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Title: Distinct Optoelectronic Signatures for Charge Transfer and Energy Transfer in Quantum Dot-MoS2 Hybrid Photodetectors Revealed by Photocurrent Imaging Microscopy

Abstract

Atomically thin transition metal dichalcogenides (TMDCs) have intriguing nanoscale properties like high charge mobility, photosensitivity, layer-thickness-dependent bandgap, and mechanical flexibility, which are all appealing for the development of next generation optoelectronic, catalytic, and sensory devices. Their atomically thin thickness, however, renders TMDCs poor absorptivity. For this study, bilayer MoS2 is combined with core-only CdSe QDs and core/shell CdSe/ZnS QDs to obtain hybrids with increased light harvesting and exhibiting interfacial charge transfer (CT) and nonradiative energy transfer (NET), respectively. Field-effect transistors based on these hybrids and their responses to varying laser power and applied gate voltage are investigated with scanning photocurrent microscopy (SPCM) in view of their potential utilization in light harvesting and photodetector applications. CdSe–MoS2 hybrids are found to exhibit encouraging properties for photodetectors, like high responsivity and fast on/off response under low light exposure while CdSe/ZnS–MoS2 hybrids show enhanced charge carrier generation with increased light exposure, thus suitable for photovoltaics. While distinguishing optically between CT and NET in QD–TMDCs is nontrivial, it is found that they can be differentiated by SPCM as these two processes exhibit distinctive light-intensity dependencies: CT causes a photogating effect, decreasing the photocurrent response with increasing light power while NET increases the photocurrent response withmore » increasing light power, opposite to CT case.« less

Authors:
 [1];  [2];  [3];  [1];  [1]; ORCiD logo [1]
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  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  3. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering; Columbia Univ., New York, NY (United States). Dept. of Physics
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1440894
Alternate Identifier(s):
OSTI ID: 1437667
Report Number(s):
BNL-205746-2018-JAAM
Journal ID: ISSN 1616-301X
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 29; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; transition metal dichalcogenides; TMDCs; colloidal quantum dots; light harvesting; excitonic nanomaterials; photocurrent imaging; charge transfer; energy transfer

Citation Formats

Li, Mingxing, Chen, Jia-Shiang, Routh, Prahlad K., Zahl, Percy, Nam, Chang-Yong, and Cotlet, Mircea. Distinct Optoelectronic Signatures for Charge Transfer and Energy Transfer in Quantum Dot-MoS2 Hybrid Photodetectors Revealed by Photocurrent Imaging Microscopy. United States: N. p., 2018. Web. doi:10.1002/adfm.201707558.
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Li, Mingxing, Chen, Jia-Shiang, Routh, Prahlad K., Zahl, Percy, Nam, Chang-Yong, & Cotlet, Mircea. Distinct Optoelectronic Signatures for Charge Transfer and Energy Transfer in Quantum Dot-MoS2 Hybrid Photodetectors Revealed by Photocurrent Imaging Microscopy. United States. https://doi.org/10.1002/adfm.201707558
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Li, Mingxing, Chen, Jia-Shiang, Routh, Prahlad K., Zahl, Percy, Nam, Chang-Yong, and Cotlet, Mircea. Thu . "Distinct Optoelectronic Signatures for Charge Transfer and Energy Transfer in Quantum Dot-MoS2 Hybrid Photodetectors Revealed by Photocurrent Imaging Microscopy". United States. https://doi.org/10.1002/adfm.201707558. https://www.osti.gov/servlets/purl/1440894.
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@article{osti_1440894,
title = {Distinct Optoelectronic Signatures for Charge Transfer and Energy Transfer in Quantum Dot-MoS2 Hybrid Photodetectors Revealed by Photocurrent Imaging Microscopy},
author = {Li, Mingxing and Chen, Jia-Shiang and Routh, Prahlad K. and Zahl, Percy and Nam, Chang-Yong and Cotlet, Mircea},
abstractNote = {Atomically thin transition metal dichalcogenides (TMDCs) have intriguing nanoscale properties like high charge mobility, photosensitivity, layer-thickness-dependent bandgap, and mechanical flexibility, which are all appealing for the development of next generation optoelectronic, catalytic, and sensory devices. Their atomically thin thickness, however, renders TMDCs poor absorptivity. For this study, bilayer MoS2 is combined with core-only CdSe QDs and core/shell CdSe/ZnS QDs to obtain hybrids with increased light harvesting and exhibiting interfacial charge transfer (CT) and nonradiative energy transfer (NET), respectively. Field-effect transistors based on these hybrids and their responses to varying laser power and applied gate voltage are investigated with scanning photocurrent microscopy (SPCM) in view of their potential utilization in light harvesting and photodetector applications. CdSe–MoS2 hybrids are found to exhibit encouraging properties for photodetectors, like high responsivity and fast on/off response under low light exposure while CdSe/ZnS–MoS2 hybrids show enhanced charge carrier generation with increased light exposure, thus suitable for photovoltaics. While distinguishing optically between CT and NET in QD–TMDCs is nontrivial, it is found that they can be differentiated by SPCM as these two processes exhibit distinctive light-intensity dependencies: CT causes a photogating effect, decreasing the photocurrent response with increasing light power while NET increases the photocurrent response with increasing light power, opposite to CT case.},
doi = {10.1002/adfm.201707558},
journal = {Advanced Functional Materials},
number = 29,
volume = 28,
place = {United States},
year = {Thu May 17 00:00:00 EDT 2018},
month = {Thu May 17 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1002/adfm.201707558
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Cited by: 61 works
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Figures / Tables:

Figure 1 Figure 1: (a) QD-MoS2 hybrids with interfacial interaction dominated by CT (left) and by NET (right). (b) Left: energy band diagram for a CdSe-MoS2 hybrid showing electron and hole transfer as possible pathways from a photoexcited CdSe QD to MoS2; Right: energy band diagram for a CdSe/ZnS-MoS2 hybrid showing NETmore » as a possible pathway from a photoexcited type I CdSe/ZnS QD to MoS2 because the insulating ZnS shell acts as a tunneling barrier and inhibits CT from the CdSe core to MoS2. (c) Confocal FLIM images and spatially resolved PL decays from QD-MoS2 hybrids (red) and QDs on Si/SiO2 substrate (black) measured with 440 nm pulsed laser excitation and PL detection around 540- 580 nm. MoS2 flakes are indicated with dash black lines. PL decay fits according to a 2-exponent model are shown in green lines.« less
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    Observation of charge transfer in mixed-dimensional heterostructures formed by transition metal dichalcogenide monolayers and PbS quantum dots
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