Universality of the Fluorescence Intermittency in Nanoscale Systems: Experiment and Theory
Abstract
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.
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.Attached Files
Published - nl3035674.pdf
Supplemental Material - nl3035674_si_001.pdf
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Additional details
- Eprint ID
- 37612
- Resolver ID
- CaltechAUTHORS:20130325-134831185
- Institute for Theoretical Sciences
- Department of Energy (DOE) Basic Energy Sciences
- ECS-0609249
- NSF-NIRT
- Created
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2013-03-25Created from EPrint's datestamp field
- Updated
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2021-11-09Created from EPrint's last_modified field