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      Realization of “warm” white light via halide substitution in polar two-dimensional hybrid perovskites (2meptH 2)PbCl xBr 4−x

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          Abstract

          A family of 2D hybrid perovskites that emit intrinsic broadband emissions with tunable photoluminescence from “cold” to “warm” white light.

          Abstract

          Broadband white-light emissive two-dimensional (2D) metal halide perovskites have attracted increasing attention in solid-state optical applications. Herein, we present a family of polar 2D hybrid perovskites, (2meptH 2)PbCl xBr 4−x (2mept = 2-methyl-1,5-diaminopentane, x = 0–4), which emit intrinsic broadband emissions with tunable photoluminescence from “cold” white light to “warm” white light. Importantly, a high-performance “warm” white light with a correlated colour temperature of 3958 K and an excellent colour rendering index of 84 was successfully realized in (2meptH 2)PbCl 4, making it ideal for indoor lighting applications. Mechanistic studies disclose that the broadband white-light emissions are attributed to self-trapped excitons stemming from the strong electron–phonon coupling in the distorted structure, which reasonably explained the emission changes in the mixed-halide perovskites. Such halide substitution inducing high tunability in white-light emissions provides a deep understanding on the underlying structure–property relationship, and further conducts the design of desirable white-light emissive materials.

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          Sequential deposition as a route to high-performance perovskite-sensitized solar cells.

          Following pioneering work, solution-processable organic-inorganic hybrid perovskites-such as CH3NH3PbX3 (X = Cl, Br, I)-have attracted attention as light-harvesting materials for mesoscopic solar cells. So far, the perovskite pigment has been deposited in a single step onto mesoporous metal oxide films using a mixture of PbX2 and CH3NH3X in a common solvent. However, the uncontrolled precipitation of the perovskite produces large morphological variations, resulting in a wide spread of photovoltaic performance in the resulting devices, which hampers the prospects for practical applications. Here we describe a sequential deposition method for the formation of the perovskite pigment within the porous metal oxide film. PbI2 is first introduced from solution into a nanoporous titanium dioxide film and subsequently transformed into the perovskite by exposing it to a solution of CH3NH3I. We find that the conversion occurs within the nanoporous host as soon as the two components come into contact, permitting much better control over the perovskite morphology than is possible with the previously employed route. Using this technique for the fabrication of solid-state mesoscopic solar cells greatly increases the reproducibility of their performance and allows us to achieve a power conversion efficiency of approximately 15 per cent (measured under standard AM1.5G test conditions on solar zenith angle, solar light intensity and cell temperature). This two-step method should provide new opportunities for the fabrication of solution-processed photovoltaic cells with unprecedented power conversion efficiencies and high stability equal to or even greater than those of today's best thin-film photovoltaic devices.
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            High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells

            Three-dimensional organic-inorganic perovskites have emerged as one of the most promising thin-film solar cell materials owing to their remarkable photophysical properties, which have led to power conversion efficiencies exceeding 20 per cent, with the prospect of further improvements towards the Shockley-Queisser limit for a single‐junction solar cell (33.5 per cent). Besides efficiency, another critical factor for photovoltaics and other optoelectronic applications is environmental stability and photostability under operating conditions. In contrast to their three-dimensional counterparts, Ruddlesden-Popper phases--layered two-dimensional perovskite films--have shown promising stability, but poor efficiency at only 4.73 per cent. This relatively poor efficiency is attributed to the inhibition of out-of-plane charge transport by the organic cations, which act like insulating spacing layers between the conducting inorganic slabs. Here we overcome this issue in layered perovskites by producing thin films of near-single-crystalline quality, in which the crystallographic planes of the inorganic perovskite component have a strongly preferential out-of-plane alignment with respect to the contacts in planar solar cells to facilitate efficient charge transport. We report a photovoltaic efficiency of 12.52 per cent with no hysteresis, and the devices exhibit greatly improved stability in comparison to their three-dimensional counterparts when subjected to light, humidity and heat stress tests. Unencapsulated two-dimensional perovskite devices retain over 60 per cent of their efficiency for over 2,250 hours under constant, standard (AM1.5G) illumination, and exhibit greater tolerance to 65 per cent relative humidity than do three-dimensional equivalents. When the devices are encapsulated, the layered devices do not show any degradation under constant AM1.5G illumination or humidity. We anticipate that these results will lead to the growth of single-crystalline, solution-processed, layered, hybrid, perovskite thin films, which are essential for high-performance opto-electronic devices with technologically relevant long-term stability.
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              Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes.

              Organic-inorganic hybrid perovskites are emerging low-cost emitters with very high color purity, but their low luminescent efficiency is a critical drawback. We boosted the current efficiency (CE) of perovskite light-emitting diodes with a simple bilayer structure to 42.9 candela per ampere, similar to the CE of phosphorescent organic light-emitting diodes, with two modifications: We prevented the formation of metallic lead (Pb) atoms that cause strong exciton quenching through a small increase in methylammonium bromide (MABr) molar proportion, and we spatially confined the exciton in uniform MAPbBr3 nanograins (average diameter = 99.7 nanometers) formed by a nanocrystal pinning process and concomitant reduction of exciton diffusion length to 67 nanometers. These changes caused substantial increases in steady-state photoluminescence intensity and efficiency of MAPbBr3 nanograin layers.
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                Author and article information

                Contributors
                Journal
                JMCCCX
                Journal of Materials Chemistry C
                J. Mater. Chem. C
                Royal Society of Chemistry (RSC)
                2050-7526
                2050-7534
                November 22 2018
                2018
                : 6
                : 45
                : 12267-12272
                Affiliations
                [1 ]State Key Laboratory of Structural Chemistry
                [2 ]Fujian Institute of Research on the Structure of Matter
                [3 ]Chinese Academy of Sciences
                [4 ]Fuzhou 350002
                [5 ]China
                Article
                10.1039/C8TC03167C
                a8e45938-102e-4eef-8312-28317f05e5e3
                © 2018

                http://rsc.li/journals-terms-of-use

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