Superparamagnetism of Green Emissive Cs4PbBr6Zero-Dimensional Perovskite Crystals

Ji Hyun Cha; Hyun Jong Lee; Sun Ha Kim; Kyoung Chul Ko; Byoung Jin Suh; Oc Hee Han; Duk Young Jung

doi:10.1021/acsenergylett.0c00964

Superparamagnetism of Green Emissive Cs₄PbBr₆Zero-Dimensional Perovskite Crystals

Ji Hyun Cha
, Hyun Jong Lee
, Sun Ha Kim
, Kyoung Chul Ko
, Byoung Jin Suh
, Oc Hee Han
, Duk Young Jung

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

40 Scopus citations

Abstract

We report the characteristic magnetic behaviors of nonemissive (N416) and green emissive (G416) Cs4PbBr6 perovskite crystals. N416 exhibits a diamagnetic behavior, while G416 shows an additional superparamagnetic behavior, demonstrating the existence of paramagnetic electron spins in the G416. Although G416 and N416 crystals belong to the same rhombohedra unit cell with zero-dimensional (0D) connectivity of the [PbBr6]4- octahedron, the G416 crystal has a smaller unit cell volume than N416. 133Cs magic-angle-spinning NMR spectroscopy demonstrated the presence of defects in G416 and the extremely low concentration of a CsPbBr3 phase in both crystals. The DFT calculation results for the defected N416 crystal structure possessing Br vacancies included the experimentally observed blue shift of the high-energy optical band in the G416, which reinforces the existence of intrinsic defects in the G416. Our findings reveal that the unusual green emission and paramagnetic domains stem from structural defects in the 0D perovskites.

Original language	English
Pages (from-to)	2208-2216
Number of pages	9
Journal	ACS Energy Letters
Volume	5
Issue number	7
DOIs	https://doi.org/10.1021/acsenergylett.0c00964
State	Published - 10 Jul 2020

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title = "Superparamagnetism of Green Emissive Cs4PbBr6Zero-Dimensional Perovskite Crystals",

abstract = "We report the characteristic magnetic behaviors of nonemissive (N416) and green emissive (G416) Cs4PbBr6 perovskite crystals. N416 exhibits a diamagnetic behavior, while G416 shows an additional superparamagnetic behavior, demonstrating the existence of paramagnetic electron spins in the G416. Although G416 and N416 crystals belong to the same rhombohedra unit cell with zero-dimensional (0D) connectivity of the [PbBr6]4- octahedron, the G416 crystal has a smaller unit cell volume than N416. 133Cs magic-angle-spinning NMR spectroscopy demonstrated the presence of defects in G416 and the extremely low concentration of a CsPbBr3 phase in both crystals. The DFT calculation results for the defected N416 crystal structure possessing Br vacancies included the experimentally observed blue shift of the high-energy optical band in the G416, which reinforces the existence of intrinsic defects in the G416. Our findings reveal that the unusual green emission and paramagnetic domains stem from structural defects in the 0D perovskites.",

author = "Cha, \{Ji Hyun\} and Lee, \{Hyun Jong\} and Kim, \{Sun Ha\} and Ko, \{Kyoung Chul\} and Suh, \{Byoung Jin\} and Han, \{Oc Hee\} and Jung, \{Duk Young\}",

note = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

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day = "10",

doi = "10.1021/acsenergylett.0c00964",

language = "English",

volume = "5",

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journal = "ACS Energy Letters",

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T1 - Superparamagnetism of Green Emissive Cs4PbBr6Zero-Dimensional Perovskite Crystals

AU - Cha, Ji Hyun

AU - Lee, Hyun Jong

AU - Kim, Sun Ha

AU - Ko, Kyoung Chul

AU - Suh, Byoung Jin

AU - Han, Oc Hee

AU - Jung, Duk Young

PY - 2020/7/10

Y1 - 2020/7/10

N2 - We report the characteristic magnetic behaviors of nonemissive (N416) and green emissive (G416) Cs4PbBr6 perovskite crystals. N416 exhibits a diamagnetic behavior, while G416 shows an additional superparamagnetic behavior, demonstrating the existence of paramagnetic electron spins in the G416. Although G416 and N416 crystals belong to the same rhombohedra unit cell with zero-dimensional (0D) connectivity of the [PbBr6]4- octahedron, the G416 crystal has a smaller unit cell volume than N416. 133Cs magic-angle-spinning NMR spectroscopy demonstrated the presence of defects in G416 and the extremely low concentration of a CsPbBr3 phase in both crystals. The DFT calculation results for the defected N416 crystal structure possessing Br vacancies included the experimentally observed blue shift of the high-energy optical band in the G416, which reinforces the existence of intrinsic defects in the G416. Our findings reveal that the unusual green emission and paramagnetic domains stem from structural defects in the 0D perovskites.

AB - We report the characteristic magnetic behaviors of nonemissive (N416) and green emissive (G416) Cs4PbBr6 perovskite crystals. N416 exhibits a diamagnetic behavior, while G416 shows an additional superparamagnetic behavior, demonstrating the existence of paramagnetic electron spins in the G416. Although G416 and N416 crystals belong to the same rhombohedra unit cell with zero-dimensional (0D) connectivity of the [PbBr6]4- octahedron, the G416 crystal has a smaller unit cell volume than N416. 133Cs magic-angle-spinning NMR spectroscopy demonstrated the presence of defects in G416 and the extremely low concentration of a CsPbBr3 phase in both crystals. The DFT calculation results for the defected N416 crystal structure possessing Br vacancies included the experimentally observed blue shift of the high-energy optical band in the G416, which reinforces the existence of intrinsic defects in the G416. Our findings reveal that the unusual green emission and paramagnetic domains stem from structural defects in the 0D perovskites.

UR - https://www.scopus.com/pages/publications/85089534256

U2 - 10.1021/acsenergylett.0c00964

DO - 10.1021/acsenergylett.0c00964

M3 - Article

AN - SCOPUS:85089534256

SN - 2380-8195

VL - 5

SP - 2208

EP - 2216

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 7

ER -

Superparamagnetism of Green Emissive Cs₄PbBr₆Zero-Dimensional Perovskite Crystals

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