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Title: Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals

Abstract

Doped metal oxide nanocrystals represent an exciting frontier for colloidal synthesis of plasmonic materials, displaying unique optoelectronic properties and showing promise for a variety of applications. However, fundamental questions about the nature of doping in these materials remain. In this article, the strong influence of radial dopant distribution on the optoelectronic properties of colloidal indium tin oxide nanocrystals is reported. Comparing elemental depth-profiling by X-ray photoelectron spectroscopy (XPS) with detailed modeling and simulation of the optical extinction of these nanocrystals using the Drude model for free electrons, a correlation between surface segregation of tin ions and the average activation of dopants is observed. A strong influence of surface segregation of tin on the line shape of the localized surface plasmon resonance (LSPR) is also reported. Samples with tin segregated near the surface show a symmetric line shape that suggests weak or no damping of the plasmon by ionized impurities. It is suggested that segregation of tin near the surface facilitates compensation of the dopant ions by electronic defects and oxygen interstitials, thus reducing activation. A core shell model is proposed to explain the observed differences in line shape. These results demonstrate the nuanced role of dopant distribution in determining themore » optoelectronic properties of semiconductor nanocrystals and suggest that more detailed study of the distribution and structure of defects in plasmonic colloidal nanocrystals is warranted.« less

Authors:
; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1211171
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 136; Journal Issue: 19; Journal ID: ISSN 0002-7863
Country of Publication:
United States
Language:
English

Citation Formats

Lounis, SD, Runnerstrom, EL, Bergerud, A, Nordlund, D, and Milliron, DJ. Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals. United States: N. p., 2014. Web. doi:10.1021/ja502541z.
Lounis, SD, Runnerstrom, EL, Bergerud, A, Nordlund, D, & Milliron, DJ. Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals. United States. https://doi.org/10.1021/ja502541z
Lounis, SD, Runnerstrom, EL, Bergerud, A, Nordlund, D, and Milliron, DJ. 2014. "Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals". United States. https://doi.org/10.1021/ja502541z.
@article{osti_1211171,
title = {Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals},
author = {Lounis, SD and Runnerstrom, EL and Bergerud, A and Nordlund, D and Milliron, DJ},
abstractNote = {Doped metal oxide nanocrystals represent an exciting frontier for colloidal synthesis of plasmonic materials, displaying unique optoelectronic properties and showing promise for a variety of applications. However, fundamental questions about the nature of doping in these materials remain. In this article, the strong influence of radial dopant distribution on the optoelectronic properties of colloidal indium tin oxide nanocrystals is reported. Comparing elemental depth-profiling by X-ray photoelectron spectroscopy (XPS) with detailed modeling and simulation of the optical extinction of these nanocrystals using the Drude model for free electrons, a correlation between surface segregation of tin ions and the average activation of dopants is observed. A strong influence of surface segregation of tin on the line shape of the localized surface plasmon resonance (LSPR) is also reported. Samples with tin segregated near the surface show a symmetric line shape that suggests weak or no damping of the plasmon by ionized impurities. It is suggested that segregation of tin near the surface facilitates compensation of the dopant ions by electronic defects and oxygen interstitials, thus reducing activation. A core shell model is proposed to explain the observed differences in line shape. These results demonstrate the nuanced role of dopant distribution in determining the optoelectronic properties of semiconductor nanocrystals and suggest that more detailed study of the distribution and structure of defects in plasmonic colloidal nanocrystals is warranted.},
doi = {10.1021/ja502541z},
url = {https://www.osti.gov/biblio/1211171}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 19,
volume = 136,
place = {United States},
year = {Wed May 14 00:00:00 EDT 2014},
month = {Wed May 14 00:00:00 EDT 2014}
}