Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3

Sebastian, M.; Peters, J. A.; Stoumpos, C. C.; Im, J.; Kostina, S. S.; Liu, Z.; Kanatzidis, M. G.; Freeman, A. J.; Wessels, B. W.

doi:10.1103/PhysRevB.92.235210

Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors $CsPbB r_{3}$ and $CsPbC l_{3}$

Journal Article · Tue Dec 29 00:00:00 EST 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.92.235210· OSTI ID:1494838

Sebastian, M. ^[1]; Peters, J. A. ^[1]; Stoumpos, C. C. ^[2]; Im, J. ^[3]; Kostina, S. S. ^[1]; Liu, Z. ^[1]; Kanatzidis, M. G. ^[2]; Freeman, A. J. ^[3]; Wessels, B. W. ^[1]

Northwestern Univ., Evanston, IL (United States). Dept. of Material Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy

The ternary compounds CsPbX₃ (X = Br or Cl) have perovskite structures that are being considered for optical and electronic applications such as lasing and gamma-ray detection. An above-band-gap excitonic photoluminescence (PL) band is seen in both CsPbX₃ compounds. An excitonic emission peak centered at 2.98 eV, ~0.1 eV above the room-temperature band gap, is observed for CsPbCl₃. The thermal quenching of the excitonic luminescence is well described by a two-step quenching model, yielding activation energies of 0.057 and 0.0076 eV for high- and low-temperature regimes, respectively. CsPbBr₃ exhibits bound excitonic luminescence peaks located at 2.29 and 2.33 eV that are attributed to recombination involving Br vacancy centers. Activation energies for thermal quenching of the excitonic luminescence of 0.017 and 0.0007 eV were calculated for CsPbBr₃. Temperature-dependent PL experiments reveal unexpected blueshifts for all excitonic emission peaks in CsPbX₃ compounds. A phonon-assisted step-up process leads to the blueshift in CsPbBr₃ emission, while there is a contribution from band-gap widening in CsPbCl₃. Finally, the absence of significant deep level defect luminescence in these compounds makes them attractive candidates for high-resolution, room-temperature radiation detection.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0002522; AC02-06CH11357

OSTI ID:: 1494838

Alternate ID(s):: OSTI ID: 1234041

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 92, Issue 23; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 235 works

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Exciton–phonon interaction in quasi-two dimensional layered (PEA) ₂ (CsPbBr ₃ ) _n−1 PbBr ₄ perovskite Long, Hao; Peng, Xiang; Lu, Jianxun Nanoscale, Vol. 11, Issue 45 https://doi.org/10.1039/c9nr06834a	journal	January 2019
Pathways toward high-performance inorganic perovskite solar cells: challenges and strategies Li, Bo; Fu, Lin; Li, Shuang Journal of Materials Chemistry A, Vol. 7, Issue 36 https://doi.org/10.1039/c9ta04114a	journal	January 2019
CsPbBr ₃ interconnected microwire structure: temperature-related photoluminescence properties and its lasing action Zhang, Canran; Duan, Junjie; Qin, Feifei Journal of Materials Chemistry C, Vol. 7, Issue 34 https://doi.org/10.1039/c9tc02913c	journal	January 2019
Excitation-intensity dependence of shallow and deep-level photoluminescence transitions in semiconductors Spindler, Conrad; Galvani, Thomas; Wirtz, Ludger Journal of Applied Physics, Vol. 126, Issue 17 https://doi.org/10.1063/1.5095235	journal	November 2019
The influence of electrode for electroluminescence devices based on all-inorganic halide perovskite CsPbBr ₃ Yu, Zhuo-Liang; Zhao, Yu-Qing; He, Peng-Bin Journal of Physics: Condensed Matter, Vol. 32, Issue 6 https://doi.org/10.1088/1361-648x/ab50cf	journal	November 2019
Comparison of superstar CsPbBr ₃ and classical LaPO ₄ :Tb ³⁺ ,Ce ³⁺ green-emitting nanophosphors Fu, Yu; He, Xianghong; Hu, Jiapei Materials Research Express, Vol. 6, Issue 5 https://doi.org/10.1088/2053-1591/ab0165	journal	February 2019
Assessment of the exact-exchange-only Kohn-Sham method for the calculation of band structures for transition metal oxide and metal halide perovskites Trushin, Egor; Fromm, Lukas; Görling, Andreas Physical Review B, Vol. 100, Issue 7 https://doi.org/10.1103/physrevb.100.075205	journal	August 2019
Carrier recombination mechanism in $CsPbB r_{3}$ revealed by time-resolved photoluminescence spectroscopy Peters, J. A.; Liu, Zhifu; Yu, Ruihan Physical Review B, Vol. 100, Issue 23 https://doi.org/10.1103/physrevb.100.235305	journal	December 2019
Alloy-Free Band Gap Tuning across the Visible Spectrum Makin, Robert A.; York, Krystal; Durbin, Steven M. Physical Review Letters, Vol. 122, Issue 25 https://doi.org/10.1103/physrevlett.122.256403	journal	June 2019
Impact of organic molecule rotation on the optoelectronic properties of hybrid halide perovskites Xu, Qiaoling; Stroppa, Alessandro; Lv, Jian Physical Review Materials, Vol. 3, Issue 12 https://doi.org/10.1103/physrevmaterials.3.125401	journal	December 2019
Frequency upconverted amplified spontaneous emission and lasing from inorganic perovskite under simultaneous six-photon absorption Yang, Decheng; Chu, Shenglong; Wang, Yunfeng Optics Letters, Vol. 43, Issue 9 https://doi.org/10.1364/ol.43.002066	journal	January 2018
Long-living nonlinear behavior in CsPbBr3 carrier recombination dynamics Gabelloni, Fabio; Biccari, Francesco; Falsini, Naomi Nanophotonics, Vol. 8, Issue 9 https://doi.org/10.1515/nanoph-2019-0013	journal	April 2019
Materials Discovery of Stable and Nontoxic Halide Perovskite Materials for High‐Efficiency Solar Cells Jacobs, Ryan; Luo, Guangfu; Morgan, Dane Advanced Functional Materials, Vol. 29, Issue 23 https://doi.org/10.1002/adfm.201804354	journal	April 2019
Inorganic and Layered Perovskites for Optoelectronic Devices Fakharuddin, Azhar; Shabbir, Umair; Qiu, Weiming Advanced Materials, Vol. 31, Issue 47 https://doi.org/10.1002/adma.201807095	journal	September 2018
Halide-Perovskite Resonant Nanophotonics Makarov, Sergey; Furasova, Aleksandra; Tiguntseva, Ekaterina Advanced Optical Materials, Vol. 7, Issue 1 https://doi.org/10.1002/adom.201800784	journal	August 2018
On the structure, synthesis, and characterization of ultrafast blue-emitting CsPbBr ₃ nanoplatelets Tomanová, Kateřina; Čuba, Václav; Brik, Mikhail G. APL Materials, Vol. 7, Issue 1 https://doi.org/10.1063/1.5079300	journal	January 2019
Coherent exciton-phonon coupling in perovskite semiconductor nanocrystals studied by two-dimensional electronic spectroscopy Zhao, Wei; Qin, Zhengyuan; Zhang, Chunfeng Applied Physics Letters, Vol. 115, Issue 24 https://doi.org/10.1063/1.5130636	journal	December 2019
Nonempirical hybrid functionals for band gaps of inorganic metal-halide perovskites Bischoff, Thomas; Wiktor, Julia; Chen, Wei Physical Review Materials, Vol. 3, Issue 12 https://doi.org/10.1103/physrevmaterials.3.123802	journal	December 2019
Halide-Perovskite Resonant Nanophotonics Makarov, Sergey; Furasova, Aleksandra; Tiguntseva, Ekaterina arXiv https://doi.org/10.48550/arxiv.1806.08917	preprint	January 2018
Materials Discovery of Stable and Nontoxic Halide Perovskite Materials for High-Efficiency Solar Cells Jacobs, Ryan; Luo, Guangfu; Morgan, Dane arXiv https://doi.org/10.48550/arxiv.1904.05690	text	January 2019

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
photoluminescence (PL)
exciton emission
gamma-ray detection
perovskite halides
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Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbB r 3 and CsPbC l 3

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