Understanding the Bias Introduced in Quantum Dot Blinking Using Change Point Analysis

The fluorescence intermittency of single CdSe/CdS quantum dots (QDs) with different shell sizes is studied using the conventional bin and threshold method and the statistically more rigorous method, change point analysis (CPA). The on-state truncation time (τc) is a critical value used to interpret the dynamics of charge trapping in single QDs; however, changing the bin size and threshold in blink traces significantly modifies τc. Herein, we use the CPA method to minimize the bias that binning and thresholding introduces and find that a widely used assumption that there is only one on and one off state is questionable. We observe that 12 out of 17 QDs exhibit more than two intensity levels and find that the τc values of individual levels differ from the values obtained when the levels are combined, i.e., when one assumes there is only one on and one off state as in the conventional bin and threshold method. For instance, one QD has τc values of 0.5 (0.1) and 2.0 (0.2) s from two different intensity levels...

[1]  Charge-tunnelling and self-trapping: common origins for blinking, grey-state emission and photoluminescence enhancement in semiconductor quantum dots. , 2016, Nanoscale.

[2]  F. Kulzer,et al.  Autocorrelation analysis for the unbiased determination of power-law exponents in single-quantum-dot blinking. , 2014, ACS Nano.

[3]  S. Volkán-Kacsó Two-state theory of binned photon statistics for a large class of waiting time distributions and its application to quantum dot blinking. , 2014, The Journal of chemical physics.

[4]  D. Oron,et al.  Studying quantum dot blinking through the addition of an engineered inorganic hole trap. , 2013, ACS nano.

[5]  S. Leone,et al.  Mechanisms for charge trapping in single semiconductor nanocrystals probed by fluorescence blinking. , 2013, Chemical Society reviews.

[6]  Ou Chen,et al.  Compact high-quality CdSe-CdS core-shell nanocrystals with narrow emission linewidths and suppressed blinking. , 2013, Nature materials.

[7]  P. Guyot-Sionnest,et al.  Evidence for the role of holes in blinking: negative and oxidized CdSe/CdS dots. , 2012, ACS nano.

[8]  C. Galland,et al.  Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots , 2011, Nature.

[9]  O. Sauter,et al.  Facts and artifacts in the blinking statistics of semiconductor nanocrystals. , 2010, Nano letters.

[10]  H. Rubinsztein-Dunlop,et al.  Exciton-trion transitions in single CdSe-CdS core-shell nanocrystals. , 2009, ACS nano.

[11]  P. Frantsuzov,et al.  Model of fluorescence intermittency of single colloidal semiconductor quantum dots using multiple recombination centers. , 2009, Physical review letters.

[12]  B. Dubertret,et al.  Bright and grey states in CdSe-CdS nanocrystals exhibiting strongly reduced blinking. , 2009, Physical review letters.

[13]  D. Nesbitt,et al.  Modified power law behavior in quantum dot blinking: a novel role for biexcitons and auger ionization. , 2009, Nano letters.

[14]  R. Marcus,et al.  Universal emission intermittency in quantum dots, nanorods and nanowires , 2008, 0810.2509.

[15]  R. Marcus,et al.  Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots , 2007, Proceedings of the National Academy of Sciences.

[16]  A. Szabó,et al.  Theory of the statistics of kinetic transitions with application to single-molecule enzyme catalysis. , 2006, The Journal of chemical physics.

[17]  A. Alivisatos,et al.  Continuous distribution of emission states from single CdSe/ZnS quantum dots. , 2006, Nano letters.

[18]  Lucas P. Watkins,et al.  Detection of intensity change points in time-resolved single-molecule measurements. , 2005, The journal of physical chemistry. B.

[19]  Moungi G. Bawendi,et al.  Relationship between single quantum-dot intermittency and fluorescence intensity decays from collections of dots , 2004 .

[20]  P. Guyot-Sionnest,et al.  Characterizing quantum-dot blinking using noise power spectra , 2004, cond-mat/0404589.

[21]  M. Bawendi,et al.  Emission Intensity Dependence and Single-Exponential Behavior In Single Colloidal Quantum Dot Fluorescence Lifetimes , 2004 .

[22]  Haw Yang,et al.  Probing single-molecule dynamics photon by photon , 2002 .

[23]  Michel Orrit,et al.  Simple model for the power-law blinking of single semiconductor nanocrystals , 2002 .

[24]  M Dahan,et al.  Bunching and antibunching in the fluorescence of semiconductor nanocrystals. , 2001, Optics letters.

[25]  Robert Neuhauser,et al.  Blinking statistics in single semiconductor nanocrystal quantum dots , 2001 .