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

Marshall, Ashley R.; Beard, Matthew C.; Johnson, Justin C.

doi:10.1016/j.chemphys.2015.07.007

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

Journal Article · Sat Aug 01 00:00:00 EDT 2015 · Chemical Physics

DOI:https://doi.org/10.1016/j.chemphys.2015.07.007· OSTI ID:1370945

Marshall, Ashley R. ^[1]; Beard, Matthew C. ^[2]; Johnson, Justin C. ^[2]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-06NA25396; AC36-08GO28308

OSTI ID:: 1370945

Journal Information:: Chemical Physics, Vol. 471, 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; ISSN 0301-0104

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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Colloidal quantum dots for optoelectronics Litvin, A. P.; Martynenko, I. V.; Purcell-Milton, F. Journal of Materials Chemistry A, Vol. 5, Issue 26 https://doi.org/10.1039/c7ta02076g	journal	January 2017
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Title: Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films

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