On the origins of the green luminescence in the “zero-dimensional perovskite” Cs<sub>4</sub>PbBr<sub>6</sub>: conclusive results from cathodoluminescence imaging

Riesen, Nicolas; Badek, Kate; Riesen, Hans

doi:10.1039/c8nr09255a

Cited by 57 publications

(66 citation statements)

References 36 publications

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“…The origin of the green photoluminescence, however, has been subject of a large debate: Nikl et al [26] were the first to suggest that unavoidable CsPbBr 3 nanocrystal impurities in Cs 4 PbBr 6 gives origins to the green photoluminescence. A recent article has yielded further convincing experimental evidence of the latter [27].…”

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confidence: 92%

Optical Characterization of Cesium Lead Bromide Perovskites

Vitale

Privitera

et al. 2019

Crystals

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CsPbBr 3 and Cs 4 PbBr 6 perovskite powders have been synthesized through a relatively simple low-temperature and low-cost method. Nanocrystalline films have also been deposited from solutions with four different molar compositions of binary salt precursors. Optical absorption, emission and excitation spectra have been performed in the UV-visible spectral range while X-ray diffraction (XRD) has been recorded to characterize the nanocrystal morphology for the different molar compositions. A preferential orientation of crystallites along the (024) crystalline plane has been observed as a function of the different deposition conditions in films growth. All the crystals show an absorption edge around 530 nm; Tauc plots of the absorption returned bandgaps ranging from 2.29 to 2.35 eV characteristic of CsPbBr 3 phase. We attribute the UV absorption band peaked at 324 nm to the fundamental band-to-band transition for Cs 4 PbBr 6 . It was observed that the samples with the most ordered Cs 4 PbBr 6 crystals exhibited the most intense emission of light, with a bright green emission at 520 nm, which are however due to the luminescence of the inclusion of CsPbBr 3 nanoclusters into the Cs 4 PbBr 6 . The latter shows instead an intense UV emission. Differently, the pure CsPbBr 3 powder did not show any intense fluorescent emission. The excitation spectra of the green fluorescent emission in all samples closely resemble the CsPbBr 3 absorption with the peculiar dip around 324 nm as expected from density of state calculations reported in the literature. and B an inorganic one, the perovskite is considered as hybrid organic-inorganic. On the contrary, if A is inorganic (mostly Cs + ) the perovskite is all-inorganic.Hybrid organic-inorganic metal halides (HOIMHs) have been extensively investigated for a wide range of applications, such as photovoltaics [2][3][4][5][6][7], light emitting diodes (LED) or lasers [8][9][10][11][12][13], radiation detection [14], and down-converting phosphors [15][16][17]. Interesting carrier transport properties have been observed in Pb-and Sn-based 3D halide perovskites [18,19]. HOIMHs, like MAPbI 3 , have been broadly studied as solar absorber materials in photovoltaic cells [20].Distinct crystalline forms with the general formula A n BX 2+n give rise to an extended perovskite family [21]. They differ in the spatial coordination of the metal-halide octahedra XBr 6 4where the value of n determines the perovskite's structural dimensionality expressing the coordination of octahedra: n = 1 characterizes three-dimensional (3D) perovskites with corner-shared octahedra along every axis, n = 4 identifies zero-dimensional (0D) perovskites with isolated octahedra, as shown in Figure 1a for cesium lead perovskites. Efficient photoluminescence is associated to the intrinsic geometric structures or the different network dimensionalities due to the occurrence of quantum confinement into the isolated octahedra of 0D-crystals [22]. The Frenkel excitons result self-trapped in correspondence of the octahedron center...

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confidence: 92%

Optical Characterization of Cesium Lead Bromide Perovskites

Vitale

Privitera

et al. 2019

Crystals

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“…Riesen et al have utilized cathodoluminescence (CL) imaging to confirm the presence of small crystals embedded in/or between larger crystallites of the prepared Cs 4 PbBr 6 (Figure 7e-g). [57] The luminescent spot emitting at 520 nm was analyzed by EDX to give a Pb:Br ratio of 2 times higher than other areas, confirming the existence of CsPbBr 3 impurities in the Cs 4 PbBr 6 bulk phase. The PL at~520 nm observed by different groups overlaps with the intrinsic PL emission of CsPbBr 3 NCs (Table 2), suggesting possible origin of the observed emission due to the embedded CsPbBr 3 phase.…”

Section: Emission From Embedded Phase Of Cspbbr 3 Ncsmentioning

confidence: 83%

“…Riesen et al. have utilized cathodoluminescence (CL) imaging to confirm the presence of small crystals embedded in/or between larger crystallites of the prepared Cs 4 PbBr 6 (Figure e–g) . The luminescent spot emitting at ∼520 nm was analyzed by EDX to give a Pb:Br ratio of 2 times higher than other areas, confirming the existence of CsPbBr 3 impurities in the Cs 4 PbBr 6 bulk phase.…”

Section: Pl Of Cs4pbbr6mentioning

confidence: 92%

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Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Jiang

Zhang

et al. 2020

ChemNanoMat

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Metal halide perovskites (MHPs) are promising materials for a range of optoelectronic applications owing to their unique structures and optical properties. The photoluminescence (PL) property of MHPs is crucial for their applications. All‐inorganic MHPs such as CsPbBr3, CsPb2Br5 and Cs4PbBr6, have been widely investigated due to their high PL quantum yield (QY). However, the PL mechanisms of these perovskites still remain controversial and lack a unifying explanation. In this review, we have summarized the recent efforts to reveal the emission process of all‐inorganic cesium lead bromide perovskites nanocrystals (NCs) by utilizing single particle spectroscopy. The recent research advances on the understanding of exciton nature in CsPbBr3 and PL emission originating from intrinsic point defects or impurity CsPbBr3 phase in CsPb2Br5 and Cs4PbBr6 are summarized. Understanding the relationship between the structure and associated PL property of MHPs paves the way for their potential applications.

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“…Unfortunately, the existence of bromide vacancy bring the green emission seems illogical. The incorporation of -OH groups as a defect is considerate to be introduced into Cs 4 PbBr 6 [34], however, through DFT calculations, the bandgap decreases with the introduction of -OH, the bandgap decreases from 3.75 to 3.50 eV ( Fig. 3(e)) without the presence of the sub-bandgap state .…”

Section: Resultsmentioning

confidence: 99%

Extrinsic photoluminescence properties of individual micro-particle of Cs₄PbBr₆ perovskite with “defect” structure

Yang¹,

Wang²,

Yang³

et al. 2019

Opt. Express

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Optical performance of the lead halide perovskites with zero-dimension (0D) structure has been in a hot debate for optoelectronic applications. Here, Cs 4 PbBr 6 hexagonal micro-particles with a remarkable green emission are first fabricated via a low-temperature solution-process employed ethanol as solvent. Our results underline that the existence of bromine vacancies and the introduction of hydroxyl induce a narrowed band gap with the formation of a defect level, which contributes to the extrinsic photoluminescence (PL) properties synergistically. Thanks to the high exciton binding energy and the unique morphology with a regular geometric structure of the as-obtained micro-particles, two-photon pumped amplified spontaneous emission (ASE) and single mode lasing from an individual Cs 4 PbBr 6 particle are realized. Our results not only provide an insight into the origin of optical emission from Cs 4 PbBr 6 , but also demonstrate that the versatile Cs 4 PbBr 6 offers a new opportunity for novel nonlinear photonics applications as an up-conversion laser.

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On the origins of the green luminescence in the “zero-dimensional perovskite” Cs₄PbBr₆: conclusive results from cathodoluminescence imaging

Abstract: Cathodoluminescence imaging reveals that the bright green emission from the zero-dimensional perovskite Cs4PbBr6 is due to nanoscale CsPbBr3 impurities.

Cited by 57 publications

References 36 publications

Optical Characterization of Cesium Lead Bromide Perovskites

Optical Characterization of Cesium Lead Bromide Perovskites

Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Extrinsic photoluminescence properties of individual micro-particle of Cs₄PbBr₆ perovskite with “defect” structure

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On the origins of the green luminescence in the “zero-dimensional perovskite” Cs4PbBr6: conclusive results from cathodoluminescence imaging

Abstract: Cathodoluminescence imaging reveals that the bright green emission from the zero-dimensional perovskite Cs4PbBr6 is due to nanoscale CsPbBr3 impurities.

Cited by 57 publications

References 36 publications

Optical Characterization of Cesium Lead Bromide Perovskites

Optical Characterization of Cesium Lead Bromide Perovskites

Photoluminescence Mechanisms of All‐Inorganic Cesium Lead Bromide Perovskites Revealed by Single Particle Spectroscopy

Extrinsic photoluminescence properties of individual micro-particle of Cs4PbBr6 perovskite with “defect” structure

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On the origins of the green luminescence in the “zero-dimensional perovskite” Cs₄PbBr₆: conclusive results from cathodoluminescence imaging

Extrinsic photoluminescence properties of individual micro-particle of Cs₄PbBr₆ perovskite with “defect” structure