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

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          Abstract

          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 CsPbX 3 (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 CsPbX 3 nanocrystals and random lasing in films of CsPbX 3 nanocrystals.

          Abstract

          Lead halide perovskite colloidal nanocrystals have promising optoelectronic properties, such as high photoluminescence quantum yields and narrow emission linewidths. Here, the authors report low-threshold amplified spontaneous emission and two kinds of lasing in nanostructured caesium lead halide perovskites.

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          Most cited references21

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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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            Colloidal nanoplatelets with two-dimensional electronic structure.

            The syntheses of strongly anisotropic nanocrystals with one dimension much smaller than the two others, such as nanoplatelets, are still greatly underdeveloped. Here, we demonstrate the formation of atomically flat quasi-two-dimensional colloidal CdSe, CdS and CdTe nanoplatelets with well-defined thicknesses ranging from 4 to 11 monolayers. These nanoplatelets have the electronic properties of two-dimensional quantum wells formed by molecular beam epitaxy, and their thickness-dependent absorption and emission spectra are described very well within an eight-band Pidgeon-Brown model. They present an extremely narrow emission spectrum with full-width at half-maximum less than 40 meV at room temperature. The radiative fluorescent lifetime measured in CdSe nanoplatelets decreases with temperature, reaching 1 ns at 6 K, two orders of magnitude less than for spherical CdSe nanoparticles. This makes the nanoplatelets the fastest colloidal fluorescent emitters and strongly suggests that they show a giant oscillator strength transition.
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              Room-temperature near-infrared high-Q perovskite whispering-gallery planar nanolasers.

              Near-infrared (NIR) solid-state micro/nanolasers are important building blocks for true integration of optoelectronic circuitry. Although significant progress has been made in III-V nanowire lasers with achieving NIR lasing at room temperature, challenges remain including low quantum efficiencies and high Auger losses. Importantly, the obstacles toward integrating one-dimensional nanowires on the planar ubiquitous Si platform need to be effectively tackled. Here we demonstrate a new family of planar room-temperature NIR nanolasers based on organic-inorganic perovskite CH3NH3PbI(3-a)X(a) (X = I, Br, Cl) nanoplatelets. Their large exciton binding energies, long diffusion lengths, and naturally formed high-quality planar whispering-gallery mode cavities ensure adequate gain and efficient optical feedback for low-threshold optically pumped in-plane lasing. We show that these remarkable wavelength tunable whispering-gallery nanolasers can be easily integrated onto conductive platforms (Si, Au, indium tin oxide, and so forth). Our findings open up a new class of wavelength tunable planar nanomaterials potentially suitable for on-chip integration.
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Pub. Group
                2041-1723
                20 August 2015
                2015
                : 6
                : 8056
                Affiliations
                [1 ]Department of Chemistry and Applied Biosciences, Laboratory of Inorganic Chemistry, ETH Zürich , Vladimir-Prelog-Weg 1, CH-8093 Zürich, Switzerland
                [2 ]Laboratory for Thin Films and Photovoltaics, Empa—Swiss Federal Laboratories for Materials Science and Technology , Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
                [3 ]Institute of Semiconductor and Solid State Physics, University Linz , Altenbergerstraße 69, 4040 Linz, Austria
                [4 ]Department of Materials, Laboratory for Multifunctional Ferroic Materials, ETH Zürich , Vladimir-Prelog-Weg 4, CH-8093 Zürich, Switzerland
                [5 ]Materials for Electronics and Energy Technology (i-MEET), Friedrich-Alexander-Universität Erlangen-Nürnberg , Martensstraße 7, 91058 Erlangen, Germany
                [6 ]Energie Campus Nürnberg (EnCN) , Fürther Straße 250, 90429 Nürnberg, Germany
                Author notes
                Article
                ncomms9056
                10.1038/ncomms9056
                4560790
                26290056
                179aeb8b-1ac4-44a8-b14d-5af31f3f9274
                Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 21 April 2015
                : 13 July 2015
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