Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids
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 t...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Elsevier BV
2020
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| Online Access: | https://hdl.handle.net/1721.1/127667 |
| _version_ | 1811069686513664000 |
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| author | Gilmore, Rachel Hoffman Liu, Yun Shcherbakov-Wu, Wenbi Dahod, Nabeel S. Lee, Elizabeth M. Weidman, Mark Clayton Li, Huashan Jean, Joel Bulovic, Vladimir Willard, Adam P. Grossman, Jeffrey C. Tisdale, William |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Gilmore, Rachel Hoffman Liu, Yun Shcherbakov-Wu, Wenbi Dahod, Nabeel S. Lee, Elizabeth M. Weidman, Mark Clayton Li, Huashan Jean, Joel Bulovic, Vladimir Willard, Adam P. Grossman, Jeffrey C. Tisdale, William |
| author_sort | Gilmore, Rachel Hoffman |
| collection | MIT |
| 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. |
| first_indexed | 2024-09-23T08:14:09Z |
| format | Article |
| id | mit-1721.1/127667 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T08:14:09Z |
| publishDate | 2020 |
| publisher | Elsevier BV |
| record_format | dspace |
| spelling | mit-1721.1/1276672022-09-30T08:31:20Z Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids Gilmore, Rachel Hoffman Liu, Yun Shcherbakov-Wu, Wenbi Dahod, Nabeel S. Lee, Elizabeth M. Weidman, Mark Clayton Li, Huashan Jean, Joel Bulovic, Vladimir Willard, Adam P. Grossman, Jeffrey C. Tisdale, William Massachusetts Institute of Technology. Department of Chemical Engineering Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Research Laboratory of Electronics 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. Department of Energy (DOE), Office of Basic Energy Sciences (Awards DE-SC0010538,DE-SC0019345) National Science Foundation (Awards 1452857 and 1122374) 2020-09-21T18:13:44Z 2020-09-21T18:13:44Z 2019-07 2019-05 2020-09-10T11:56:52Z Article http://purl.org/eprint/type/JournalArticle 2590-2385 https://hdl.handle.net/1721.1/127667 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 en http://dx.doi.org/10.1016/j.matt.2019.05.015 Matter Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Elsevier BV chemRxiv |
| spellingShingle | Gilmore, Rachel Hoffman Liu, Yun Shcherbakov-Wu, Wenbi Dahod, Nabeel S. Lee, Elizabeth M. Weidman, Mark Clayton Li, Huashan Jean, Joel Bulovic, Vladimir Willard, Adam P. Grossman, Jeffrey C. Tisdale, William Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title | Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title_full | Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title_fullStr | Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title_full_unstemmed | Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title_short | Epitaxial Dimers and Auger-Assisted Detrapping in PbS Quantum Dot Solids |
| title_sort | epitaxial dimers and auger assisted detrapping in pbs quantum dot solids |
| url | https://hdl.handle.net/1721.1/127667 |
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