Atomic-scale understanding on the physics and control of intrinsic point defects in lead halide perovskites

Jun Kang; Jingbo Li; Su-Huai Wei

doi:10.1063/5.0052402

Origin of Luminescent Centers and Edge States in Low-Dimensional Lead Halide Perovskites: Controversies, Challenges and Instructive Approaches

Nano-Micro Letters ◽

10.1007/s40820-019-0254-4 ◽

2019 ◽

Vol 11 (1) ◽

Cited By ~ 17

Author(s):

Jiming Bao ◽

Viktor G. Hadjiev

Keyword(s):

Point Defects ◽

Density Functional ◽

High Efficiency ◽

Deep Level ◽

Edge States ◽

Intrinsic Point Defects ◽

Halide Perovskites ◽

Low Dimensional ◽

Luminescent Centers ◽

Lead Halide

Abstract With only a few deep-level defect states having a high formation energy and dominance of shallow carrier non-trapping defects, the defect-tolerant electronic and optical properties of lead halide perovskites have made them appealing materials for high-efficiency, low-cost, solar cells and light-emitting devices. As such, recent observations of apparently deep-level and highly luminescent states in low-dimensional perovskites have attracted enormous attention as well as intensive debates. The observed green emission in 2D CsPb2Br5 and 0D Cs4PbBr6 poses an enigma over whether it is originated from intrinsic point defects or simply from highly luminescent CsPbBr3 nanocrystals embedded in the otherwise transparent wide band gap semiconductors. The nature of deep-level edge emission in 2D Ruddlesden–Popper perovskites is also not well understood. In this mini review, the experimental evidences that support the opposing interpretations are analyzed, and challenges and root causes for the controversy are discussed. Shortcomings in the current density functional theory approaches to modeling of properties and intrinsic point defects in lead halide perovskites are also noted. Selected experimental approaches are suggested to better correlate property with structure of a material and help resolve the controversies. Understanding and identification of the origin of luminescent centers will help design and engineer perovskites for wide device applications.

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Intrinsic doping limit and defect-assisted luminescence in Cs4PbBr6

Journal of Materials Chemistry A ◽

10.1039/c9ta06874k ◽

2019 ◽

Vol 7 (35) ◽

pp. 20254-20261 ◽

Cited By ~ 15

Author(s):

Young-Kwang Jung ◽

Joaquín Calbo ◽

Ji-Sang Park ◽

Lucy D. Whalley ◽

Sunghyun Kim ◽

...

Keyword(s):

Point Defects ◽

Halide Perovskites ◽

Lead Halide

The type and behaviour of point defects in 0D lead halide perovskites is found to be radically different from their 3D counterparts

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Atomic-scale microstructure of metal halide perovskite

Science ◽

10.1126/science.abb5940 ◽

2020 ◽

Vol 370 (6516) ◽

pp. eabb5940 ◽

Cited By ~ 1

Author(s):

Mathias Uller Rothmann ◽

Judy S. Kim ◽

Juliane Borchert ◽

Kilian B. Lohmann ◽

Colum M. O’Leary ◽

...

Keyword(s):

Scanning Transmission Electron Microscopy ◽

Atomic Scale ◽

Energy Applications ◽

Transmission Electron ◽

Metal Halide Perovskite ◽

Scanning Transmission ◽

Halide Perovskites ◽

Crystalline Solar Cell ◽

Lead Halide ◽

Perovskite Lattice

Hybrid organic-inorganic perovskites have high potential as materials for solar energy applications, but their microscopic properties are still not well understood. Atomic-resolution scanning transmission electron microscopy has provided invaluable insights for many crystalline solar cell materials, and we used this method to successfully image formamidinium lead triiodide [CH(NH2)2PbI3] thin films with a low dose of electron irradiation. Such images reveal a highly ordered atomic arrangement of sharp grain boundaries and coherent perovskite/PbI2 interfaces, with a striking absence of long-range disorder in the crystal. We found that beam-induced degradation of the perovskite leads to an initial loss of formamidinium [CH(NH2)2+] ions, leaving behind a partially unoccupied perovskite lattice, which explains the unusual regenerative properties of these materials. We further observed aligned point defects and climb-dissociated dislocations. Our findings thus provide an atomic-level understanding of technologically important lead halide perovskites.

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Determining Atomic-Scale Structure and Composition of Organo-Lead Halide Perovskites by Combining High-Resolution X-ray Absorption Spectroscopy and First-Principles Calculations

ACS Energy Letters ◽

10.1021/acsenergylett.7b00182 ◽

2017 ◽

Vol 2 (5) ◽

pp. 1183-1189 ◽

Cited By ~ 11

Author(s):

Walter S. Drisdell ◽

Linn Leppert ◽

Carolin M. Sutter-Fella ◽

Yufeng Liang ◽

Yanbo Li ◽

...

Keyword(s):

High Resolution ◽

Absorption Spectroscopy ◽

First Principles ◽

Scale Structure ◽

Atomic Scale ◽

First Principles Calculations ◽

X Ray ◽

Halide Perovskites ◽

X Ray Absorption ◽

Lead Halide

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Point Defects, Diffusion and Gettering in Silicon

MRS Proceedings ◽

10.1557/proc-469-13 ◽

1997 ◽

Vol 469 ◽

Cited By ~ 4

Author(s):

U. Gösele ◽

D. Conrad ◽

P. Werner ◽

Q.-Y. Tong ◽

R. Gafiteanu ◽

...

Keyword(s):

Point Defects ◽

Diffusion Processes ◽

Silicon On Insulator ◽

Intrinsic Point Defects ◽

The Status ◽

Long Time ◽

Effective Diffusivities ◽

And Control ◽

Soi Substrates ◽

Measurement And Control

ABSTRACTThe status of our knowledge on intrinsic point defects and diffusion mechanisms is reviewed. Special attention is given to the question of the possible role of carbon in influencing effective diffusivities of intrinsic point defects and the resulting consequences for the values of vacancy and self-interstitial thermal equilibrium concentrations and diffusivities. It is pointed out that we might have to deal with the unfortunate situation that the effective diffusivities of intrinsic point defects might be influenced already by a carbon concentration which is below the detection limit and therefore not amenable to measurement and control. Whereas dopant diffusion processes have been modeled and simulated for a long time the first attempts to quantitatively simulate various gettering processes have just started as will be described in the paper. Finally, the subject of microcrack formation in hydrogen implanted silicon will be dealt with as used for the so-called “smart-cut” process for fabricating silicon-on-insulator (SOI) substrates with thin and uniform silicon layers by wafer bonding. Presently no quantitative treatment of this fascinating hydrogen agglomeration phenomenon is available.

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