Fluorescence intermittency is a random switching between emitting (on) and non-emitting (off) periods found for many single chromophores such as semiconductor quantum dots and organic molecules. The statistics of the duration of on- and off-periods are commonly determined by thresholding the emission time trace of a single chromophore and appear to be power law distributed. Here we test with the help of simulations if the experimentally determined power law distributions can actually reflect the underlying statistics. We find that with the experimentally limited time resolution real power law statistics with exponents αon/off ≳ 1.6, especially if αon ≠ αoff would not be observed as such in the experimental data after binning and thresholding. Instead, a power law appearance could simply be obtained from the continuous distribution of intermediate intensity levels. This challenges much of the obtained data and the models describing the so-called power law blinking.
REFERENCES
1.
F.
Cichos
, C.
von Borczyskowski
, and M.
Orrit
, “Power-law intermittency of single emitters
,” Curr. Opin. Colloid Interface Sci.
12
, 272
(2007
).2.
P.
Frantsuzov
, M.
Kuno
, B.
Jankó
, and R. A.
Marcus
, “Universal emission intermittency in quantum dots, nanorods and nanowires
,” Nat. Phys.
4
, 519
(2008
).3.
J.
Zhao
, G.
Nair
, B. R.
Fisher
, and M. G.
Bawendi
, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking
,” Phys. Rev. Lett.
104
, 157403
(2010
).4.
S.
Rosen
, O.
Schwartz
, and D.
Oron
, “Transient fluorescence of the off state in blinking CdSe/CdS/ZnS semiconductor nanocrystals is not governed by auger recombination
,” Phys. Rev. Lett.
104
, 157404
(2010
).5.
A. W.
Cohn
, A. M.
Schimpf
, C. E.
Gunthardt
, and D. R.
Gamelin
, “Size-dependent trap-assisted auger recombination in semiconductor nanocrystals
,” Nano Lett.
13
, 1810
–1815
(2013
).6.
K.
Shimizu
, R.
Neuhauser
, C.
Leatherdale
, S.
Empedocles
, W.
Woo
, and M.
Bawendi
, “Blinking statistics in single semiconductor nanocrystal quantum dots
,” Phys. Rev. B
63
, 205316
(2001
).7.
L.
Li
, G.
Tian
, Y.
Luo
, H.
Brismar
, and Y.
Fu
, “Blinking, flickering, and correlation in fluorescence of single colloidal CdSe quantum dots with different shells under different excitations
,” J. Phys. Chem. C
117
, 4844
–4851
(2013
).8.
C.
Galland
, Y.
Ghosh
, A.
Steinbrück
, M.
Sykora
, J. A.
Hollingsworth
, V. I.
Klimov
, and H.
Htoon
, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
,” Nature
479
, 203
–207
(2011
).9.
W.
Qin
and P.
Guyot-Sionnest
, “Evidence for the role of holes in blinking: Negative and oxidized CdSe/CdS dots
,” ACS Nano
6
, 9125
–9132
(2012
).10.
M.
Kuno
, D. P.
Fromm
, H. F.
Hamann
, A.
Gallagher
, and D. J.
Nesbitt
, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior
,” J. Chem. Phys.
112
, 3117
(2000
).11.
R.
Verberk
, A.
van Oijen
, and M.
Orrit
, “Simple model for the power-law blinking of single semiconductor nanocrystals
,” Phys. Rev. B
66
, 233202
(2002
).12.
J.
Tang
and R. A.
Marcus
, “Mechanisms of fluorescence blinking in semiconductor nanocrystal quantum dots
,” J. Chem. Phys.
123
, 054704
(2005
).13.
M.
Pelton
, D. G.
Grier
, and P.
Guyot-Sionnest
, “Characterizing quantum-dot blinking using noise power spectra
,” Appl. Phys. Lett.
85
, 819
(2004
).14.
M.
Pelton
, G.
Smith
, N. F.
Scherer
, and R. A.
Marcus
, “Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots
,” PNAS
104
, 14249
(2007
).15.
J.
Tang
, D.-H.
Lee
, Y.-C.
Yeh
, and C.-T.
Yuan
, “Short-time power-law blinking statistics of single quantum dots and a test of the diffusion-controlled electron transfer model
,” J. Chem. Phys.
131
, 064506
(2009
).16.
L. P.
Watkins
and H.
Yang
, “Detection of intensity change points in time-resolved single-molecule measurements
,” J. Phys. Chem. B
109
, 617
(2005
).17.
K.
Zhang
, H.
Chang
, A.
Fu
, A. P.
Alivisatos
, and H.
Yang
, “Continuous distribution of emission states from single CdSe/ZnS quantum dots
,” Nano Lett.
6
, 843
(2006
).18.
R.
Schmidt
, C.
Krasselt
, and C.
von Borczyskowski
, “Change point analysis of matrix dependent photoluminescence intermittency of single CdSe/ZnS quantum dots with intermediate intensity levels
,” Chem. Phys.
406
, 9
(2012
).19.
M.
Lippitz
, F.
Kulzer
, and M.
Orrit
, “Statistical evaluation of single nano-object fluorescence
,” ChemPhysChem
6
, 770
(2005
).20.
C. H.
Crouch
, O.
Sauter
, X.
Wu
, R.
Purcell
, C.
Querner
, M.
Drndic
, and M.
Pelton
, “Facts and artifacts in the blinking statistics of semiconductor nanocrystals
,” Nano Lett.
10
, 1692
(2010
).21.
T. G.
Terentyeva
, H.
Engelkamp
, A. E.
Rowan
, T.
Komatsuzaki
, J.
Hofkens
, C.-B.
Li
, and K.
Blank
, “Dynamic disorder in single-enzyme experiments: Facts and artifacts
,” ACS Nano
6
, 346
–354
(2012
).22.
P. H.
Sher
, J. M.
Smith
, P. A.
Dalgarno
, R. J.
Warburton
, X.
Chen
, P. J.
Dobson
, S. M.
Daniels
, N. L.
Pickett
, and P.
O’Brien
, “Power law carrier dynamics in semiconductor nanocrystals at nanosecond timescales
,” Appl. Phys. Lett.
92
, 101111
(2008
).23.
F. D.
Stefani
, W.
Knoll
, M.
Kreiter
, X.
Zhong
, and M. Y.
Han
, “Quantification of photoinduced and spontaneous quantum-dot luminescence blinking
,” Phys. Rev. B
72
, 125304
(2005
).24.
I.
Chung
and M. G.
Bawendi
, “Relationship between single quantum-dot intermittency and fluorescence intensity decays from collections of dots
,” Phys. Rev. B
70
, 165304
(2004
).25.
M.
Kuno
, D.
Fromm
, S.
Johnson
, A.
Gallagher
, and D.
Nesbitt
, “Modeling distributed kinetics in isolated semiconductor quantum dots
,” Phys. Rev. B
67
, 125304
(2003
).26.
J. P.
Hoogenboom
, W. K.
den Otter
, and H. L.
Offerhaus
, “Accurate and unbiased estimation of power-law exponents from single-emitter blinking data
,” J. Chem. Phys.
125
, 204713
(2006
).27.
See supplementary material at http://dx.doi.org/10.1063/1.4868252 for estimations to the relative importance of unresolved events for different exponents, the analytical description of intensity histograms in the long bin time limit, as well as an estimation to the induced cut-off time by Poisson noise.
28.
R. T.
Sibatov
and V. V.
Uchaikin
, “Statistics of photocounts of blinking fluorescence of quantum dots
,” Opt. Spectrosc.
108
, 761
(2010
).29.
G.
Margolin
, V.
Protasenko
, M.
Kuno
, and E.
Barkai
, Fractals, Diffusion, and Relaxation in Disordered Complex Systems
, Advances in Chemical Physics
Vol. 133
, edited by W. T.
Coffey
and Y. P.
Kalmykov
(John Wiley and Sons, Inc.
, 2005
), p. 327
.30.
C.
Krasselt
, J.
Schuster
, and C.
von Borczyskowski
, “Photoinduced hole trapping in single semiconductor quantum dots at specific sites at silicon oxide interfaces
,” Phys. Chem. Chem. Phys.
13
, 17084
–17092
(2011
).31.
D.
Gómez
, J.
Van Embden
, P.
Mulvaney
, M.
Fernée
, and H.
Rubinsztein-Dunlop
, “Exciton- trion transitions in single CdSe–CdS Core–Shell nanocrystals
,” ACS Nano
3
, 2281
–2287
(2009
).32.
N.
Amecke
and F.
Cichos
, “Intermediate intensity levels during the emission intermittency of single CdSe/ZnS quantum dots
,” J. Lumin.
131
, 375
–378
(2011
).33.
A.
Biebricher
, M.
Sauer
, and P.
Tinnefeld
, “Radiative and nonradiative rate fluctuations of single colloidal semiconductor nanocrystals
,” J. Phys. Chem. B.
110
, 5174
–5178
(2006
).34.
W. G. J. H. M.
van Sark
, P. L. T. M.
Frederix
, A. A.
Bol
, H. C.
Gerritsen
, and A.
Meijerink
, “Blueing, bleaching, and blinking of single CdSe/ZnS quantum dots
,” ChemPhysChem
3
, 871
(2002
).35.
F.
Cichos
, J.
Martin
, and C.
von Borczyskowski
, “Emission intermittency in silicon nanocrystals
,” Phys. Rev. B
70
, 115314
(2004
).36.
E. A.
Riley
, C. M.
Hess
, P. J.
Whitham
, and P. J.
Reid
, “Beyond power laws: A new approach for analyzing single molecule photoluminescence intermittency
,” J. Chem. Phys.
136
, 184508
(2012
).37.
M. L.
Goldstein
, S. A.
Morris
, and G. G.
Yen
, “Problems with fitting to the power-law distribution
,” Eur. Phys. J. B
41
, 255
(2004
).38.
F. D.
Stefani
, X.
Zhong
, W.
Knoll
, M.
Han
, and M.
Kreiter
, “Memory in quantum-dot photoluminescence blinking
,” New J. Phys.
7
, 197
–197
(2005
).39.
A. A.
Cordones
, K. L.
Knappenberger
, and S. R.
Leone
, “Linking on-state memory and distributed kinetics in single nanocrystal blinking
,” J. Phys. Chem. B
117
, 4241
(2013
).© 2014 AIP Publishing LLC.
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