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Title: Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films

Abstract

Using photoluminescence (PL) spectroscopy we investigate the radiative recombination pathways in PbS quantum dots (QDs) synthesized by two methods. We compare conventionally synthesized PbS from a PbO precursor to PbS synthesized using cation-exchange from CdS QDs. We show that strongly coupled films of PbS QDs from the cation-exchange luminesce with significant efficiency at room temperature. This is in stark contrast to conventional PbS QDs, which have exceedingly weak room temperature emission. Furthermore, the power dependence of the emission is quadratic, indicating bimolecular radiative recombination that is reasonably competitive with trap-assisted recombination, a feature previously unreported in coupled PbS QD films. We interpret these results in terms of a greatly reduced defect concentration for cation-exchanged QDs that mitigates the influence of trap-assisted recombination. Cation-exchanged QDs have recently been employed in highly efficient and air-stable lead chalcogenide QD devices, and the reduced number of trap states inferred here may lead to improved current collection and higher open circuit voltage.

Authors:
 [1];  [2];  [2]
+ Show Author Affiliations
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
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:
1370945
Grant/Contract Number:  
AC52-06NA25396; AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Physics
Additional Journal Information:
Journal Volume: 471; Journal Issue: C; Related Information: CASP partners with Los Alamos National Laboratory (lead); University of California, Irvine; University of Colorado; Colorado School of Mines; George Mason University; Los Alamos National Laboratory; University of Minnesota; National Renewable Energy Laboratory; Journal ID: ISSN 0301-0104
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Photoluminescence; PbS; Quantum dots; Nanocrystals; Bimolecular recombination

Citation Formats

Marshall, Ashley R., Beard, Matthew C., and Johnson, Justin C. Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films. United States: N. p., 2015. Web. doi:10.1016/j.chemphys.2015.07.007.
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Marshall, Ashley R., Beard, Matthew C., & Johnson, Justin C. Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films. United States. https://doi.org/10.1016/j.chemphys.2015.07.007
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Marshall, Ashley R., Beard, Matthew C., and Johnson, Justin C. Sat . "Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films". United States. https://doi.org/10.1016/j.chemphys.2015.07.007. https://www.osti.gov/servlets/purl/1370945.
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@article{osti_1370945,
title = {Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films},
author = {Marshall, Ashley R. and Beard, Matthew C. and Johnson, Justin C.},
abstractNote = {Using photoluminescence (PL) spectroscopy we investigate the radiative recombination pathways in PbS quantum dots (QDs) synthesized by two methods. We compare conventionally synthesized PbS from a PbO precursor to PbS synthesized using cation-exchange from CdS QDs. We show that strongly coupled films of PbS QDs from the cation-exchange luminesce with significant efficiency at room temperature. This is in stark contrast to conventional PbS QDs, which have exceedingly weak room temperature emission. Furthermore, the power dependence of the emission is quadratic, indicating bimolecular radiative recombination that is reasonably competitive with trap-assisted recombination, a feature previously unreported in coupled PbS QD films. We interpret these results in terms of a greatly reduced defect concentration for cation-exchanged QDs that mitigates the influence of trap-assisted recombination. Cation-exchanged QDs have recently been employed in highly efficient and air-stable lead chalcogenide QD devices, and the reduced number of trap states inferred here may lead to improved current collection and higher open circuit voltage.},
doi = {10.1016/j.chemphys.2015.07.007},
journal = {Chemical Physics},
number = C,
volume = 471,
place = {United States},
year = {Sat Aug 01 00:00:00 EDT 2015},
month = {Sat Aug 01 00:00:00 EDT 2015}
}
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Publisher's Version of Record
https://doi.org/10.1016/j.chemphys.2015.07.007
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    Works referencing / citing this record:

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