Publisher Correction: Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

Arunkumar, Paulraj; Cho, Han Bin; Gil, Kyeong Hun; Unithrattil, Sanjith; Kim, Yoon Hwa

doi:10.1038/s41467-018-07910-7

Cited by 4 publications

(3 citation statements)

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“…Surface of nanocrystals is essential to optimize their properties and performance in device applications, , in particular for materials like lead halide perovskites whose “easy to make, easy to break” nature is well known. − Because of the successful use of nanocrystalline MAPbX 3 as the light harvester in solar cells, there has been enormous development of perovskite NCs of diverse compositions for employment in high-performance optoelectronic devices. − All-inorganic cesium lead halide perovskite nanocrystals (PNCs) attract a lot of interest owing to demonstrations of the high photoluminescence quantum yield (PLQY), narrow emission linewidth, wide color gamut, intrinsic defect tolerance, and better chemical stability compared to their organic–inorganic counterparts. − Their practical utilization nevertheless remains challenging as the structural integrity and the properties of the solution-processed nanocrystals exhibit degradation in solid films, as well as under the influence of environmental factors (humidity/heat/light). − This instability is generally attributed to their soft ionic nature and labile surface . With isolation of [PbX 6 ] octahedra in crystal lattices, the development of lower dimensional perovskites, especially zero-dimensional (0D) Cs 4 PbBr 6 , has shown potential for improvement in stability and retaining high QY in the solid state compared to three-dimensional (3D) CsPbX 3 nanocrystals. − The microscopic origin of the green emission in Cs 4 PbBr 6 is, however, still debated, and the material is not completely immune to environmental effects. ,,− …”

Section: Introductionmentioning

confidence: 99%

Interface Matters: Enhanced Photoluminescence and Long-Term Stability of Zero-Dimensional Cesium Lead Bromide Nanocrystals via Gas-Phase Aluminum Oxide Encapsulation

Bose

Zheng

Guo

et al. 2020

ACS Appl. Mater. Interfaces

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Cesium lead halide perovskite nanocrystals (PNCs), while possessing facile chemical synthesis routes and high photoluminescence (PL) properties, are still challenged by issues of instability and degradation. Although atomic layer deposition (ALD) of metal oxides has been one of the common encapsulation approaches for longer term stability, its application inevitably resulted in severe loss of emission efficiency and at times partial loss of structural integrity of perovskites, creating a bottleneck in its practical viability. We demonstrate a nondestructive modified gasphase technique with codeposition of both precursors trimethylaluminum and water to dramatically enhance the PL emission in zero-dimensional (0D) Cs 4 PbBr 6 PNCs via alumina encapsulation. X-ray photoelectron spectroscopy analysis of Cs 4 PbBr 6 films reveals the alumina deposition to be accompanied by elemental composition changes, particularly by the reduction of the excessive cesium content. Ab initio density functional theory simulations further unfold that the presence of excess Cs on the surface of PNCs leads to decomposition of structural [PbBr 6 ] 4− octahedra in the 0D perovskite lattice, which can be prevented in the presence of added hydroxyl groups. Our study thus unveils the pivotal role of the PNC surface composition and treatment in the process of its interaction with metal oxide precursors to control the PL properties as well as the stability of PNCs, providing an unprecedented way to use the conventional ALD technique for their successful integration into optoelectronic and photonic devices with improved properties.

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Section: Introductionmentioning

confidence: 99%

Interface Matters: Enhanced Photoluminescence and Long-Term Stability of Zero-Dimensional Cesium Lead Bromide Nanocrystals via Gas-Phase Aluminum Oxide Encapsulation

Bose

Zheng

Guo

et al. 2020

ACS Appl. Mater. Interfaces

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“…There are also numerous reports which have shown an increase in the carrier lifetime and increase in the PLQY in Mn-doped CsPbCl 3 , thus making it a good candidate for photovoltaic applications. 56,57 Our studies provide useful insight into the origins of the long recombination lifetimes observed in Mndoped CsPbCl 3 underpinning a stabilized polaron formation. The clear experimental evidence of an activated phonon mode due to polaronic origin can be used as a marker to understand the structure and property relationship in these LHPs, which is fundamental for using them as potential materials for optoelectronic applications.…”

Section: Resultsmentioning

confidence: 88%

“…Overall, Mn doping stabilizes the polaronic mode, but the effects are more pronounced in Cl-rich systems than with Br incorporation. One of the previous studies by Arunkumar et al has shown that upon Mn doping between 5% and 10%, the covalent character increases in the (Pb/Mn)–Cl bond as opposed to the usual more electrostatic bond. As a result, the distortion in the lattice increases, which leads to polaron formation.…”

Section: Resultsmentioning

confidence: 93%

Polaronic Signatures in Doped and Undoped Cesium Lead Halide Perovskite Nanocrystals through a Photoinduced Raman Mode

Jain

Mazumder

Pradeep

et al. 2022

ACS Appl. Mater. Interfaces

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Lead halide perovskites (LHPs) are promising candidates for photovoltaic applications as they exhibit large carrier diffusion lengths and long carrier lifetimes among many other interesting properties. One of the widely accepted mechanisms for these properties is polaron formation, which is mainly driven by octahedral distortions of the inorganic framework. Since structure modifications of the framework largely affect associated distortions, we investigated Mn-doped and undoped CsPbX3 (where X = Cl, Br, Cl/Br) using a local probe via micro-Raman spectroscopy and density functional theory (DFT) calculations for polaron formation. Our results highlight a new vibrational lattice mode at 132 cm–1 due to polaronic distortion upon photoinduction. From the DFT studies, we have shown that the polaronic states are dominated by the B-site cation in the perovskite structure, but it is the strong covalent overlap of the halide which determines its stability. This elucidation to map polaronic signatures with excellent spatial resolution using traditional Raman spectroscopy can be used as a simple tool to understand the structural changes and their impacted electronic properties and thus design superior devices using its in situ applications.

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Large and Small Polarons in Highly Efficient and Stable Organic‐Inorganic Lead Halide Perovskite Solar Cells: A Review

Nandi,

Shin,

Park

et al. 2024

Solar RRL

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Polarons, which arise from the intricate interplay between excess electrons and/or holes and lattice vibrations (phonons), represent quasiparticles pivotal to the electronic behavior of materials. This review reaffirms the established classification of small and large polarons, emphasizing its relevance in the context of recent advances in understanding lead halide perovskites' behavior. The distinct characteristics of large and small polarons stem from the electron–phonon interaction range, which exerts a profound influence on materials’ characteristics and functionalities. Concurrently, lead halides have emerged with exceptional opto‐electronic properties, featuring prolonged carrier lifetimes, low recombination rates, high defect tolerance, and moderate charge carrier mobilities; these characteristics make them a compelling contender for integration of optoelectronic devices. In this review, the formation of both small and large polarons within the lattice of lead halide perovskites, elucidating their role in protecting photogenerated charge carriers from recombination processes, is discussed. As optoelectronic devices continue to advance, this review underscores the importance of unraveling polaron dynamics to pave the way for innovative strategies for enhancing the performance of next‐generation photovoltaic technologies. Future research should explore novel polaronic effects using advanced computational and experimental techniques, enhancing our understanding and unlocking new applications in materials science and device engineering.

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Publisher Correction: Probing molecule-like isolated octahedra via phase stabilization of zero-dimensional cesium lead halide nanocrystals

Cited by 4 publications

References 0 publications

Interface Matters: Enhanced Photoluminescence and Long-Term Stability of Zero-Dimensional Cesium Lead Bromide Nanocrystals via Gas-Phase Aluminum Oxide Encapsulation

Interface Matters: Enhanced Photoluminescence and Long-Term Stability of Zero-Dimensional Cesium Lead Bromide Nanocrystals via Gas-Phase Aluminum Oxide Encapsulation

Polaronic Signatures in Doped and Undoped Cesium Lead Halide Perovskite Nanocrystals through a Photoinduced Raman Mode

Large and Small Polarons in Highly Efficient and Stable Organic‐Inorganic Lead Halide Perovskite Solar Cells: A Review

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