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Title: Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO3 phosphors

Abstract

We report on the synthesis and structural characterization of novel semiconducting heterostructures composed of cadmium selenide (CdSe) quantum dots (QDs) attached onto the surfaces of novel high-surface area, porous rare-earth-ion doped alkaline earth titanate micron-scale spherical motifs, i.e. both Eu-doped and Pr-doped CaTiO3, composed of constituent, component nanoparticles. These unique metal oxide perovskite building blocks were created by a multi-pronged synthetic strategy involving molten salt and hydrothermal protocols. Subsequently, optical characterization of these heterostructures indicated a clear behavioral dependence of charge transfer in these systems upon a number of parameters such as the nature of the dopant, the reaction temperature, and particle size. Specifically, 2.7 nm diameter ligand-functionalized CdSe QDs were anchored onto sub-micron sized CaTiO3-based spherical assemblies, prepared by molten salt protocols. We found that both the Pr- and Eu-doped CaTiO3 displayed pronounced PL emissions, with maximum intensities observed using optimized lanthanide concentrations of 0.2 mol% and 6 mol%, respectively. Analogous experiments were performed on Eu-doped BaTiO3 and SrTiO3 motifs, but CaTiO3 still performed as the most effective host material amongst the three perovskite systems tested. Furthermore, the ligand-capped CdSe QD-doped CaTiO3 heterostructures exhibited effective charge transfer between the two individual constituent nanoscale components, an assertion corroborated by themore » corresponding quenching of their measured PL signals.« less

Authors:
;  [1];  [1];  [2];  [1];  [1];  [1]
  1. State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1235862
Report Number(s):
BNL-111622-2015-JA
Journal ID: ISSN 2040-3364; NANOHL; R&D Project: PM037; KC0201030
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 8; Journal Issue: 4; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; CaTiO3; praseodymium; europium; rare earth ion-doped materials; doped perovskites; metal titanates; fluorescent and luminescent materials; optical properties

Citation Formats

Crystal S. Lewis, Wong, Stanislaus S., Liu, Haiqing, Han, Jinkyu, Wang, Lei, Yue, Shiyu, and Brennan, Nicholas A. Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO3 phosphors. United States: N. p., 2016. Web. doi:10.1039/C5NR06697B.
Crystal S. Lewis, Wong, Stanislaus S., Liu, Haiqing, Han, Jinkyu, Wang, Lei, Yue, Shiyu, & Brennan, Nicholas A. Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO3 phosphors. United States. https://doi.org/10.1039/C5NR06697B
Crystal S. Lewis, Wong, Stanislaus S., Liu, Haiqing, Han, Jinkyu, Wang, Lei, Yue, Shiyu, and Brennan, Nicholas A. Mon . "Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO3 phosphors". United States. https://doi.org/10.1039/C5NR06697B. https://www.osti.gov/servlets/purl/1235862.
@article{osti_1235862,
title = {Probing charge transfer in a novel class of luminescent perovskite-based heterostructures composed of quantum dots bound to RE-activated CaTiO3 phosphors},
author = {Crystal S. Lewis and Wong, Stanislaus S. and Liu, Haiqing and Han, Jinkyu and Wang, Lei and Yue, Shiyu and Brennan, Nicholas A.},
abstractNote = {We report on the synthesis and structural characterization of novel semiconducting heterostructures composed of cadmium selenide (CdSe) quantum dots (QDs) attached onto the surfaces of novel high-surface area, porous rare-earth-ion doped alkaline earth titanate micron-scale spherical motifs, i.e. both Eu-doped and Pr-doped CaTiO3, composed of constituent, component nanoparticles. These unique metal oxide perovskite building blocks were created by a multi-pronged synthetic strategy involving molten salt and hydrothermal protocols. Subsequently, optical characterization of these heterostructures indicated a clear behavioral dependence of charge transfer in these systems upon a number of parameters such as the nature of the dopant, the reaction temperature, and particle size. Specifically, 2.7 nm diameter ligand-functionalized CdSe QDs were anchored onto sub-micron sized CaTiO3-based spherical assemblies, prepared by molten salt protocols. We found that both the Pr- and Eu-doped CaTiO3 displayed pronounced PL emissions, with maximum intensities observed using optimized lanthanide concentrations of 0.2 mol% and 6 mol%, respectively. Analogous experiments were performed on Eu-doped BaTiO3 and SrTiO3 motifs, but CaTiO3 still performed as the most effective host material amongst the three perovskite systems tested. Furthermore, the ligand-capped CdSe QD-doped CaTiO3 heterostructures exhibited effective charge transfer between the two individual constituent nanoscale components, an assertion corroborated by the corresponding quenching of their measured PL signals.},
doi = {10.1039/C5NR06697B},
journal = {Nanoscale},
number = 4,
volume = 8,
place = {United States},
year = {Mon Jan 04 00:00:00 EST 2016},
month = {Mon Jan 04 00:00:00 EST 2016}
}

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Cited by: 18 works
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Works referencing / citing this record:

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