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PredicateObject
rdf:type
lifeskim:mentions
pubmed:issue
6
pubmed:dateCreated
2011-6-28
pubmed:abstractText
We conduct measurements of photocharging of PbSe and PbS nanocrystal quantum dots (NQDs) as a function of excitation energy (??). We observe a rapid growth of the degree of photocharging with increasing ??, which indicates an important role of hot-carrier transfer in the photoionization process. The corresponding spectral dependence exhibits two thresholds that mark the onsets of weak and strong photocharging. Interestingly, both thresholds are linked to the NQD band gap energy (E(g)) and scale as ?1.5E(g) and ?3E(g), indicating that the onsets of photoionization are associated with specific nanocrystal states (tentatively, 1P and 2P, respectively) and are not significantly dependent on the energy of external acceptor sites. For all samples, the hot-electron transfer probability increases by nearly 2 orders of magnitude as photon energy increases from 1.5 to 3.5 eV, although at any given wavelength the photoionization probability shows significant sample-to-sample variations (?10(-6) to 10(-3) for 1.5 eV and ?10(-4) to 10(-1) for 3.5 eV). In addition to the effect of the NQD size, these variations are likely due to differences in the properties of the NQD surface and/or the number and identity of external acceptor trap sites. The charge-separated states produced by photoionization are characterized by extremely long lifetimes (20 to 85 s) that become longer with increasing NQD size.
pubmed:language
eng
pubmed:journal
pubmed:citationSubset
IM
pubmed:chemical
pubmed:status
MEDLINE
pubmed:month
Jun
pubmed:issn
1936-086X
pubmed:author
pubmed:issnType
Electronic
pubmed:day
28
pubmed:volume
5
pubmed:owner
NLM
pubmed:authorsComplete
Y
pubmed:pagination
5045-55
pubmed:meshHeading
pubmed:year
2011
pubmed:articleTitle
Spectral dependence of nanocrystal photoionization probability: the role of hot-carrier transfer.
pubmed:affiliation
Center for Advanced Solar Photophysics, C-PCS, Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.
pubmed:publicationType
Journal Article, Research Support, U.S. Gov't, Non-P.H.S.