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Polarons Explain Luminescence Behavior of Colloidal Quantum Dots at Low Temperature.

ABSTRACT: Luminescence properties of colloidal quantum dots have found applications in imaging, displays, light-emitting diodes and lasers, and single photon sources. Despite wide interest, several experimental observations in low-temperature photoluminescence of these quantum dots, such as the short lifetime on the scale of microseconds and a zero-longitudinal optical phonon line in spectrum, both attributed to a dark exciton in literature, remain unexplained by existing models. Here we propose a theoretical model including the effect of solid-state environment on luminescence. The model captures both coherent and incoherent interactions of band-edge exciton with phonon modes. Our model predicts formation of dressed states by coupling of the exciton with a confined acoustic phonon mode, and explains the short lifetime and the presence of the zero-longitudinal optical phonon line in the spectrum. Accounting for the interaction of the exciton with bulk phonon modes, the model also explains the experimentally observed temperature-dependence of the photoluminescence decay dynamics and temperature-dependence of the photoluminescence spectrum.

SUBMITTER: Khosla M

PROVIDER: S-EPMC5976793 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature

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Polarons Explain Luminescence Behavior of Colloidal Quantum Dots at Low Temperature.

Khosla Meenakshi M Rao Sravya S Gupta Shilpi S

Scientific reports 20180530 1

Luminescence properties of colloidal quantum dots have found applications in imaging, displays, light-emitting diodes and lasers, and single photon sources. Despite wide interest, several experimental observations in low-temperature photoluminescence of these quantum dots, such as the short lifetime on the scale of microseconds and a zero-longitudinal optical phonon line in spectrum, both attributed to a dark exciton in literature, remain unexplained by existing models. Here we propose a theoret ...[more]

PMID: 29849075

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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

Polarons Explain Luminescence Behavior of Colloidal Quantum Dots at Low Temperature.

Publications

Polarons Explain Luminescence Behavior of Colloidal Quantum Dots at Low Temperature.

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