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Title: One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells

Abstract

Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifested in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.

Authors:
; ; ; ; ;  [1];  [1]; ; ORCiD logo
  1. Department of Chemistry and Biochemistry, St. Mary’s University, San Antonio, Texas 78228, United States
Publication Date:
Research Org.:
Bowling Green State Univ., Bowling Green, OH (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1361222
Alternate Identifier(s):
OSTI ID: 1372222
Grant/Contract Number:  
SC0016872
Resource Type:
Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Name: Journal of the American Chemical Society Journal Volume: 139 Journal Issue: 23; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Razgoniaeva, Natalia, Moroz, Pavel, Yang, Mingrui, Budkina, Darya S., Eckard, Holly, Augspurger, Marissa, Khon, Dmitriy, Tarnovsky, Alexander N., and Zamkov, Mikhail. One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells. United States: N. p., 2017. Web. doi:10.1021/jacs.7b02054.
Razgoniaeva, Natalia, Moroz, Pavel, Yang, Mingrui, Budkina, Darya S., Eckard, Holly, Augspurger, Marissa, Khon, Dmitriy, Tarnovsky, Alexander N., & Zamkov, Mikhail. One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells. United States. doi:10.1021/jacs.7b02054.
Razgoniaeva, Natalia, Moroz, Pavel, Yang, Mingrui, Budkina, Darya S., Eckard, Holly, Augspurger, Marissa, Khon, Dmitriy, Tarnovsky, Alexander N., and Zamkov, Mikhail. Mon . "One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells". United States. doi:10.1021/jacs.7b02054.
@article{osti_1361222,
title = {One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells},
author = {Razgoniaeva, Natalia and Moroz, Pavel and Yang, Mingrui and Budkina, Darya S. and Eckard, Holly and Augspurger, Marissa and Khon, Dmitriy and Tarnovsky, Alexander N. and Zamkov, Mikhail},
abstractNote = {Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifested in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.},
doi = {10.1021/jacs.7b02054},
journal = {Journal of the American Chemical Society},
number = 23,
volume = 139,
place = {United States},
year = {2017},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/jacs.7b02054

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Cited by: 1 work
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