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Tunable Band-Edge Potentials and Charge Storage in Colloidal Tin-Doped Indium Oxide (ITO) Nanocrystals

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    Tunable Band-Edge Potentials and Charge Storage in Colloidal Tin-Doped Indium Oxide (ITO) Nanocrystals
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    ACS Nano

    Cite this: ACS Nano 2021, 15, 9, 14116–14124
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    https://doi.org/10.1021/acsnano.1c04660
    Published August 13, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Degenerately doped metal-oxide nanocrystals (NCs) show localized surface plasmon resonances (LSPRs) that are tunable via their tunable excess charge-carrier densities. Modulation of excess charge carriers has also been used to control magnetism in colloidal doped metal-oxide NCs. The addition of excess delocalized conduction-band (CB) electrons can be achieved through aliovalent doping or by postsynthetic techniques such as electrochemistry or photodoping. Here, we examine the influence of charge-compensating aliovalent dopants on the potentials of excess CB electrons in free-standing colloidal degenerately doped oxide NCs, both experimentally and through modeling. Taking Sn4+:In2O3 (ITO) NCs as a model system, we use spectroelectrochemical techniques to examine differences between aliovalent doping and photodoping. We demonstrate that whereas photodoping introduces excess CB electrons by raising the Fermi level relative to the CB edge, aliovalent impurity substitution introduces excess CB electrons by stabilizing the CB edge relative to an externally defined Fermi level. Significant differences are thus observed electrochemically between spectroscopically similar delocalized CB electrons compensated by aliovalent dopants and those compensated by surface cations (e.g., protons) during photodoping. Theoretical modeling illustrates the very different potentials that arise from charge compensation via aliovalent substitution and surface charge compensation. Spectroelectrochemical titrations allow the ITO NC band-edge stabilization as a function of Sn4+ doping to be quantified. Extremely large capacitances are observed in both In2O3 and ITO NCs, making these NCs attractive for reversible charge-storage applications.

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    • Size analysis, absorption, and titration data for In2O3 and ITO NCs of varying Sn4+ concentration, potentiometric titration data, description of computational methods, and charged sphere model calculations (PDF)

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    This article is cited by 14 publications.

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    ACS Nano

    Cite this: ACS Nano 2021, 15, 9, 14116–14124
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.1c04660
    Published August 13, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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