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Title: Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites

Abstract

The strong spin–orbit coupling (SOC) in lead halide perovskites, when inversion symmetry is lifted, has provided opportunities for investigating the Rashba effect in these systems. Moreover, the strong orbital moment, which, in turn, impacts the spin-pair in singlet and triplet electronic states, plays a significant role in enhancing the optoelectronic properties in the presence of external magnetic fields in lead halide perovskites. Here, we investigate the effect of weak magnetic fields (<1 T) on the photoluminescence (PL) properties of CsPbBr3 nanocrystals with and without Ruddlesden–Popper (RP) faults and single crystals of CH3NH3PbBr3 . Along with an enhancement in the PL intensity as a function of an external magnetic field, which is observed in both lead bromide perovskites, the PL emission red-shifts in CsPbBr3 nanocrystals. Density-functional theory calculations of the electronic band-edge in CsPbBr3 show almost no change in the energy gap as a function of the external magnetic field. The experimental results, thus, suggest the role of mixing of the triplet and singlet excitonic states under weak magnetic fields. This is further deduced from an enhancement in PL lifetimes as a function of the field in CsPbBr3⁠. In CH3NH3PbBr3⁠, an increase in PL intensity is observed under weak magnetic fields;more » however, no changes in the peak energy or PL lifetimes are observed. The internal magnetic fields due to SOC are characterized for all three samples and found to be the highest for CsPbBr3 nanocrystals with RP faults.« less

Authors:
 [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Missouri, Columbia, MO (United States)
Publication Date:
Research Org.:
Univ. of Missouri, Columbia, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
1979054
Alternate Identifier(s):
OSTI ID: 1856622
Grant/Contract Number:  
SC0019109; DMR-1807263; ECCS-1827846
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 131; Journal Issue: 12; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Physics; Density functional theory; Band gap; Spin-orbit interactions; Magnetic fields; Photoluminescence; Nanocrystals; Optoelectronic properties; Crystal structure; Inorganic compounds; Perovskites

Citation Formats

Butler, Rory, Burns, Randy, Babaian, Dallar, Anderson, Matthew J., Ullrich, Carsten A., Morrell, Maria V., Xing, Yangchuan, Lee, Jaewon, Yu, Ping, and Guha, Suchismita. Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites. United States: N. p., 2022. Web. doi:10.1063/5.0085947.
Butler, Rory, Burns, Randy, Babaian, Dallar, Anderson, Matthew J., Ullrich, Carsten A., Morrell, Maria V., Xing, Yangchuan, Lee, Jaewon, Yu, Ping, & Guha, Suchismita. Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites. United States. https://doi.org/10.1063/5.0085947
Butler, Rory, Burns, Randy, Babaian, Dallar, Anderson, Matthew J., Ullrich, Carsten A., Morrell, Maria V., Xing, Yangchuan, Lee, Jaewon, Yu, Ping, and Guha, Suchismita. Mon . "Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites". United States. https://doi.org/10.1063/5.0085947. https://www.osti.gov/servlets/purl/1979054.
@article{osti_1979054,
title = {Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites},
author = {Butler, Rory and Burns, Randy and Babaian, Dallar and Anderson, Matthew J. and Ullrich, Carsten A. and Morrell, Maria V. and Xing, Yangchuan and Lee, Jaewon and Yu, Ping and Guha, Suchismita},
abstractNote = {The strong spin–orbit coupling (SOC) in lead halide perovskites, when inversion symmetry is lifted, has provided opportunities for investigating the Rashba effect in these systems. Moreover, the strong orbital moment, which, in turn, impacts the spin-pair in singlet and triplet electronic states, plays a significant role in enhancing the optoelectronic properties in the presence of external magnetic fields in lead halide perovskites. Here, we investigate the effect of weak magnetic fields (<1 T) on the photoluminescence (PL) properties of CsPbBr3 nanocrystals with and without Ruddlesden–Popper (RP) faults and single crystals of CH3NH3PbBr3 . Along with an enhancement in the PL intensity as a function of an external magnetic field, which is observed in both lead bromide perovskites, the PL emission red-shifts in CsPbBr3 nanocrystals. Density-functional theory calculations of the electronic band-edge in CsPbBr3 show almost no change in the energy gap as a function of the external magnetic field. The experimental results, thus, suggest the role of mixing of the triplet and singlet excitonic states under weak magnetic fields. This is further deduced from an enhancement in PL lifetimes as a function of the field in CsPbBr3⁠. In CH3NH3PbBr3⁠, an increase in PL intensity is observed under weak magnetic fields; however, no changes in the peak energy or PL lifetimes are observed. The internal magnetic fields due to SOC are characterized for all three samples and found to be the highest for CsPbBr3 nanocrystals with RP faults.},
doi = {10.1063/5.0085947},
journal = {Journal of Applied Physics},
number = 12,
volume = 131,
place = {United States},
year = {Mon Mar 28 00:00:00 EDT 2022},
month = {Mon Mar 28 00:00:00 EDT 2022}
}

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