Plasmonic Oleylamine-Capped Gold and Silver Nanoparticle-Assisted Synthesis of Luminescent Alloyed CdZnSeS Quantum Dots

Oluwasesan Adegoke (Lead / Corresponding author), Kenshin Takemura, Enoch Y. Park (Lead / Corresponding author)

Research output: Contribution to journalArticle

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Abstract

We report on a novel strategy to tune the structural and optical properties of luminescent alloyed quantum dot (QD) nanocrystals using plasmonic gold (Au) and silver (Ag) nanoparticles (NPs). Alloyed CdZnSeS QDs were synthesized via the organometallic synthetic route with different fabrication strategies that involve alternative utilization of blends of organic surfactants, ligands, capping agents, and plasmonic oleylamine (OLA)-functionalized AuNPs and AgNPs. Ligand exchange with thiol l-cysteine (l-cyst) was used to prepare the hydrophilic nanocrystals. Analysis of the structural properties using powder X-ray diffraction revealed that under the same experimental condition, the plasmonic NPs altered the diffractive crystal structure of the alloyed QDs. Depending on the fabrication strategy, the crystal nature of OLA-AuNP-assisted CdZnSeS QDs was a pure hexagonal wurtzite domain and a cubic zinc-blende domain, whereas the diffraction pattern of OLA-AgNP-assisted CdZnSeS QDs was dominantly a cubic zinc-blende domain. Insights into the growth morphology of the QDs revealed a steady transformation from a heterogeneous growth pattern to a homogenous growth pattern that was strongly influenced by the plasmonic NPs. Tuning the optical properties of the alloyed QDs via plasmonic optical engineering showed that the photoluminescence (PL) quantum yield (QY) of the AuNP-assisted l-cyst-CdZnSeS QDs was tuned from 10 to 31%, whereas the PL QY of the AgNP-assisted l-cyst-CdZnSeS QDs was tuned from 15 to 90%. The low PL QY was associated with the surface defect state, while the remarkably high PL QY exhibited by the AgNP-assisted l-cyst-CdZnSeS QDs lends strong affirmation that the fabrication strategy employed in this work provides a unique opportunity to create single ensemble, multifunctional, highly fluorescent alloyed QDs for tailored biological applications.
Original languageEnglish
Pages (from-to)1357-1366
Number of pages10
JournalACS Omega
Volume3
Issue number2
DOIs
Publication statusPublished - 1 Feb 2018

Cite this

@article{2889a42e21c04f19831e69980c6504d0,
title = "Plasmonic Oleylamine-Capped Gold and Silver Nanoparticle-Assisted Synthesis of Luminescent Alloyed CdZnSeS Quantum Dots",
abstract = "We report on a novel strategy to tune the structural and optical properties of luminescent alloyed quantum dot (QD) nanocrystals using plasmonic gold (Au) and silver (Ag) nanoparticles (NPs). Alloyed CdZnSeS QDs were synthesized via the organometallic synthetic route with different fabrication strategies that involve alternative utilization of blends of organic surfactants, ligands, capping agents, and plasmonic oleylamine (OLA)-functionalized AuNPs and AgNPs. Ligand exchange with thiol l-cysteine (l-cyst) was used to prepare the hydrophilic nanocrystals. Analysis of the structural properties using powder X-ray diffraction revealed that under the same experimental condition, the plasmonic NPs altered the diffractive crystal structure of the alloyed QDs. Depending on the fabrication strategy, the crystal nature of OLA-AuNP-assisted CdZnSeS QDs was a pure hexagonal wurtzite domain and a cubic zinc-blende domain, whereas the diffraction pattern of OLA-AgNP-assisted CdZnSeS QDs was dominantly a cubic zinc-blende domain. Insights into the growth morphology of the QDs revealed a steady transformation from a heterogeneous growth pattern to a homogenous growth pattern that was strongly influenced by the plasmonic NPs. Tuning the optical properties of the alloyed QDs via plasmonic optical engineering showed that the photoluminescence (PL) quantum yield (QY) of the AuNP-assisted l-cyst-CdZnSeS QDs was tuned from 10 to 31{\%}, whereas the PL QY of the AgNP-assisted l-cyst-CdZnSeS QDs was tuned from 15 to 90{\%}. The low PL QY was associated with the surface defect state, while the remarkably high PL QY exhibited by the AgNP-assisted l-cyst-CdZnSeS QDs lends strong affirmation that the fabrication strategy employed in this work provides a unique opportunity to create single ensemble, multifunctional, highly fluorescent alloyed QDs for tailored biological applications.",
author = "Oluwasesan Adegoke and Kenshin Takemura and Park, {Enoch Y.}",
note = "O.A. gratefully acknowledges the Japan Society for the Promotion of Science (JSPS) for a postdoctoral fellowship for overseas researchers (P13454). This work was supported by the Grantin-Aid for a JSPS fellow (no. 26-04354).",
year = "2018",
month = "2",
day = "1",
doi = "10.1021/acsomega.7b01724",
language = "English",
volume = "3",
pages = "1357--1366",
journal = "ACS Omega",
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publisher = "American Chemical Society",
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Plasmonic Oleylamine-Capped Gold and Silver Nanoparticle-Assisted Synthesis of Luminescent Alloyed CdZnSeS Quantum Dots. / Adegoke, Oluwasesan (Lead / Corresponding author); Takemura, Kenshin; Park, Enoch Y. (Lead / Corresponding author).

In: ACS Omega, Vol. 3, No. 2, 01.02.2018, p. 1357-1366.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Plasmonic Oleylamine-Capped Gold and Silver Nanoparticle-Assisted Synthesis of Luminescent Alloyed CdZnSeS Quantum Dots

AU - Adegoke, Oluwasesan

AU - Takemura, Kenshin

AU - Park, Enoch Y.

N1 - O.A. gratefully acknowledges the Japan Society for the Promotion of Science (JSPS) for a postdoctoral fellowship for overseas researchers (P13454). This work was supported by the Grantin-Aid for a JSPS fellow (no. 26-04354).

PY - 2018/2/1

Y1 - 2018/2/1

N2 - We report on a novel strategy to tune the structural and optical properties of luminescent alloyed quantum dot (QD) nanocrystals using plasmonic gold (Au) and silver (Ag) nanoparticles (NPs). Alloyed CdZnSeS QDs were synthesized via the organometallic synthetic route with different fabrication strategies that involve alternative utilization of blends of organic surfactants, ligands, capping agents, and plasmonic oleylamine (OLA)-functionalized AuNPs and AgNPs. Ligand exchange with thiol l-cysteine (l-cyst) was used to prepare the hydrophilic nanocrystals. Analysis of the structural properties using powder X-ray diffraction revealed that under the same experimental condition, the plasmonic NPs altered the diffractive crystal structure of the alloyed QDs. Depending on the fabrication strategy, the crystal nature of OLA-AuNP-assisted CdZnSeS QDs was a pure hexagonal wurtzite domain and a cubic zinc-blende domain, whereas the diffraction pattern of OLA-AgNP-assisted CdZnSeS QDs was dominantly a cubic zinc-blende domain. Insights into the growth morphology of the QDs revealed a steady transformation from a heterogeneous growth pattern to a homogenous growth pattern that was strongly influenced by the plasmonic NPs. Tuning the optical properties of the alloyed QDs via plasmonic optical engineering showed that the photoluminescence (PL) quantum yield (QY) of the AuNP-assisted l-cyst-CdZnSeS QDs was tuned from 10 to 31%, whereas the PL QY of the AgNP-assisted l-cyst-CdZnSeS QDs was tuned from 15 to 90%. The low PL QY was associated with the surface defect state, while the remarkably high PL QY exhibited by the AgNP-assisted l-cyst-CdZnSeS QDs lends strong affirmation that the fabrication strategy employed in this work provides a unique opportunity to create single ensemble, multifunctional, highly fluorescent alloyed QDs for tailored biological applications.

AB - We report on a novel strategy to tune the structural and optical properties of luminescent alloyed quantum dot (QD) nanocrystals using plasmonic gold (Au) and silver (Ag) nanoparticles (NPs). Alloyed CdZnSeS QDs were synthesized via the organometallic synthetic route with different fabrication strategies that involve alternative utilization of blends of organic surfactants, ligands, capping agents, and plasmonic oleylamine (OLA)-functionalized AuNPs and AgNPs. Ligand exchange with thiol l-cysteine (l-cyst) was used to prepare the hydrophilic nanocrystals. Analysis of the structural properties using powder X-ray diffraction revealed that under the same experimental condition, the plasmonic NPs altered the diffractive crystal structure of the alloyed QDs. Depending on the fabrication strategy, the crystal nature of OLA-AuNP-assisted CdZnSeS QDs was a pure hexagonal wurtzite domain and a cubic zinc-blende domain, whereas the diffraction pattern of OLA-AgNP-assisted CdZnSeS QDs was dominantly a cubic zinc-blende domain. Insights into the growth morphology of the QDs revealed a steady transformation from a heterogeneous growth pattern to a homogenous growth pattern that was strongly influenced by the plasmonic NPs. Tuning the optical properties of the alloyed QDs via plasmonic optical engineering showed that the photoluminescence (PL) quantum yield (QY) of the AuNP-assisted l-cyst-CdZnSeS QDs was tuned from 10 to 31%, whereas the PL QY of the AgNP-assisted l-cyst-CdZnSeS QDs was tuned from 15 to 90%. The low PL QY was associated with the surface defect state, while the remarkably high PL QY exhibited by the AgNP-assisted l-cyst-CdZnSeS QDs lends strong affirmation that the fabrication strategy employed in this work provides a unique opportunity to create single ensemble, multifunctional, highly fluorescent alloyed QDs for tailored biological applications.

U2 - 10.1021/acsomega.7b01724

DO - 10.1021/acsomega.7b01724

M3 - Article

VL - 3

SP - 1357

EP - 1366

JO - ACS Omega

JF - ACS Omega

SN - 2470-1343

IS - 2

ER -