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Title: Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene

Abstract

Colloidal nanocrystals (NCs) of lead chalcogenides are a promising class of tunable infrared materials for applications in devices such as photodetectors and solar cells. Such devices typically employ electronic materials in which charge carrier concentrations are manipulated through “doping;” however, persistent electronic doping of these NCs remains a challenge. In this paper, we demonstrate that heavily doped n-type PbSe and PbS NCs can be realized utilizing ground-state electron transfer from cobaltocene. This allows injecting up to eight electrons per NC into the band-edge state and maintaining the doping level for at least a month at room temperature. Doping is confirmed by inter- and intra-band optical absorption, as well as by carrier dynamics. In conclusion, FET measurements of doped NC films and the demonstration of a p-n diode provide additional evidence that the developed doping procedure allows for persistent incorporation of electrons into the quantum-confined NC states.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1]
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  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Advanced Solar Photophysics
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1321722
Report Number(s):
LA-UR-12-25467
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 3; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; inorganic and physical chemistry; material science; electronic properties and materials; infrared spectroscopy; quantum dots

Citation Formats

Koh, Weon-kyu, Koposov, Alexey Y., Stewart, John T., Pal, Bhola N., Robel, Istvan, Pietryga, Jeffrey M., and Klimov, Victor I. Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene. United States: N. p., 2013. Web. doi:10.1038/srep02004.
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Koh, Weon-kyu, Koposov, Alexey Y., Stewart, John T., Pal, Bhola N., Robel, Istvan, Pietryga, Jeffrey M., & Klimov, Victor I. Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene. United States. https://doi.org/10.1038/srep02004
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Koh, Weon-kyu, Koposov, Alexey Y., Stewart, John T., Pal, Bhola N., Robel, Istvan, Pietryga, Jeffrey M., and Klimov, Victor I. Tue . "Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene". United States. https://doi.org/10.1038/srep02004. https://www.osti.gov/servlets/purl/1321722.
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@article{osti_1321722,
title = {Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene},
author = {Koh, Weon-kyu and Koposov, Alexey Y. and Stewart, John T. and Pal, Bhola N. and Robel, Istvan and Pietryga, Jeffrey M. and Klimov, Victor I.},
abstractNote = {Colloidal nanocrystals (NCs) of lead chalcogenides are a promising class of tunable infrared materials for applications in devices such as photodetectors and solar cells. Such devices typically employ electronic materials in which charge carrier concentrations are manipulated through “doping;” however, persistent electronic doping of these NCs remains a challenge. In this paper, we demonstrate that heavily doped n-type PbSe and PbS NCs can be realized utilizing ground-state electron transfer from cobaltocene. This allows injecting up to eight electrons per NC into the band-edge state and maintaining the doping level for at least a month at room temperature. Doping is confirmed by inter- and intra-band optical absorption, as well as by carrier dynamics. In conclusion, FET measurements of doped NC films and the demonstration of a p-n diode provide additional evidence that the developed doping procedure allows for persistent incorporation of electrons into the quantum-confined NC states.},
doi = {10.1038/srep02004},
journal = {Scientific Reports},
number = ,
volume = 3,
place = {United States},
year = {Tue Jun 18 00:00:00 EDT 2013},
month = {Tue Jun 18 00:00:00 EDT 2013}
}
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https://doi.org/10.1038/srep02004
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New Aspects of Carrier Multiplication in Semiconductor Nanocrystals
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Controlled Chemical Doping of Semiconductor Nanocrystals Using Redox Buffers
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A Reduction Pathway in the Synthesis of PbSe Nanocrystal Quantum Dots
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Comparison of Carrier Multiplication Yields in PbS and PbSe Nanocrystals: The Role of Competing Energy-Loss Processes
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PbSe Quantum Dot Field-Effect Transistors with Air-Stable Electron Mobilities above 7 cm 2 V –1 s –1
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Effect of Air Exposure on Surface Properties, Electronic Structure, and Carrier Relaxation in PbSe Nanocrystals
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  • ACS Nano, Vol. 4, Issue 4
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Control of the Carrier Type in InAs Nanocrystal Films by Predeposition Incorporation of Cd
journal, December 2010

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  • ACS Nano, Vol. 4, Issue 12
  • DOI: 10.1021/nn101772n

Size-Dependent Valence and Conduction Band-Edge Energies of Semiconductor Nanocrystals
journal, June 2011

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A Charge-Orbital Balance Picture of Doping in Colloidal Quantum Dot Solids
journal, August 2012

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Electron Injection from Colloidal PbS Quantum Dots into Titanium Dioxide Nanoparticles
journal, October 2008

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  • ACS Nano, Vol. 2, Issue 11
  • DOI: 10.1021/nn800336b

Size-Dependent Optical Properties of Colloidal PbS Quantum Dots
journal, September 2009

  • Moreels, Iwan; Lambert, Karel; Smeets, Dries
  • ACS Nano, Vol. 3, Issue 10
  • DOI: 10.1021/nn900863a

n-type colloidal semiconductor nanocrystals
journal, October 2000

  • Shim, Moonsub; Guyot-Sionnest, Philippe
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Role of mid-gap states in charge transport and photoconductivity in semiconductor nanocrystal films
journal, September 2011

  • Nagpal, Prashant; Klimov, Victor I.
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PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors
journal, October 2005

Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell
journal, December 2011

Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals
journal, May 2007

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    25th Anniversary Article: Colloidal Quantum Dot Materials and Devices: A Quarter-Century of Advances
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