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      Lasing Supraparticles Self-Assembled from Nanocrystals

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          Abstract

          One of the most attractive commercial applications of semiconductor nanocrystals (NCs) is their use in lasers. Thanks to their high quantum yield, tunable optical properties, photostability, and wet-chemical processability, NCs have arisen as promising gain materials. Most of these applications, however, rely on incorporation of NCs in lasing cavities separately produced using sophisticated fabrication methods and often difficult to manipulate. Here, we present whispering gallery mode lasing in supraparticles (SPs) of self-assembled NCs. The SPs composed of NCs act as both lasing medium and cavity. Moreover, the synthesis of the SPs, based on an in-flow microfluidic device, allows precise control of the dimensions of the SPs, i.e. the size of the cavity, in the micrometer range with polydispersity as low as several percent. The SPs presented here show whispering gallery mode resonances with quality factors up to 320. Whispering gallery mode lasing is evidenced by a clear threshold behavior, coherent emission, and emission lifetime shortening due to the stimulation process.

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          Most cited references39

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          Is Open Access

          Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites

          Metal halide semiconductors with perovskite crystal structures have recently emerged as highly promising optoelectronic materials. Despite the recent surge of reports on microcrystalline, thin-film and bulk single-crystalline metal halides, very little is known about the photophysics of metal halides in the form of uniform, size-tunable nanocrystals. Here we report low-threshold amplified spontaneous emission and lasing from ∼10 nm monodisperse colloidal nanocrystals of caesium lead halide perovskites CsPbX3 (X=Cl, Br or I, or mixed Cl/Br and Br/I systems). We find that room-temperature optical amplification can be obtained in the entire visible spectral range (440–700 nm) with low pump thresholds down to 5±1 μJ cm−2 and high values of modal net gain of at least 450±30 cm−1. Two kinds of lasing modes are successfully observed: whispering-gallery-mode lasing using silica microspheres as high-finesse resonators, conformally coated with CsPbX3 nanocrystals and random lasing in films of CsPbX3 nanocrystals.
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            Optical gain and stimulated emission in nanocrystal quantum dots.

            The development of optical gain in chemically synthesized semiconductor nanoparticles (nanocrystal quantum dots) has been intensely studied as the first step toward nanocrystal quantum dot lasers. We examined the competing dynamical processes involved in optical amplification and lasing in nanocrystal quantum dots and found that, despite a highly efficient intrinsic nonradiative Auger recombination, large optical gain can be developed at the wavelength of the emitting transition for close-packed solids of these dots. Narrowband stimulated emission with a pronounced gain threshold at wavelengths tunable with the size of the nanocrystal was observed, as expected from quantum confinement effects. These results unambiguously demonstrate the feasibility of nanocrystal quantum dot lasers.
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              All-Inorganic Colloidal Perovskite Quantum Dots: A New Class of Lasing Materials with Favorable Characteristics.

              All-inorganic colloidal cesium lead halide perovskite quantum dots (CsPbX3 , X = Cl, Br, I) are revealed to be a new class of favorable optical-gain materials, which show -combined merits of both colloidal quantum dots and halide perovskites. Low-threshold and -ultrastable stimulated emission is -demonstrated under atmospheric conditions with wavelength tunability across the whole -visible spectrum via either size or composition control.

                Author and article information

                Journal
                ACS Nano
                ACS Nano
                nn
                ancac3
                ACS Nano
                American Chemical Society
                1936-0851
                1936-086X
                12 December 2018
                26 December 2018
                : 12
                : 12
                : 12788-12794
                Affiliations
                [1] Condensed Matter and Interfaces and Soft Condensed Matter groups, Debye Institute for Nanomaterials Science, Utrecht University , P.O. Box 80000, 3508 TA Utrecht, The Netherlands
                [§ ]IBM Research − Zurich , Säumerstrasse 4, 8803 Rüschlikon, Switzerland
                Author notes
                Article
                10.1021/acsnano.8b07896
                6307080
                30540430
                8e908801-f745-43fd-950c-6657c95281ea
                Copyright © 2018 American Chemical Society

                This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.

                History
                : 16 October 2018
                : 12 December 2018
                Categories
                Article
                Custom metadata
                nn8b07896
                nn-2018-07896q

                Nanotechnology
                self-assembly,whispering gallery modes,supraparticles,semiconductor nanocrystals,lasing

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