Spontaneous Spectral Diffusion in CdSe Quantum Dots

Spectral diffusion of the emission line of single colloidal nanocrystals is generally regarded as a random process. Here, we show that each new spectral position has a finite memory of previous spectral positions, as evidenced by persistent anticorrelations in time series of spectral jumps. The anti...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2012-06, Vol.3 (12), p.1716-1720
Main Authors: Fernée, Mark J, Plakhotnik, Taras, Louyer, Yann, Littleton, Bradley N, Potzner, Christian, Tamarat, Philippe, Mulvaney, Paul, Lounis, Brahim
Format: Article
Language:English
Subjects:
Condensed Matter
Other
Physical Processes in Nanomaterials and Nanostructures
Physics
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Summary:Spectral diffusion of the emission line of single colloidal nanocrystals is generally regarded as a random process. Here, we show that each new spectral position has a finite memory of previous spectral positions, as evidenced by persistent anticorrelations in time series of spectral jumps. The anticorrelation indicates that there is an enhanced probability of the charge distribution around the nanocrystal returning to a previous configuration. We show both statistically and directly that this memory manifests as an observable spontaneous “relaxation” in the absence of a pump laser, so that spectral diffusion progresses in a manner of “two steps forward and one step back”.
ISSN:1948-7185
1948-7185
DOI:10.1021/jz300456h