Direct Observation of Rapid Discrete Spectral Dynamics in Single Colloidal CdSe-CdS Core-Shell Quantum Dots

We measure the anomalous spectral diffusion of single colloidal quantum dots over eight temporal decades simultaneously by combining single-molecule spectroscopy and photon-correlation Fourier spectroscopy. Our technique distinguishes between discrete and continuous dynamics and directly reveals tha...

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Bibliographic Details
Main Authors: Marshall, Lisa F., Cui, Jian, Brokmann, Xavier, Bawendi, Moungi G., Beyler, Andrew Paul
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: American Physical Society 2014
Online Access:http://hdl.handle.net/1721.1/84957
https://orcid.org/0000-0003-2220-4365
https://orcid.org/0000-0002-5613-8928
Description
Summary:We measure the anomalous spectral diffusion of single colloidal quantum dots over eight temporal decades simultaneously by combining single-molecule spectroscopy and photon-correlation Fourier spectroscopy. Our technique distinguishes between discrete and continuous dynamics and directly reveals that the quasicontinuous spectral diffusion observed using conventional spectroscopy is composed of rapid, discrete spectral jumps. Despite their multiple time scales, these dynamics can be captured by a single mechanism whose parameters vary widely between dots and over time in individual dots.