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Title: Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films

Abstract

Here, the use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II–VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid–base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surfacemore » chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.« less

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. New Mexico State Univ., Las Cruces, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1459632
Report Number(s):
LA-UR-17-22680
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 19; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lin, Qianglu, Yun, Hyeong Jin, Liu, Wenyong, Song, Hyung -Jun, Makarov, Nikolay S., Isaienko, Oleksandr, Nakotte, Tom, Chen, Gen, Luo, Hongmei, Klimov, Victor Ivanovich, and Pietryga, Jeffrey Michael. Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films. United States: N. p., 2017. Web. doi:10.1021/jacs.7b01327.
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Lin, Qianglu, Yun, Hyeong Jin, Liu, Wenyong, Song, Hyung -Jun, Makarov, Nikolay S., Isaienko, Oleksandr, Nakotte, Tom, Chen, Gen, Luo, Hongmei, Klimov, Victor Ivanovich, & Pietryga, Jeffrey Michael. Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films. United States. https://doi.org/10.1021/jacs.7b01327
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Lin, Qianglu, Yun, Hyeong Jin, Liu, Wenyong, Song, Hyung -Jun, Makarov, Nikolay S., Isaienko, Oleksandr, Nakotte, Tom, Chen, Gen, Luo, Hongmei, Klimov, Victor Ivanovich, and Pietryga, Jeffrey Michael. Fri . "Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films". United States. https://doi.org/10.1021/jacs.7b01327. https://www.osti.gov/servlets/purl/1459632.
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@article{osti_1459632,
title = {Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films},
author = {Lin, Qianglu and Yun, Hyeong Jin and Liu, Wenyong and Song, Hyung -Jun and Makarov, Nikolay S. and Isaienko, Oleksandr and Nakotte, Tom and Chen, Gen and Luo, Hongmei and Klimov, Victor Ivanovich and Pietryga, Jeffrey Michael},
abstractNote = {Here, the use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II–VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid–base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surface chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.},
doi = {10.1021/jacs.7b01327},
journal = {Journal of the American Chemical Society},
number = 19,
volume = 139,
place = {United States},
year = {Fri Apr 21 00:00:00 EDT 2017},
month = {Fri Apr 21 00:00:00 EDT 2017}
}
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Publisher's Version of Record
https://doi.org/10.1021/jacs.7b01327
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Figures / Tables:

Figure 1 Figure 1: (a) Schematic diagram of the ligand exchange process, showing the transition from hydrophobic/steric to electrostatic stabilization. (b) Photographs of the ligand exchange and accompanying phase transfer of PbSe QDs from hexane (top) to DMF phase (bottom) using NH4I. (c) Absorption and emission spectra of PbS (4.0 nm, black),more » PbSe (4.0 nm, red), and PbTe (3.0 nm,blue) QDs before (solid) and after (dash) ligand exchange with LiI.« less
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