N-Doping of Quantum Dots by Lithium Ion Intercalation

Woo Je Chang; Kyu Young Park; Yizhou Zhu; Christopher Wolverton; Mark C. Hersam; Emily A. Weiss

doi:10.1021/acsami.0c09366

N-Doping of Quantum Dots by Lithium Ion Intercalation

Woo Je Chang, Kyu Young Park, Yizhou Zhu, Christopher Wolverton, Mark C. Hersam, Emily A. Weiss^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

The optical properties of colloidal quantum dots (QDs) are controllable through introduction of excess electrons or holes into their delocalized bands. Crucial to robust and energy-efficient electronic doping of QDs is suitable charge compensation. Compensation by surface modification and substitutional impurities are however not sufficiently controllable to enable effective doping of QDs. This article describes electrochemical n-type doping of CdSe QDs where injected electrons are compensated by interstitial Li+ to form LixCdSe, x ≤ 0.3. n-type degenerate doping reversibly decreases absorption into the lowest-energy excitonic state of the QD, activates intraband optical transitions, and shifts the photoluminescence of the QD to higher energy. This work establishes electrochemical interstitial doping as a reversible and highly controllable method for tuning the optical properties of colloidal QDs.

Original language	English (US)
Pages (from-to)	36523-36529
Number of pages	7
Journal	ACS Applied Materials and Interfaces
Volume	12
Issue number	32
DOIs	https://doi.org/10.1021/acsami.0c09366
State	Published - Aug 12 2020

Keywords

CdSe
electronic doping
interstitial doping
lithiation
optical spectra
quantum dot

ASJC Scopus subject areas

Materials Science(all)

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10.1021/acsami.0c09366

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@article{0947b3868c674667910e67944cb7d0bb,

title = "N-Doping of Quantum Dots by Lithium Ion Intercalation",

abstract = "The optical properties of colloidal quantum dots (QDs) are controllable through introduction of excess electrons or holes into their delocalized bands. Crucial to robust and energy-efficient electronic doping of QDs is suitable charge compensation. Compensation by surface modification and substitutional impurities are however not sufficiently controllable to enable effective doping of QDs. This article describes electrochemical n-type doping of CdSe QDs where injected electrons are compensated by interstitial Li+ to form LixCdSe, x ≤ 0.3. n-type degenerate doping reversibly decreases absorption into the lowest-energy excitonic state of the QD, activates intraband optical transitions, and shifts the photoluminescence of the QD to higher energy. This work establishes electrochemical interstitial doping as a reversible and highly controllable method for tuning the optical properties of colloidal QDs.",

keywords = "CdSe, electronic doping, interstitial doping, lithiation, optical spectra, quantum dot",

author = "Chang, {Woo Je} and Park, {Kyu Young} and Yizhou Zhu and Christopher Wolverton and Hersam, {Mark C.} and Weiss, {Emily A.}",

note = "Funding Information: This research was supported by the National Science Foundation (NSF) Materials Research Science and Engineering Center (MRSEC) of Northwestern University (NSF DMR-1720139). W.J.C. acknowledges support from the Kwanjeong Fellowship. Y.Z. and C.W. acknowledge support from the Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center funded by the U.S. Department of Energy under award no. DE-AC02-06CH11357 (first principles calculations). W.J.C. acknowledges Suyog Padgaonkar for TEM imaging. Publisher Copyright: {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = aug,

day = "12",

doi = "10.1021/acsami.0c09366",

language = "English (US)",

volume = "12",

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journal = "ACS Applied Materials and Interfaces",

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publisher = "American Chemical Society",

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AU - Chang, Woo Je

AU - Park, Kyu Young

AU - Zhu, Yizhou

AU - Wolverton, Christopher

AU - Hersam, Mark C.

AU - Weiss, Emily A.

N1 - Funding Information: This research was supported by the National Science Foundation (NSF) Materials Research Science and Engineering Center (MRSEC) of Northwestern University (NSF DMR-1720139). W.J.C. acknowledges support from the Kwanjeong Fellowship. Y.Z. and C.W. acknowledge support from the Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center funded by the U.S. Department of Energy under award no. DE-AC02-06CH11357 (first principles calculations). W.J.C. acknowledges Suyog Padgaonkar for TEM imaging. Publisher Copyright: © 2020 American Chemical Society.

PY - 2020/8/12

Y1 - 2020/8/12

N2 - The optical properties of colloidal quantum dots (QDs) are controllable through introduction of excess electrons or holes into their delocalized bands. Crucial to robust and energy-efficient electronic doping of QDs is suitable charge compensation. Compensation by surface modification and substitutional impurities are however not sufficiently controllable to enable effective doping of QDs. This article describes electrochemical n-type doping of CdSe QDs where injected electrons are compensated by interstitial Li+ to form LixCdSe, x ≤ 0.3. n-type degenerate doping reversibly decreases absorption into the lowest-energy excitonic state of the QD, activates intraband optical transitions, and shifts the photoluminescence of the QD to higher energy. This work establishes electrochemical interstitial doping as a reversible and highly controllable method for tuning the optical properties of colloidal QDs.

AB - The optical properties of colloidal quantum dots (QDs) are controllable through introduction of excess electrons or holes into their delocalized bands. Crucial to robust and energy-efficient electronic doping of QDs is suitable charge compensation. Compensation by surface modification and substitutional impurities are however not sufficiently controllable to enable effective doping of QDs. This article describes electrochemical n-type doping of CdSe QDs where injected electrons are compensated by interstitial Li+ to form LixCdSe, x ≤ 0.3. n-type degenerate doping reversibly decreases absorption into the lowest-energy excitonic state of the QD, activates intraband optical transitions, and shifts the photoluminescence of the QD to higher energy. This work establishes electrochemical interstitial doping as a reversible and highly controllable method for tuning the optical properties of colloidal QDs.

KW - CdSe

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KW - optical spectra

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N-Doping of Quantum Dots by Lithium Ion Intercalation

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