Direct Measurement of Off-State Trapping Rate Fluctuations in Single Quantum Dot Fluorescence

Cordones, Amy A.; Bixby, Teresa J.; Leone, Stephen R.

doi:10.1021/nl2017674

Cited by 42 publications

(55 citation statements)

References 26 publications

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“…Indeed, the present findings contribute to the growing body of evidence supporting a multi-state picture of blinking. 3, 13, 32, 37-39 Emission lifetime measurements in CdSe/ZnS QDs have demonstrated that the off state can be further resolved into a manifold of states 38,39 which is consistent with the evidence indicating a distribution of dark intensity states (Fig. 2).…”

Section: Implications Of the Distributed States On Models Of Blinkingsupporting

confidence: 67%

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

Volkan-Kacso

2014

The Journal of Chemical Physics

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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. © 2014 AIP Publishing LLC. [http://dx

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Section: Implications Of the Distributed States On Models Of Blinkingsupporting

confidence: 67%

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

Volkan-Kacso

2014

The Journal of Chemical Physics

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“…On the other hand, PL blinking linked to mechanisms other than Auger recombination, 60,62,63 resulting only in minor changes in PL decay, has also been reported and attributed to “electron-accepting surface sites” 60 or charge carrier traps that are associated with the surface of quantum dots where coordination of ions is incomplete. 61,62 Therefore, the observation of minor changes of PL decay alongside OHP nanorods PL blinking in this study is likely related to surface defects or surface charge trap sites, similar to their semiconductor quantum dot counterparts.…”

Section: Results and Discussionmentioning

confidence: 99%

Photoluminescence Blinking of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods Induced by Surface Traps

et al. 2016

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Photoluminescence (PL) of organometal halide perovskite materials reflects the charge dynamics inside of the material and thus contains important information for understanding the electro-optical properties of the material. Interpretation of PL blinking of methylammonium lead iodide (MAPbI3) nanostructures observed on polycrystalline samples remains puzzling owing to their intrinsic disordered nature. Here, we report a novel method for the synthesis of high-quality single-crystal MAPbI3 nanorods and demonstrate a single-crystal study on MAPbI3 PL blinking. At low excitation power densities, two-state blinking was found on individual nanorods with dimensions of several hundred nanometers. A super-resolution localization study on the blinking of individual nanorods showed that single crystals of several hundred nanometers emit and blink as a whole, without showing changes in the localization center over the crystal. Moreover, both the blinking ON and OFF times showed power-law distributions, indicating trapping–detrapping processes. This is further supported by the PL decay times of the individual nanorods, which were found to correlate with the ON/OFF states. Furthermore, a strong environmental dependence of the nanorod PL blinking was revealed by comparing the measurements in vacuum, nitrogen, and air, implying that traps locate close to crystal surfaces. We explain our observations by proposing surface charge traps that are likely related to under-coordinated lead ions and methylammonium vacancies to result in the PL blinking observed here.

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“…Section 2.9) it decreases the quantum yield of ensemble measurements 173. The investigation of fluorescence flickering in these materials is of ongoing interest with several current models 174. Another problem for bioapplications is the often increased overall QD diameter of up to 30 nm after surface functionalization for stability and biocompatibility reasons.…”

Section: Fluorophores For Nanobiotechnologymentioning

confidence: 99%

“…[ 173 ] The investigation of fl uorescence fl ickering in these materials is of ongoing interest with several current models. [ 174 ] Another problem for bioapplications is the often increased overall QD diameter of up to 30 nm after surface functionalization for stability and biocompatibility reasons. This can alter the functions and dynamics of conjugated biomolecules with similar or smaller dimensions.…”

Section: Semiconductor Quantum Dotsmentioning

confidence: 99%

Fluorescence in Nanobiotechnology: Sophisticated Fluorophores for Novel Applications

Hötzer

Medintz

Hildebrandt

2012

Small

192

121

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Nanobiotechnology is one of the fastest growing and broadest-ranged interdisciplinary subfields of the nanosciences. Countless hybrid bio-inorganic composites are currently being pursued for various uses, including sensors for medical and diagnostic applications, light- and energy-harvesting devices, along with multifunctional architectures for electronics and advanced drug-delivery. Although many disparate biological and nanoscale materials will ultimately be utilized as the functional building blocks to create these devices, a common element found among a large proportion is that they exert or interact with light. Clearly continuing development will rely heavily on incorporating many different types of fluorophores into these composite materials. This review covers the growing utility of different classes of fluorophores in nanobiotechnology, from both a photophysical and a chemical perspective. For each major structural or functional class of fluorescent probe, several representative applications are provided, and the necessary technological background for acquiring the desired nano-bioanalytical information are presented.

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Direct Measurement of Off-State Trapping Rate Fluctuations in Single Quantum Dot Fluorescence

Cited by 42 publications

References 26 publications

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

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

Photoluminescence Blinking of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods Induced by Surface Traps

Fluorescence in Nanobiotechnology: Sophisticated Fluorophores for Novel Applications

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