期刊
NANO LETTERS
卷 12, 期 6, 页码 3031-3037出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl3008659
关键词
Giant nanocrystal quantum dot (g-NQD); stable red phosphor; self-reabsorption; Stokes shift; down-conversion light-emitting device
类别
资金
- Los Alamos National Laboratory Directed Research and Development (LDRD)
- Single Investigator Small Group [2009LANL1096]
- Office of Basic Energy Sciences (OBES), Office of Science (OS), U.S. Department of Energy (DOE)
- Center for Integrated Nanotechnologies (CINT)
A new class of nanocrystal quantum dot (NQD), the giant NQD (g-NQD), was investigated for its potential to address outstanding issues associated with the use of NQDs as down-conversion phosphors in light-emitting devices, namely, insufficient chemical/photostability and extensive self-reabsorption when packed in high densities or in thick films. Here, we demonstrate that g-NQDs afford significantly enhanced operational stability compared to their conventional NQD counterparts and minimal self-reabsorption losses. The latter results from a characteristic large Stokes shift (>100 nm; >0.39 eV), which itself is a manifestation of the internal structure of these uniquely thick-shelled NQDs. In carefully prepared g-NQDs, light absorption occurs predominantly in the shell but emission occurs exclusively from the core. We directly compare for the first time the processes of shell -> core energy relaxation and core -> core energy transfer by evaluating CdS -> CdSe down-conversion of blue -> red light in g-NQDs and in a comparable mixed-NQD (CdSe and CdS) thin film, revealing that the internal energy relaxation process affords a more efficient and color-pure conversion of blue to red light compared to energy transfer. Lastly, we demonstrate the facile fabrication of white-light devices with correlated color temperature tuned from similar to 3200 to 5800 K.
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