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Electrically control amplified spontaneous emission in colloidal quantum dots.

ABSTRACT: Colloidal quantum dots (CQDs) are highly promising materials for light amplification thanks to their efficient photoluminescence, tunable emission wavelength and low-cost synthesis. Unfortunately, CQDs are suffering from band-edge state degeneracy which demands multiple excitons to achieve population inversion. As a result, non-radiative Auger recombination increases the lasing threshold and limits the gain lifetime. Here, benefiting from the negative charging, we demonstrate that the amplified spontaneous emission (ASE) threshold is controllable in a device where CQD film is exposed to an external electric field. Specifically, singly charged CQDs lower the threshold due to the preexisting electron in the conduction band, while strongly enhanced Auger recombination in doubly charged CQDs stymies the ASE. Experimental results and kinetic equation model show that ASE threshold reduces 10% even if our device only charges ~17% of the CQD population. Our results open new possibilities for controlling exciton recombination dynamics and achieving electrically pumped CQD lasers.

SUBMITTER: Yu J

PROVIDER: S-EPMC6814376 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Electrically control amplified spontaneous emission in colloidal quantum dots.

Yu Junhong J Shendre Sushant S Koh Weon-Kyu WK Liu Baiquan B Li Mingjie M Hou Songyan S Hettiarachchi Chathuranga C Delikanli Savas S Hernández-Martínez Pedro P Birowosuto Muhammad Danang MD Wang Hong H Sum TzeChien T Demir Hilmi Volkan HV Dang Cuong C

Science advances 20191025 10

Colloidal quantum dots (CQDs) are highly promising materials for light amplification thanks to their efficient photoluminescence, tunable emission wavelength and low-cost synthesis. Unfortunately, CQDs are suffering from band-edge state degeneracy which demands multiple excitons to achieve population inversion. As a result, non-radiative Auger recombination increases the lasing threshold and limits the gain lifetime. Here, benefiting from the negative charging, we demonstrate that the amplified ...[more]

PMID: 31692653

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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

Electrically control amplified spontaneous emission in colloidal quantum dots.

Publications

Electrically control amplified spontaneous emission in colloidal quantum dots.

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