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1.
Adv Mater ; 35(1): e2207678, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36333885

ABSTRACT

The use of colloidal quantum dots (CQDs) as a gain medium in infrared laser devices has been underpinned by the need for high pumping intensities, very short gain lifetimes, and low gain coefficients. Here, PbS/PbSSe core/alloyed-shell CQDs are employed as an infrared gain medium that results in highly suppressed Auger recombination with a lifetime of 485 ps, lowering the amplified spontaneous emission (ASE) threshold down to 300 µJ cm-2 , and showing a record high net modal gain coefficient of 2180 cm-1 . By doping these engineered core/shell CQDs up to nearly filling the first excited state, a significant reduction of optical gain threshold is demonstrated, measured by transient absorption, to an average-exciton population-per-dot 〈Nth 〉g of 0.45 due to bleaching of the ground state absorption. This in turn have led to a fivefold reduction in ASE threshold at 〈Nth 〉ASE  = 0.70 excitons-per-dot, associated with a gain lifetime of 280 ps. Finally, these heterostructured QDs are used to achieve near-infrared lasing at 1670 nm at a pump fluences corresponding to sub-single-exciton-per-dot threshold (〈Nth 〉Las  = 0.87). This work brings infrared CQD lasing thresholds on par to their visible counterparts, and paves the way toward solution-processed infrared laser diodes.

2.
Adv Sci (Weinh) ; 9(8): e2104758, 2022 Mar.
Article in English | MEDLINE | ID: mdl-35038253

ABSTRACT

Passive radiative cooling (RC) enables the cooling of objects below ambient temperature during daytime without consuming energy, promising to be a game changer in terms of energy savings and CO2 reduction. However, so far most RC surfaces are obtained by energy-intensive nanofabrication processes or make use of unsustainable materials. These limitations are overcome by developing cellulose films with unprecedentedly low absorption of solar irradiance and strong mid-infrared (mid-IR) emittance. In particular, a cellulose-derivative (cellulose acetate) is exploited to produce porous scattering films of two different thicknesses, L ≈ 30 µm (thin) and L ≈ 300 µm (thick), making them adaptable to above and below-ambient cooling applications. The thin and thick films absorb only ≈ 5 % ${\approx}5\%$ of the solar irradiance, which represents a net cooling power gain of at least 17 W m-2 , compared to state-of-the-art cellulose-based radiative-cooling materials. Field tests show that the films can reach up to ≈5 °C below ambient temperature, when solar absorption and conductive/convective losses are minimized. Under dryer conditions (water column = 1 mm), it is estimated that the films can reach average minimum temperatures of ≈7-8 °C below the ambient. The work presents an alternative cellulose-based material for efficient radiative cooling that is simple to fabricate, cost-efficient and avoids the use of polluting materials.

3.
Adv Mater ; 34(3): e2107532, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34762320

ABSTRACT

Pb-chalcogenide colloidal quantum dots (CQDs) are attractive materials to be used as tuneable laser media across the infrared spectrum. However, excessive nonradiative Auger recombination due to the presence of trap states outcompetes light amplification by rapidly annihilating the exciton population, leading to high gain thresholds. Here, a binary blend is employed of CQDs and ZnO nanocrystals in order to passivate the in-gap trap states of PbS-CQD gain medium. Using transient absorption, a fivefold increase is measured in Auger lifetime demonstrating the suppression of trap-assisted Auger recombination. By doing so, a twofold reduction is achieved in amplified spontaneous emission (ASE) threshold. Finally, by integrating the proposed binary blend to a distributed feedback (DFB) resonator, single-mode lasing emission is demonstrated at 1650 nm with a linewidth of 1.23 nm (0.62 meV), operating at a low lasing threshold of ≈385 µJ cm-2 . The Auger suppression in this system has allowed to achieve unprecedented lasing emission stability for a CQD laser with recorded continuous operation of 5 h at room temperature and ambient conditions.

4.
Sci Rep ; 10(1): 5371, 2020 Mar 25.
Article in English | MEDLINE | ID: mdl-32214137

ABSTRACT

Surface patterning technologies represent a worldwide growing industry, creating smart surfaces and micro/nanoscale device. The advent of large-area, high-speed imprinting technologies has created an ever-growing need for rapid and non-destructive dimensional metrology techniques to keep pace with the speed of production. Here we present a new real-time optical scatterometry technique, applicable at the mesoscale when optical inspection produces multiple orders of diffraction. We validate this method by inspecting multiple silicon gratings with a variety of structural parameters. These measurements are cross-referenced with FIB, SEM and scanning stylus profilometry. Finally, we measure thermally imprinted structures as a function of imprinting temperature in order to demonstrate the method suitable for in-line quality control in nanoimprint lithography.

5.
Small ; 15(52): e1905290, 2019 Dec.
Article in English | MEDLINE | ID: mdl-31650687

ABSTRACT

The regulation of temperature is a major energy-consuming process of humankind. Today, around 15% of the global-energy consumption is dedicated to refrigeration and this figure is predicted to triple by 2050, thus linking global warming and cooling needs in a worrying negative feedback-loop. Here, an inexpensive solution is proposed to this challenge based on a single layer of silica microspheres self-assembled on a soda-lime glass. This 2D crystal acts as a visibly translucent thermal-blackbody for above-ambient radiative cooling and can be used to improve the thermal performance of devices that undergo critical heating during operation. The temperature of a silicon wafer is found to be 14 K lower during daytime when covered with the thermal emitter, reaching an average temperature difference of 19 K when the structure is backed with a silver layer. In comparison, the soda-lime glass reference used in the measurements lowers the temperature of the silicon by just 5 K. The cooling power of this simple radiative cooler under direct sunlight is found to be 350 W m-2 when applied to hot surfaces with relative temperatures of 50 K above the ambient. This is crucial to radiatively cool down devices, i.e., solar cells, where an increase in temperature has drastic effects on performance.

6.
Opt Express ; 24(21): 23677-23684, 2016 Oct 17.
Article in English | MEDLINE | ID: mdl-27828204

ABSTRACT

Hybrid perovskite materials have considerable potential for light emitting devices such as LEDs and lasers. We combine solution processed CH3NH3PbI3 perovskite with UV nanoimprinted polymer gratings to fabricate distributed feedback (DFB) lasers. The lead acetate deposition route is shown to be an effective method for fabricating low-loss waveguides (loss coefficient ~6 cm-1) and highly compatible with the polymer grating substrates. The nanoimprinted perovskite exhibited single-mode band-edge lasing, confirmed by angle-dependent transmission measurements. Depending on the excitation pulse duration the lasing threshold shows a value of 110 µJ/cm2 under nanosecond pumping and 4 µJ/cm2 under femtosecond pumping. We demonstrate further that this laser has excellent stability with a lifetime of 108 pulses.

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