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Universality of the Fluorescence Intermittency in Nanoscale Systems: Experiment and Theory

Frantsuzov, Pavel A. and Volkán-Kacsó, Sándor and Jankó, Boldizsár (2013) Universality of the Fluorescence Intermittency in Nanoscale Systems: Experiment and Theory. Nano Letters, 13 (2). pp. 402-408. ISSN 1530-6984.

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A variety of optically active nanoscale objects show extremely long correlations in the fluctuations of fluorescence intensity (blinking). Here we performed a systematic study to quantitatively estimate the power spectral density (PSD) of the fluorescence trajectories of colloidal and self-assembled quantum dots (QDs), nanorods (NRs), nanowires (NWs), and organic molecules. We report for the first time a statistically correct method of PSD estimation suitable for these systems. Our method includes a detailed analysis of the confidence intervals. The striking similarity in the spectra of these nanoscale systems, including even a “nonblinking” quantum dot investigated by Wang and collaborators (Nature2009, 459, 685–689), is powerful evidence for the existence of a universal physical mechanism underlying the blinking phenomenon in all of these fluorophores (Frantsuzov et al. Nat. Phys.2008, 4, 519–522). In this paper we show that the features of this universal mechanism can be captured phenomenologically by the multiple recombination center model (MRC) we suggested recently for explaining single colloidal QD intermittency. Within the framework of the MRCs we qualitatively explain all of the important features of fluorescence intensity fluctuations for a broad spectrum of nanoscale emitters.

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Additional Information:© 2012 American Chemical Society. Received: September 25, 2012; Revised: December 17, 2012; Published: December 31, 2012. The authors would like to thank Drs. C. Crouch, M. Drndic, D. Gomez, J. Hoogenboom, T. Krauss, M. Kuno, R. Loomis, P. Mulvaney, M. Pelton, V. Protasenko, and M. Sugisaki for kindly sharing their experimental data with us. We would also like to acknowledge the support of the Institute for Theoretical Sciences, the Department of Energy, Basic Energy Sciences, and the National Science Foundation via the NSF-NIRT Grant No. ECS-0609249.
Funding AgencyGrant Number
Institute for Theoretical SciencesUNSPECIFIED
Department of Energy (DOE) Basic Energy SciencesUNSPECIFIED
Subject Keywords:Blinking; quantum dot; nanorod; nanowire; organic dye; recombination centers
Issue or Number:2
Record Number:CaltechAUTHORS:20130325-134831185
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Official Citation:Universality of the Fluorescence Intermittency in Nanoscale Systems: Experiment and Theory Pavel A. Frantsuzov, Sándor Volkán-Kacsó, and Boldizsár Jankó Nano Letters201313 (2), 402-408
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:37612
Deposited By: Tony Diaz
Deposited On:25 Mar 2013 21:29
Last Modified:03 Oct 2019 04:49

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