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Two-state theory of binned photon statistics for a large class of waiting time distributions and its application to quantum dot blinking

Volkán-Kacsó, Sándor (2014) Two-state theory of binned photon statistics for a large class of waiting time distributions and its application to quantum dot blinking. Journal of Chemical Physics, 140 (22). Art. No. 224110. ISSN 0021-9606. https://resolver.caltech.edu/CaltechAUTHORS:20140725-091614569

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Abstract

A theoretical method is proposed for the calculation of the photon counting probability distribution during a bin time. Two-state fluorescence and steady excitation are assumed. A key feature is a kinetic scheme that allows for an extensive class of stochastic waiting time distribution functions, including power laws, expanded as a sum of weighted decaying exponentials. The solution is analytic in certain conditions, and an exact and simple expression is found for the integral contribution of “bright” and “dark” states. As an application for power law kinetics, theoretical results are compared with experimental intensity histograms from a number of blinking CdSe/ZnS quantum dots. The histograms are consistent with distributions of intensity states around a “bright” and a “dark” maximum. A gap of states is also revealed in the more-or-less flat inter-peak region. The slope and to some extent the flatness of the inter-peak feature are found to be sensitive to the power-law exponents. Possible models consistent with these findings are discussed, such as the combination of multiple charging and fluctuating non-radiative channels or the multiple recombination center model. A fitting of the latter to experiment provides constraints on the interaction parameter between the recombination centers. Further extensions and applications of the photon counting theory are also discussed.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1063/1.4881460DOIArticle
http://scitation.aip.org/content/aip/journal/jcp/140/22/10.1063/1.4881460PublisherArticle
Additional Information:© 2014 AIP Publishing LLC. Received 27 February 2014; accepted 22 May 2014; published online 12 June 2014. The author would like to thank Dr. R. A. Marcus, Dr. B. Jankó, Dr. P. A. Frantsuzov, Dr. A. Szabo, and Dr. M. Kuno for fruitful discussions and valuable advice. Support by grants from the James W. Glanville Foundation at the California Institute of Technology, the Office of Naval Research, and the Army Research Office are gratefully acknowledged. The author feels indebted to Dr. M. Kuno for sharing a large number of trajectories.
Funders:
Funding AgencyGrant Number
James W. Glanville FoundationUNSPECIFIED
Office of Naval Research (ONR)UNSPECIFIED
Army Research Office (ARO)UNSPECIFIED
Issue or Number:22
Record Number:CaltechAUTHORS:20140725-091614569
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140725-091614569
Official Citation:Two-state theory of binned photon statistics for a large class of waiting time distributions and its application to quantum dot blinking Volkán-Kacsó, Sándor, The Journal of Chemical Physics, 140, 224110 (2014), DOI:http://dx.doi.org/10.1063/1.4881460
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:47493
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:25 Jul 2014 17:17
Last Modified:03 Oct 2019 06:54

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