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dc.contributor.author
du Fossé, Indy
dc.contributor.author
Boehme, Simon C.
dc.contributor.author
Infante, Ivan
dc.contributor.author
Houtepen, Arjan J.
dc.date.accessioned
2021-06-16T11:20:36Z
dc.date.available
2021-06-11T02:26:12Z
dc.date.available
2021-06-16T11:20:36Z
dc.date.issued
2021-05-11
dc.identifier.issn
0897-4756
dc.identifier.other
10.1021/acs.chemmater.1c00561
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/489164
dc.description.abstract
Trap states play a crucial role in the design of colloidal quantum dot (QD)-based technologies. The presence of these in-gap states can either significantly limit the efficiency of devices (e.g., in solar cells or LEDs) or play a pivotal role in the functioning of the technology (e.g., in catalysis). Understanding the atomistic nature of traps is therefore of the highest importance. Although the mechanism through which undercoordinated chalcogenide atoms can lead to trap states in II–VI QDs is generally well understood, the nature of metal-based traps remains more elusive. Previous research has shown that reduction of metal sites in negatively charged QDs can lead to in-gap states. Here, we use density functional theory to show that metal-based traps are also formed in charge-neutral but photoexcited CdSe QDs. It is found that Cd–Cd dimers and the concomitant trap states are transient in nature and appear and disappear on the picosecond time scale. Subsequent nonradiative recombination from the trap is shown to be much faster than radiative recombination, indicating that dimer-related trap states can quench the photoluminescence. These results are expected to be transferable to other II–VI materials and highlight the importance of surface redox reactions for the optical properties of QDs. Moreover, they show that photoexcitation can lead to atomic rearrangements on the surface and thus create transient in-gap states.
en_US
dc.language.iso
en
en_US
dc.publisher
American Chemical Society
en_US
dc.title
Dynamic Formation of Metal-Based Traps in Photoexcited Colloidal Quantum Dots and Their Relevance for Photoluminescence
en_US
dc.type
Journal Article
dc.date.published
2021-04-21
ethz.journal.title
Chemistry of Materials
ethz.journal.volume
33
en_US
ethz.journal.issue
9
en_US
ethz.journal.abbreviated
Chem. Mater.
ethz.pages.start
3349
en_US
ethz.pages.end
3358
en_US
ethz.identifier.wos
ethz.identifier.scopus
ethz.publication.place
Washington, DC
en_US
ethz.publication.status
published
en_US
ethz.date.deposited
2021-06-11T02:26:16Z
ethz.source
SCOPUS
ethz.eth
yes
en_US
ethz.availability
Metadata only
en_US
ethz.rosetta.installDate
2021-06-16T11:20:46Z
ethz.rosetta.lastUpdated
2021-06-16T11:20:46Z
ethz.rosetta.exportRequired
true
ethz.rosetta.versionExported
true
ethz.COinS
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