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Title: Bandgap Engineering of Indium Phosphide-Based Core/Shell Heterostructures Through Shell Composition and Thickness

Abstract

The large bulk bandgap (1.35 eV) and Bohr radius (~10 nm) of InP semiconductor nanocrystals provides bandgap tunability over a wide spectral range, providing superior color tuning compared to that of CdSe quantum dots. In this paper, the dependence of the bandgap, photoluminescence emission, and exciton radiative lifetime of core/shell quantum dot heterostructures has been investigated using colloidal InP core nanocrystals with multiple diameters (1.5, 2.5, and 3.7 nm). The shell thickness and composition dependence of the bandgap for type-I and type-II heterostructures was observed by coating the InP core with ZnS, ZnSe, CdS, or CdSe through one to ten iterations of a successive ion layer adsorption and reaction (SILAR)-based shell deposition. The empirical results are compared to bandgap energy predictions made with effective mass modeling. Photoluminescence emission colors have been successfully tuned throughout the visible and into the near infrared (NIR) wavelength ranges for type-I and type-II heterostructures, respectively. Based on sizing data from transmission electron microscopy (TEM), it is observed that at the same particle diameter, average radiative lifetimes can differ as much as 20-fold across different shell compositions due to the relative positions of valence and conduction bands. In this direct comparison of InP/ZnS, InP/ZnSe, InP/CdS, andmore » InP/CdSe core/shell heterostructures, we clearly delineate the impact of core size, shell composition, and shell thickness on the resulting optical properties. Specifically, Zn-based shells yield type-I structures that are color tuned through core size, while the Cd-based shells yield type-II particles that emit in the NIR regardless of the starting core size if several layers of CdS(e) have been successfully deposited. Particles with thicker CdS(e) shells exhibit longer photoluminescence lifetimes, while little shell-thickness dependence is observed for the Zn-based shells. Taken together, these InP-based heterostructures demonstrate the extent to which we are able to precisely tailor the material properties of core/shell particles using core/shell dimensions and composition as variables.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1482841
Alternate Identifier(s):
OSTI ID: 1484664
Report Number(s):
LA-UR-18-28366
Journal ID: ISSN 2296-2646; 567
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Published Article
Journal Name:
Frontiers in Chemistry
Additional Journal Information:
Journal Name: Frontiers in Chemistry Journal Volume: 6; Journal ID: ISSN 2296-2646
Publisher:
Frontiers Media SA
Country of Publication:
Switzerland
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science

Citation Formats

Toufanian, Reyhaneh, Piryatinski, Andrei, Mahler, Andrew H., Iyer, Radhika, Hollingsworth, Jennifer A., and Dennis, Allison M. Bandgap Engineering of Indium Phosphide-Based Core/Shell Heterostructures Through Shell Composition and Thickness. Switzerland: N. p., 2018. Web. doi:10.3389/fchem.2018.00567.
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Toufanian, Reyhaneh, Piryatinski, Andrei, Mahler, Andrew H., Iyer, Radhika, Hollingsworth, Jennifer A., & Dennis, Allison M. Bandgap Engineering of Indium Phosphide-Based Core/Shell Heterostructures Through Shell Composition and Thickness. Switzerland. doi:10.3389/fchem.2018.00567.
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Toufanian, Reyhaneh, Piryatinski, Andrei, Mahler, Andrew H., Iyer, Radhika, Hollingsworth, Jennifer A., and Dennis, Allison M. Tue . "Bandgap Engineering of Indium Phosphide-Based Core/Shell Heterostructures Through Shell Composition and Thickness". Switzerland. doi:10.3389/fchem.2018.00567.
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@article{osti_1482841,
title = {Bandgap Engineering of Indium Phosphide-Based Core/Shell Heterostructures Through Shell Composition and Thickness},
author = {Toufanian, Reyhaneh and Piryatinski, Andrei and Mahler, Andrew H. and Iyer, Radhika and Hollingsworth, Jennifer A. and Dennis, Allison M.},
abstractNote = {The large bulk bandgap (1.35 eV) and Bohr radius (~10 nm) of InP semiconductor nanocrystals provides bandgap tunability over a wide spectral range, providing superior color tuning compared to that of CdSe quantum dots. In this paper, the dependence of the bandgap, photoluminescence emission, and exciton radiative lifetime of core/shell quantum dot heterostructures has been investigated using colloidal InP core nanocrystals with multiple diameters (1.5, 2.5, and 3.7 nm). The shell thickness and composition dependence of the bandgap for type-I and type-II heterostructures was observed by coating the InP core with ZnS, ZnSe, CdS, or CdSe through one to ten iterations of a successive ion layer adsorption and reaction (SILAR)-based shell deposition. The empirical results are compared to bandgap energy predictions made with effective mass modeling. Photoluminescence emission colors have been successfully tuned throughout the visible and into the near infrared (NIR) wavelength ranges for type-I and type-II heterostructures, respectively. Based on sizing data from transmission electron microscopy (TEM), it is observed that at the same particle diameter, average radiative lifetimes can differ as much as 20-fold across different shell compositions due to the relative positions of valence and conduction bands. In this direct comparison of InP/ZnS, InP/ZnSe, InP/CdS, and InP/CdSe core/shell heterostructures, we clearly delineate the impact of core size, shell composition, and shell thickness on the resulting optical properties. Specifically, Zn-based shells yield type-I structures that are color tuned through core size, while the Cd-based shells yield type-II particles that emit in the NIR regardless of the starting core size if several layers of CdS(e) have been successfully deposited. Particles with thicker CdS(e) shells exhibit longer photoluminescence lifetimes, while little shell-thickness dependence is observed for the Zn-based shells. Taken together, these InP-based heterostructures demonstrate the extent to which we are able to precisely tailor the material properties of core/shell particles using core/shell dimensions and composition as variables.},
doi = {10.3389/fchem.2018.00567},
journal = {Frontiers in Chemistry},
number = ,
volume = 6,
place = {Switzerland},
year = {2018},
month = {11}
}
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DOI: 10.3389/fchem.2018.00567
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Figures / Tables:

FIGURE 1 FIGURE 1: (A) Schematic representation of the relative positions of conduction and valence bands in different core/shell heterostructures. (B) Relative positions of the conduction and valance bands of the semiconductors used in this study (Wei and Zunger, 1998; Reiss et al., 2009).
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