Unraveling the Emission Pathways in Copper Indium Sulfide Quantum Dots
Semiconductor copper indium sulfide quantum dots are emerging as promising alternatives to cadmium- and lead-based chalcogenides in solar cells, luminescent solar concentrators, and deep-tissue bioimaging due to their inherently lower toxicity and outstanding photoluminescence properties. However, t...
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| Published in | ACS nano Vol. 15; no. 11; pp. 17573 - 17581 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
23.11.2021
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1936-0851 1936-086X 1936-086X |
| DOI | 10.1021/acsnano.1c04909 |
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| Abstract | Semiconductor copper indium sulfide quantum dots are emerging as promising alternatives to cadmium- and lead-based chalcogenides in solar cells, luminescent solar concentrators, and deep-tissue bioimaging due to their inherently lower toxicity and outstanding photoluminescence properties. However, the nature of their emission pathways remains a subject of debate. Using low-temperature single quantum dot spectroscopy on core–shell copper indium sulfide nanocrystals, we observe two subpopulations of particles with distinct spectral features. The first class shows sharp resolution-limited emission lines that are attributed to zero-phonon recombination lines of a long-lived band-edge exciton. Such emission results from the perfect passivation of the copper indium sulfide core by the zinc sulfide shell and points to an inversion in the band-edge hole levels. The second class exhibits ultrabroad spectra regardless of the temperature, which is a signature of the extrinsic self-trapping of the hole assisted by defects in imperfectly passivated quantum dots. |
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| AbstractList | Semiconductor copper indium sulfide quantum dots are emerging as promising alternatives to cadmium- and lead-based chalcogenides in solar cells, luminescent solar concentrators, and deep-tissue bioimaging due to their inherently lower toxicity and outstanding photoluminescence properties. However, the nature of their emission pathways remains a subject of debate. Using low-temperature single quantum dot spectroscopy on core-shell copper indium sulfide nanocrystals, we observe two subpopulations of particles with distinct spectral features. The first class shows sharp resolution-limited emission lines that are attributed to zero-phonon recombination lines of a long-lived band-edge exciton. Such emission results from the perfect passivation of the copper indium sulfide core by the zinc sulfide shell and points to an inversion in the band-edge hole levels. The second class exhibits ultrabroad spectra regardless of the temperature, which is a signature of the extrinsic self-trapping of the hole assisted by defects in imperfectly passivated quantum dots.Semiconductor copper indium sulfide quantum dots are emerging as promising alternatives to cadmium- and lead-based chalcogenides in solar cells, luminescent solar concentrators, and deep-tissue bioimaging due to their inherently lower toxicity and outstanding photoluminescence properties. However, the nature of their emission pathways remains a subject of debate. Using low-temperature single quantum dot spectroscopy on core-shell copper indium sulfide nanocrystals, we observe two subpopulations of particles with distinct spectral features. The first class shows sharp resolution-limited emission lines that are attributed to zero-phonon recombination lines of a long-lived band-edge exciton. Such emission results from the perfect passivation of the copper indium sulfide core by the zinc sulfide shell and points to an inversion in the band-edge hole levels. The second class exhibits ultrabroad spectra regardless of the temperature, which is a signature of the extrinsic self-trapping of the hole assisted by defects in imperfectly passivated quantum dots. Semiconductor copper indium sulfide quantum dots are emerging as promising alternatives to cadmium- and lead-based chalcogenides in solar cells, luminescent solar concentrators, and deep-tissue bioimaging due to their inherently lower toxicity and outstanding photoluminescence properties. However, the nature of their emission pathways remains a subject of debate. Using low-temperature single quantum dot spectroscopy on core–shell copper indium sulfide nanocrystals, we observe two subpopulations of particles with distinct spectral features. The first class shows sharp resolution-limited emission lines that are attributed to zero-phonon recombination lines of a long-lived band-edge exciton. Such emission results from the perfect passivation of the copper indium sulfide core by the zinc sulfide shell and points to an inversion in the band-edge hole levels. The second class exhibits ultrabroad spectra regardless of the temperature, which is a signature of the extrinsic self-trapping of the hole assisted by defects in imperfectly passivated quantum dots. |
| Author | Hou, Lei Meeldijk, Johannes D de Mello Donega, Celso Busatto, Serena Tamarat, Philippe Lounis, Brahim Xia, Chenghui |
| AuthorAffiliation | Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science LP2N Electron Microscopy Utrecht, Debye Institute for Nanomaterials Science Institut d’Optique and CNRS Utrecht University |
| AuthorAffiliation_xml | – name: Electron Microscopy Utrecht, Debye Institute for Nanomaterials Science – name: Condensed Matter and Interfaces, Debye Institute for Nanomaterials Science – name: Institut d’Optique and CNRS – name: LP2N – name: Utrecht University |
| Author_xml | – sequence: 1 givenname: Chenghui orcidid: 0000-0001-5087-8805 surname: Xia fullname: Xia, Chenghui organization: Institut d’Optique and CNRS – sequence: 2 givenname: Philippe surname: Tamarat fullname: Tamarat, Philippe organization: Institut d’Optique and CNRS – sequence: 3 givenname: Lei surname: Hou fullname: Hou, Lei organization: Institut d’Optique and CNRS – sequence: 4 givenname: Serena surname: Busatto fullname: Busatto, Serena organization: Utrecht University – sequence: 5 givenname: Johannes D surname: Meeldijk fullname: Meeldijk, Johannes D organization: Electron Microscopy Utrecht, Debye Institute for Nanomaterials Science – sequence: 6 givenname: Celso orcidid: 0000-0002-4403-3627 surname: de Mello Donega fullname: de Mello Donega, Celso organization: Utrecht University – sequence: 7 givenname: Brahim orcidid: 0000-0001-7501-0236 surname: Lounis fullname: Lounis, Brahim email: brahim.lounis@u-bordeaux.fr organization: Institut d’Optique and CNRS |
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| Title | Unraveling the Emission Pathways in Copper Indium Sulfide Quantum Dots |
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