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

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.7b01327· OSTI ID:1459632
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.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1459632
Report Number(s):
LA-UR--17-22680
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 19 Vol. 139; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (21)

Different Modes of Anion Response Cause Circulatory Phase Transfer of a Coordination Cage with Controlled Directionality journal September 2019
Colloidal Quantum Dot Inks for Single-Step-Fabricated Field-Effect Transistors: The Importance of Postdeposition Ligand Removal journal January 2018
Comparing Halide Ligands in PbS Colloidal Quantum Dots for Field-Effect Transistors and Solar Cells journal November 2018
Surface-Modified Substrates for Quantum Dot Inks in Printed Electronics journal February 2019
Ligands as a universal molecular toolkit in synthesis and assembly of semiconductor nanocrystals journal January 2020
Lead Selenide (PbSe) Colloidal Quantum Dot Solar Cells with >10% Efficiency journal June 2019
Enhancing Quantum Dot Solar Cells Stability with a Semiconducting Single‐Walled Carbon Nanotubes Interlayer Below the Top Anode journal October 2018
In Situ Fabricated Perovskite Nanocrystals: A Revolution in Optical Materials journal June 2018
Giant Photo‐Induced Current Enhancement in a Core–Shell‐Type Quantum‐Dot Thin Film journal January 2020
Different Modes of Anion Response Cause Circulatory Phase Transfer of a Coordination Cage with Controlled Directionality journal July 2019
Interfacial N→Sb Nonbonded Interaction Enhances the Photoelectronic Performance of PVP-Capped Sb 2 S 3 Amorphous Colloids journal August 2018
PbSe Quantum Dot Passivated Via Mixed Halide Perovskite Nanocrystals for Solar Cells With Over 9% Efficiency journal October 2018
Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2 journal September 2018
Highly photoluminescent, dense solid films from organic-capped CH 3 NH 3 PbBr 3 perovskite colloids journal January 2018
Enhanced mobility in PbS quantum dot films via PbSe quantum dot mixing for optoelectronic applications journal January 2019
Photoexcited carrier dynamics in colloidal quantum dot solar cells: insights into individual quantum dots, quantum dot solid films and devices journal January 2020
Colloidal PbS nanoplatelets synthesized via cation exchange for electronic applications journal January 2019
Pressure-enhanced electronic coupling of highly passivated quantum dot films to improve photovoltaic performance journal November 2019
Photophysical and electronic properties of bismuth-perovskite shelled lead sulfide quantum dots journal December 2019
PbE (E = S, Se) Colloidal Quantum Dot-Layered 2D Material Hybrid Photodetectors journal January 2020
Enhancing Quantum Dot Solar Cells Stability with a Semiconducting Single-Walled Carbon Nanotubes Interlayer Below the Top Anode text January 2018

Figures / Tables (6)


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