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Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

ABSTRACT: Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an important constraint on possible mechanisms for the blinking. In particular, the observations are consistent with the predictions of models wherein blinking is controlled by diffusion of the energies of electron or hole trap states.

SUBMITTER: Pelton M

PROVIDER: S-EPMC1964845 | biostudies-other | 2007 Sep

REPOSITORIES: biostudies-other

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Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

Pelton Matthew M Smith Glenna G Scherer Norbert F NF Marcus Rudolph A RA

Proceedings of the National Academy of Sciences of the United States of America 20070824 36

Fluorescence blinking in nanocrystal quantum dots is known to exhibit power-law dynamics, and several different mechanisms have been proposed to explain this behavior. We have extended the measurement of quantum-dot blinking by characterizing fluctuations in the fluorescence of single dots over time scales from microseconds to seconds. The power spectral density of these fluctuations indicates a change in the power-law statistics that occurs at a time scale of several milliseconds, providing an ...[more]

PMID: 17720807

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Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

Dataset Information

Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

Publications

Evidence for a diffusion-controlled mechanism for fluorescence blinking of colloidal quantum dots.

Similar Datasets

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