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1.
Sci Adv ; 5(10): eaav3140, 2019 10.
Article in English | MEDLINE | ID: mdl-31692653

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.

2.
ACS Nano ; 13(12): 14529-14539, 2019 Dec 24.
Article in English | MEDLINE | ID: mdl-31702890

ABSTRACT

The intricate features of many-body interactions and spin-orbit coupling play a significant role in numerous physical phenomena. Particularly in two-dimensional transition metal dichalcogenides (2D-TMDs), excitonic dynamics are a key phenomenon that promises opportunities for diverse range of device applications. Here, we report the direct observation of a visible-range three-dimensional resonant exciton and its associated charged exciton in monolayer tungsten diselenide, as compared to monolayer molybdenum disulfide. A comprehensive experimental study that includes high-resolution TEM, Raman, high-resolution spectroscopic ellipsometry over a wide temperature range down to 4 K, high-energy temperature, and excitation power-dependent photoluminescence spectroscopy has been conducted. It is supported by first-principles calculations to unravel the influence of spin-orbit coupling in the formation of the resonant exciton and to identify its in-plane and out-of-plane features. Furthermore, we study the impact of temperature and thickness on the spin-orbit coupling strength in 2D-TMDs. This work is crucial in creating a platform in the fundamental understanding of high-energy resonant exciton in layered two-dimensional systems and that such high-energy optoelectronic features make them an increasingly attractive candidate for novel electronic and optoelectronic applications particularly in the aspects of solar cells and light-emitting diodes via the manipulation of excitonic states.

3.
ACS Appl Mater Interfaces ; 11(45): 42838-42845, 2019 Nov 13.
Article in English | MEDLINE | ID: mdl-31635449

ABSTRACT

Hybrid organic-inorganic lead perovskites have a great potential in optoelectronic device applications because of their high stability, narrow band emission, and strong luminescence. Single crystals with few defects are the best candidates to disclose a variety of interesting and important properties for light-emitting devices. Here, we investigate a single-crystalline CH3NH3PbBr3 perovskite for its transport and electroluminescence properties. A simple fabrication method was used to obtain a 10 ± 2 µm channel between two gold wire electrodes, which showed bright intermittent electroluminescence near the interface of one wire after cooling down with a constant biasing voltage. The active region of the perovskite single crystal was pristine, well isolated from surroundings through fabrication to the characterization process. Our presented sample provided an ideal condition to study bulk ionic-electronic properties of hybrid halide perovskites. At constant 6 V bias, the current through the sample shows temperature-dependent oscillation with Arrhenius behavior, suggesting a thermally activated process. The light emission from the sample experiences an intermittent emission rate once every 26 ± 6 min. Here, we envisage that the current oscillations and intermittent emission are caused by ion-mediated negative differential resistance and conductive filament formation, respectively. The latter observation inspires future applications of the material from neuromorphic computing to the development of electroluminescence devices.

4.
Small ; 15(38): e1901983, 2019 Sep.
Article in English | MEDLINE | ID: mdl-31379086

ABSTRACT

Copper-doped colloidal quantum wells (Cu-CQWs) are considered a new class of optoelectronic materials. To date, the electroluminescence (EL) property of Cu-CQWs has not been revealed. Additionally, it is desirable to achieve ultrapure green, tunable dual-emission and white light to satisfy the various requirement of display and lighting applications. Herein, light-emitting diodes (LEDs) based on colloidal Cu-CQWs are demonstrated. For the 0% Cu-doped concentration, the LED exhibits Commission Internationale de L'Eclairage 1931 coordinates of (0.103, 0.797) with a narrow EL full-wavelength at half-maximum of 12 nm. For the 0.5% Cu-doped concentration, a dual-emission LED is realized. Remarkably, the dual emission can be tuned by manipulating the device engineering. Furthermore, at a high doping concentration of 2.4%, a white LED based on CQWs is developed. With the management of doping concentrations, the color tuning (green, dual-emission to white) is shown. The findings not only show that LEDs with CQWs can exhibit polychromatic emission but also unlock a new direction to develop LEDs by exploiting 2D impurity-doped CQWs that can be further extended to the application of other impurities (e.g., Mn, Ag).

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