Sangam: A Confluence of Knowledge Streams

Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids

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dc.contributor Massachusetts Institute of Technology. Department of Chemical Engineering
dc.contributor Massachusetts Institute of Technology. Department of Materials Science and Engineering
dc.contributor Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
dc.contributor Massachusetts Institute of Technology. Department of Chemistry
dc.contributor Massachusetts Institute of Technology. Research Laboratory of Electronics
dc.creator Gilmore, Rachel Hoffman
dc.creator Liu, Yun
dc.creator Shcherbakov-Wu, Wenbi
dc.creator Dahod, Nabeel S.
dc.creator Lee, Elizabeth M.
dc.creator Weidman, Mark Clayton
dc.creator Li, Huashan
dc.creator Jean, Joel
dc.creator Bulovic, Vladimir
dc.creator Willard, Adam P.
dc.creator Grossman, Jeffrey C.
dc.creator Tisdale, William
dc.date 2020-09-21T18:13:44Z
dc.date 2020-09-21T18:13:44Z
dc.date 2019-07
dc.date 2019-05
dc.date 2020-09-10T11:56:52Z
dc.date.accessioned 2023-03-01T18:06:44Z
dc.date.available 2023-03-01T18:06:44Z
dc.identifier 2590-2385
dc.identifier https://hdl.handle.net/1721.1/127667
dc.identifier Gilmore, Rachel H. et al. "Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids." Matter 1, 1 (July 2019): P250-265 © 2019 Elsevier Inc
dc.identifier.uri http://localhost:8080/xmlui/handle/CUHPOERS/278791
dc.description We explore the dynamic interaction of charge carriers between band-edge states and sub-band trap states in PbS quantum dot (QD) solids using time-resolved spectroscopy. In monodisperse arrays of 4- to 5-nm diameter PbS QDs, we observe an optically active trap state ∼100–200 meV below the band edge that occurs at a frequency of 1 in ∼2,500 QDs. Uncoupled QD solids with oleic acid ligands show trap-to-ground-state recombination that resembles Auger recombination. In electronically coupled QD solids, we observe entropically driven uphill thermalization of trapped charge carriers from the trap state to the band edge via two distinct mechanisms: Auger-assisted charge transfer (∼35 ps) and thermally activated hopping (∼500 ps). Photophysical characterization combined with atomistic simulations and high-resolution electron microscopy suggest that these states arise from epitaxially fused pairs of QDs rather than electron or hole traps at the QD surface, offering new strategies for improving the optoelectronic performance of QD materials.
dc.description Department of Energy (DOE), Office of Basic Energy Sciences (Awards DE-SC0010538,DE-SC0019345)
dc.description National Science Foundation (Awards 1452857 and 1122374)
dc.format application/pdf
dc.language en
dc.publisher Elsevier BV
dc.relation http://dx.doi.org/10.1016/j.matt.2019.05.015
dc.relation Matter
dc.rights Creative Commons Attribution-NonCommercial-NoDerivs License
dc.rights http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.source chemRxiv
dc.title Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids
dc.type Article
dc.type http://purl.org/eprint/type/JournalArticle


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