discussion regarding interatomic distances, supplementary tables regarding local structure around atoms, calculated energies of formation of complexes, percentage of Sb dopants in oxide phase (PDF)

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