Postsynthetic Doping of MnCl<sub>2</sub> Molecules into Preformed CsPbBr<sub>3</sub> Perovskite Nanocrystals via a Halide Exchange‐Driven Cation Exchange

Huang, Gui Chao; Wang, Chunlei; Zong, Shenfei; Ju, Lu; Wang, Zhuyuan; Lü, Changgui; Cui, Yiping

doi:10.1002/adma.201700095

Cited by 211 publications

(201 citation statements)

References 41 publications

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“…[24] However, color tunability and PLQY improvement were typically achieved only in nanostructures, [25] including inorganic perovskite nanocrystals, [26][27][28][29][30][31] probably due to the low doping limit that is not sufficient to compensate for the abundant defects in bulk. [24] However, color tunability and PLQY improvement were typically achieved only in nanostructures, [25] including inorganic perovskite nanocrystals, [26][27][28][29][30][31] probably due to the low doping limit that is not sufficient to compensate for the abundant defects in bulk.…”

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confidence: 99%

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

et al. 2018

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Metal-halide perovskites represent a class of promising light absorbers for efficient solar cells. [1][2][3][4][5] The propensity of perovskite films for low-cost solution processing also encourages scientists to explore potential applications beyond solar cells. [6][7][8][9] In particular, as emitters, perovskites exhibit intriguing luminescent properties such as narrowband emission, spectral tunability, and high quantum efficiency, which enables applications in the microlasers and light-emitting diodes (LEDs). [10][11][12][13] The luminescence efficiency of perovskites generally relies on nanostructures that can spatially confine excitons, and consequently reduce the possibility of nonradiative recombination during the carrier/ exciton migration. However, nanocrystals, due to boundary scattering of carriers, generally face the problem of poor charge transport, which is undesirable for LED performance. 2D perovskites, where bulky organic layers and inorganic layers are alternately and periodically arranged, feature natural quantum-well structures. This quantum-well structure is regarded as promising LED emitters for decades. [14][15][16] However, low photoluminescence quantum yields (PLQYs, typically < 1%) of 2D perovskites at room temperature is a bottleneck to achieving high-performance LEDs. [17] The low PLQYs may be attributed to insufficient confinement of Wannier type excitons within the inorganic layers [18] as suggested by the long charge-carrier/exciton diffusion length (60 nm). [19] Engineering crystal structures of low-dimensional (0D to 2D) perovskites by employing suitable organic ammonium cations is the predominant methods for the tuning of luminescence, both in spectral coverage and efficiency. [20,21] In these cases, severe structural distortion of metal halide octahedra is a common feature because of the size mismatch between organic and inorganic components, which results in potential fluctuations. [22,23] Such fluctuations of potential within an inorganic layer of perovskite sometimes, but not always, [20,21] slow the diffusion of carriers or excitons, and consequently induce self-trapped excitons (STEs), which represents a type of bound states for efficient radiative recombination. However, the occurrence of exciton self-trapping in semiconductors is the exception rather than the rule. [24] In parallel, compositional engineering As emerging efficient emitters, metal-halide perovskites offer the intriguing potential to the low-cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron-hole pairs). Here, Sn-triggered extrinsic self-trapping of excitons in bulk 2D perovskite crystal, PEA 2 PbI 4 (PEA = phenylethylammonium), is reported, where exciton self-trapping never occurs in its pure state. By creating local potential wells, isoelectronic Sn dopants initiate the localization of excitons, which would further induce the large lattice deformation around the impurities to accommodate the se...

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Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

et al. 2018

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“…That phenomenon suggests that Ce 3+ ions are not discharged in whole exchange process, and it could be explained by the electronegativity difference of those cations. Based on the electronegativities of Ca 2+ (1.132 for CN=8), Sr 2+ (1.123 for CN=8), and Ce 3+ (1.298 for CN=8) cations calculated by D. Xue, the difference between Ca 2+ and Ce 3+ cations is much larger than that between Ca 2+ and Sr 3+ cations and hence the exchange reaction between Ca 2+ and Sr 3+ cations is prior to that between Ca 2+ and Ce 3+ cations . The above‐discussed results further illustrate the selective substitution of the ion exchange technique, and it would be beneficial for boosting the relative widespread applications in the luminescence modulation of phosphors.…”

Section: Resultsmentioning

confidence: 65%

Facile Post‐Synthesis of a Ce³⁺‐Doped Ca_xSr_1‐xSc₂O₄ Phosphor by Means of Cation Exchange

Wang

Liu

et al. 2018

ChemistrySelect

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Ion exchange is a useful method to synthesize the materials by the ion replacement from the template crystal structure. Here, by means of the cation exchange technique, we demonstrate a facile post‐synthesis CaxSr1‐xSc2O4:Ce3+ from SrSc2O4:Ce3+. In this exchange process, the framework of ScO6 octahedra is remaining, and Sr2+ ions are substituted by the Ca2+ ions from the CaCl2 melt. After optimizing the relevant parameters (the reaction mole ratio, temperature, and time), the largest exchange ratio could reach ∼97%. In addition, Ce3+ ions are almost not escaped through the exchange process, and the luminescent performance of final exchanged phosphors is comparable to the products from traditional bottom‐up approaches. Hence, the demonstration in this work manifests the excellent simplification and controllability of ion exchange in adjusting the luminescent property of phosphors and gives some significant inspirations for the design and preparation of lanthanide‐activated materials.

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“…The synthesis of CsPbBr 3 is following our previous work [10]. 0.191 g of Cs(AC) was dissolved in 1 ml DMF forming the 'aqueous phase' Cs-precursor, and 0.367 g of PbBr 2 was dissolved in 1 ml DMF forming Pbprecursor, respectively.…”

Section: Synthesis Of Cspbbr 3 Ncsmentioning

confidence: 99%

“…Lead halide perovskite materials have attracted more and more attention for their good optical properties and potential applications [1][2][3][4]. All-inorganic cesium lead halide (CsPbX 3 ) NCs with superb photo-physical properties and facile chemical tunability of the bandgap have shown great application potential in fields of highefficiency solar cells, color-tunable light-emitting diodes (LEDs), laser and so on [5][6][7][8][9][10]. More papers make great efforts to control over the electronic and optical properties of CsPbX 3 NCs.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Mn-doped CsPbCl_xBr_3−x perovskite nanocrystals using ultrasonic irradiation-promoted with decrease of reaction order

Xu¹,

Zhang²,

Wu³

et al. 2020

Nano Ex.

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The incorporation of impurity cation as a way of introducing various novel functionalities provides an additional level of control over the electronic and optical properties of perovskite nanocrystals (NCs). However, the conventional post-synthetic cation exchange approaches suffer from large time and energy consumption. In this work, we developed a novel one-pot method to synthesize Mn-doped CsPbCl x Br 3−x NCs by merit of sonochemical technique, achieving dramatically rapid reduce of time and energy consumption. The localized hot spots with high transient temperature, pressure, and cooling rate, as well as an excellent stirring action of ultrasonic preparation facilitate the diffusion of Mn 2+ in perovskite lattice. Besides, further reaction kinetics investigation reveals an apparent decrease of reaction order from original method (2.4) to our ultrasound-assisted method (1.0).

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Postsynthetic Doping of MnCl₂ Molecules into Preformed CsPbBr₃ Perovskite Nanocrystals via a Halide Exchange‐Driven Cation Exchange

Cited by 211 publications

References 41 publications

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

Facile Post‐Synthesis of a Ce³⁺‐Doped Ca_xSr_1‐xSc₂O₄ Phosphor by Means of Cation Exchange

Synthesis of Mn-doped CsPbCl_xBr_3−x perovskite nanocrystals using ultrasonic irradiation-promoted with decrease of reaction order

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Postsynthetic Doping of MnCl2 Molecules into Preformed CsPbBr3 Perovskite Nanocrystals via a Halide Exchange‐Driven Cation Exchange

Cited by 211 publications

References 41 publications

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites

Facile Post‐Synthesis of a Ce3+‐Doped CaxSr1‐xSc2O4 Phosphor by Means of Cation Exchange

Synthesis of Mn-doped CsPbClxBr3−x perovskite nanocrystals using ultrasonic irradiation-promoted with decrease of reaction order

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Postsynthetic Doping of MnCl₂ Molecules into Preformed CsPbBr₃ Perovskite Nanocrystals via a Halide Exchange‐Driven Cation Exchange

Facile Post‐Synthesis of a Ce³⁺‐Doped Ca_xSr_1‐xSc₂O₄ Phosphor by Means of Cation Exchange

Synthesis of Mn-doped CsPbCl_xBr_3−x perovskite nanocrystals using ultrasonic irradiation-promoted with decrease of reaction order