Octahedral distortion driven by CsPbI<sub>3</sub> nanocrystal reaction temperature – the effects on phase stability and beyond

Matuhina, Anastasia; Grandhi, G. Krishnamurthy; Liu, Maning; Smått, Jan‐Henrik; Viswanath, Noolu Srinivasa Manikanta; Ali‐Löytty, Harri; Lahtonen, Kimmo; Vivo, Paola

doi:10.1039/d1nr04071e

Cited by 10 publications

(11 citation statements)

References 40 publications

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“…The formation of r-CsMnCl 3 NCs instead of c-CsMnCl 3 NCs at higher injection temperatures is similar to the formation of the hexagonal structure of bulk CsMnCl 3 after heating its cubic structure at 300 °C for a few hours . Similar injection temperature-dependent phase control has already been achieved in the case of Pb-based perovskite NCs. − The anticipated 1:1 Cs/Mn ratio of all NCs was further confirmed by ICP–MS (see Table S3).…”

Section: Resultssupporting

confidence: 66%

“…To elucidate the dependence of the luminescence properties of CsMnCl 3 NCs on the structural parameters, we report the synthesis of these Pb-free NCs in two different crystal phases produced via the hot injection route, which is a well-known approach for the phase control of NCs. − The formation of cubic (c-) and rhombohedral (r-) phases of CsMnCl 3 NCs is demonstrated by the structural refinement of their X-ray diffraction (XRD) patterns. The two phases exhibit striking differences in luminescence properties, which are rationalized through the study of their electronic band structures by density functional theory (DFT) calculations.…”

Section: Introductionmentioning

confidence: 99%

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Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Matuhina

Grandhi

Pan

et al. 2023

ACS Appl. Nano Mater.

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Cesium manganese chloride (CsMnCl 3 ) nanocrystals (NCs) have recently been recognized as potential lead-free perovskite candidates for red emission. To ascertain how the luminescence properties depend on the NC structures formed under different synthesis conditions, we synthesized CsMnCl 3 NCs in two polymorphic structures, namely, cubic (c-CsMnCl 3 ) and rhombohedral (r-CsMnCl 3 ), by tuning the reaction temperature of a hot injection route. c-CsMnCl 3 NCs are found to be nonemissive, whereas r-CsMnCl 3 NCs exhibit red emission at 670 nm with a photoluminescence quantum yield of 40%. Density functional theory calculations reveal an indirect band gap for c-CsMnCl 3 �the electronic transitions between valence and conduction band edges are prohibited by orbital symmetry and spin. Conversely, r-CsMnCl 3 NCs possess a direct band gap. Further, transient absorption measurements suggest self-trapped exciton formation in r-CsMnCl 3 NCs, which contributes to their emission characteristics. Our proof-of-concept demonstration of photocurrent generated from the emitting r-CsMnCl 3 NCs indicates their suitability for luminescent solar concentrator applications. The findings of this work highlight the importance of understanding structure-luminescence relationship of emerging lead-free perovskites providing design criteria for red-emitting materials.

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Section: Resultssupporting

confidence: 66%

Section: Introductionmentioning

confidence: 99%

Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Matuhina

Grandhi

Pan

et al. 2023

ACS Appl. Nano Mater.

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“…Among the cesium lead halide (CsPbX 3 with X = Cl, Br, and I) perovskite nanocrystals (NCs), the CsPbI 3 NCs, because of their low band gap, are the most promising candidates for solar photovoltaic and various optoelectronic applications. − However, poor phase stability of these NCs even under ambient condition is a major obstacle to these applications. − Apart from the stability-related issues, photoluminescence (PL) blinking of the single NCs is another factor that restricts the applications of the CsPbI 3 NCs as single-photon emitters and other light-emitting applications. − PL blinking is indeed an issue for all single emitters. Among different models invoked for explaining the PL blinking of semiconductor NCs, a charging model based on trapping of the carrier in long-lived trap states ,− and a multiple recombination center (MRC) model based on the trapping of the carrier in short-lived trap states ,− are the most common ones.…”

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confidence: 99%

Phase-Stable and Highly Luminescent CsPbI₃ Perovskite Nanocrystals with Suppressed Photoluminescence Blinking

Paul

Samanta

2022

J. Phys. Chem. Lett.

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Despite their low band gap, the utility of CsPbI 3 nanocrystals (NCs) in solar photovoltaic and optoelectronic applications is rather limited because of their phase instability and photoluminescence (PL) intermittency. Herein we show that phase-pure, monodispersed, stable and highly luminescent CsPbI 3 NCs can be obtained by tweaking the conventional hot-injection method employing NH 4 I as an additional precursor. Single-particle studies show a significant suppression of PL blinking. Among all NCs studied, 60% exhibit only high-intensity ON states with a narrow distribution of intensity. The remaining 40% of NCs exhibit a much wider distribution of PL intensity with a significant contribution of low-intensity OFF states. Excellent characteristics of these CsPbI 3 NCs are shown to be the result of NH 4 + replacing some surface Cs + of an iodide-rich surface of the NCs. These phase-stable and highly luminescent CsPbI 3 NCs with significantly suppressed PL blinking can be useful single-photon emitters and promising materials for optoelectronic and solar photovoltaic applications.

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“…For instance, the phase stability of lead halide perovskites is enhanced by simply varying the reaction temperature. [ 12 ] Hence, the reaction temperatures for CSC:Sb 3+ NC synthesis were determined. Upon increasing the reaction temperature from 120 to 220 °C, the NCs transformed from spherical to cylindrical rod shapes, as shown in Figure a–c.…”

Section: Resultsmentioning

confidence: 99%

Thermally Stable Self‐Trapped Assisted Single‐Component White Light from Lead‐Free Zero‐Dimensional Metal Halide Nanocrystals

Samanta

Viswanath

Jang

et al. 2023

Advanced Optical Materials

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White‐light‐emitting single‐component materials are in high demand for lighting applications. However, achieving white light in single‐doped metal halide materials remains a challenge. Herein, for the first time, zero‐dimensional Cs3ScCl6:Sb3+(CSC:Sb3+) nanocrystals (NCs) are reported that exhibit bright white‐light emission, which is a result of combination of the excessive blue and yellow emissions of carbon dots and spin‐forbidden electronic transitions of Sb3+ ions. CSC:Sb3+ NCs exhibit a high photoluminescence quantum yield of 48%. Furthermore, they retain 75% of their original photoluminescence efficiency at 100 °C. This high thermal stability is mainly attributed to its lower dimensionality and high exciton binding energy as they facilitate the creation of stable white light at elevated temperatures. A single‐component white‐light‐emitting diode fabricated using CSC:Sb3+ NCs exhibits a high‐color rendering index and luminous efficacy values of 90 and 23 lm W−1 at a high flux current of 200 mA. Therefore, the findings may pave the way for developing the next generation of white‐light‐emitting devices using a single component of white‐light‐emitting material.

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Octahedral distortion driven by CsPbI₃ nanocrystal reaction temperature – the effects on phase stability and beyond

Abstract: Cesium lead iodide (CsPbI3) perovskite nanocrystals (NCs) suffer from a known transformation at room temperature from their red-emitting (black) to non-emitting (yellow) phase, induced by the tilting of PbI6 octahedra....

Cited by 10 publications

References 40 publications

Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Phase-Stable and Highly Luminescent CsPbI₃ Perovskite Nanocrystals with Suppressed Photoluminescence Blinking

Thermally Stable Self‐Trapped Assisted Single‐Component White Light from Lead‐Free Zero‐Dimensional Metal Halide Nanocrystals

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Octahedral distortion driven by CsPbI3 nanocrystal reaction temperature – the effects on phase stability and beyond

Abstract: Cesium lead iodide (CsPbI3) perovskite nanocrystals (NCs) suffer from a known transformation at room temperature from their red-emitting (black) to non-emitting (yellow) phase, induced by the tilting of PbI6 octahedra....

Cited by 10 publications

References 40 publications

Role of CsMnCl3 Nanocrystal Structure on Its Luminescence Properties

Role of CsMnCl3 Nanocrystal Structure on Its Luminescence Properties

Phase-Stable and Highly Luminescent CsPbI3 Perovskite Nanocrystals with Suppressed Photoluminescence Blinking

Thermally Stable Self‐Trapped Assisted Single‐Component White Light from Lead‐Free Zero‐Dimensional Metal Halide Nanocrystals

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Product

Resources

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Octahedral distortion driven by CsPbI₃ nanocrystal reaction temperature – the effects on phase stability and beyond

Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Role of CsMnCl₃ Nanocrystal Structure on Its Luminescence Properties

Phase-Stable and Highly Luminescent CsPbI₃ Perovskite Nanocrystals with Suppressed Photoluminescence Blinking