Photoluminescence spectroscopy of excitonic emission in CsPbCl3 perovskite single crystals

John A. Peters; Zhifu Liu; Michael C. De Siena; Mercouri G. Kanatzidis; Bruce W. Wessels

doi:10.1016/j.jlumin.2021.118661

Photoluminescence spectroscopy of excitonic emission in CsPbCl₃ perovskite single crystals

John A. Peters, Zhifu Liu, Michael C. De Siena, Mercouri G. Kanatzidis, Bruce W. Wessels^*

^*Corresponding author for this work

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

25 Scopus citations

Abstract

We analyzed low-temperature photoluminescence (PL) and the band edge excitonic emission in bulk halide perovskite CsPbCl₃ single crystals. Strong near band edge excitonic emission is observed at 420 nm and a series of excitonic states was observed. Temperature-dependent PL measurements on cesium lead chloride over a wide temperature range from 13 K to 295 K revealed significant electron phonon coupling with a Huang-Rhys parameter ranging from 1.34 to 3.38. A primary experimental finding is that the near band edge PL emission shows existence of multiple sharp features at low temperatures that are attributable to free excitons, bound excitons, and their phonon replicas. The PL also shows evidence of band tailing effects due to disorder. We investigated the recombination mechanism of photogenerated charge carriers by means of time-resolved PL (TR-PL) spectroscopy at low temperatures and various excitation powers and observed competing mono- and bimolecular recombination processes. A dynamic model is proposed to describe the TR-PL. We observed both long-lived and short-lived recombination where the short-lived time decay is attributed to free exciton recombination, whereas the long-lived decay to bound exciton recombination involving traps due to intrinsic disorder.

Original language	English (US)
Article number	118661
Journal	Journal of Luminescence
Volume	243
DOIs	https://doi.org/10.1016/j.jlumin.2021.118661
State	Published - Mar 2022

Funding

This research is sponsored by the Defense Threat Reduction Agency (DTRA) as part of the Interaction of Ionizing Radiation with Matter University Research Alliance (IIRM-URA) under contract number HDTRA1-20-2-0002 . This work made use of the Materials Processing and Microfabrication Facility supported by the MRSEC program of the National Science Foundation ( DMR-1720139 ) at the Materials Research Center of Northwestern University . This work made use of the Perkin Elmer Lambda 1050 instrument at the Keck Biophysics facility at Northwestern University, which is supported by the Robert H. Lurie Comprehensive Cancer Center ( NCI CCSG P30 CA060553 ). This work made use of the IMSERC Physical Characterization facility at Northwestern University , which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource ( NSF ECCS-2025633 ), and Northwestern University .

Keywords

CsPbCl single crystal
Electron-phonon interaction
Photoluminescence
Thermal expansion

ASJC Scopus subject areas

Biophysics
Atomic and Molecular Physics, and Optics
General Chemistry
Biochemistry
Condensed Matter Physics

Access to Document

10.1016/j.jlumin.2021.118661

Cite this

@article{f9710997df7d4060a1063ea1aeb7f015,

title = "Photoluminescence spectroscopy of excitonic emission in CsPbCl3 perovskite single crystals",

abstract = "We analyzed low-temperature photoluminescence (PL) and the band edge excitonic emission in bulk halide perovskite CsPbCl3 single crystals. Strong near band edge excitonic emission is observed at 420 nm and a series of excitonic states was observed. Temperature-dependent PL measurements on cesium lead chloride over a wide temperature range from 13 K to 295 K revealed significant electron phonon coupling with a Huang-Rhys parameter ranging from 1.34 to 3.38. A primary experimental finding is that the near band edge PL emission shows existence of multiple sharp features at low temperatures that are attributable to free excitons, bound excitons, and their phonon replicas. The PL also shows evidence of band tailing effects due to disorder. We investigated the recombination mechanism of photogenerated charge carriers by means of time-resolved PL (TR-PL) spectroscopy at low temperatures and various excitation powers and observed competing mono- and bimolecular recombination processes. A dynamic model is proposed to describe the TR-PL. We observed both long-lived and short-lived recombination where the short-lived time decay is attributed to free exciton recombination, whereas the long-lived decay to bound exciton recombination involving traps due to intrinsic disorder.",

keywords = "CsPbCl single crystal, Electron-phonon interaction, Photoluminescence, Thermal expansion",

author = "Peters, \{John A.\} and Zhifu Liu and \{De Siena\}, \{Michael C.\} and Kanatzidis, \{Mercouri G.\} and Wessels, \{Bruce W.\}",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

year = "2022",

month = mar,

doi = "10.1016/j.jlumin.2021.118661",

language = "English (US)",

volume = "243",

journal = "Journal of Luminescence",

issn = "0022-2313",

publisher = "Elsevier B.V.",

}

TY - JOUR

T1 - Photoluminescence spectroscopy of excitonic emission in CsPbCl3 perovskite single crystals

AU - Peters, John A.

AU - Liu, Zhifu

AU - De Siena, Michael C.

AU - Kanatzidis, Mercouri G.

AU - Wessels, Bruce W.

PY - 2022/3

Y1 - 2022/3

N2 - We analyzed low-temperature photoluminescence (PL) and the band edge excitonic emission in bulk halide perovskite CsPbCl3 single crystals. Strong near band edge excitonic emission is observed at 420 nm and a series of excitonic states was observed. Temperature-dependent PL measurements on cesium lead chloride over a wide temperature range from 13 K to 295 K revealed significant electron phonon coupling with a Huang-Rhys parameter ranging from 1.34 to 3.38. A primary experimental finding is that the near band edge PL emission shows existence of multiple sharp features at low temperatures that are attributable to free excitons, bound excitons, and their phonon replicas. The PL also shows evidence of band tailing effects due to disorder. We investigated the recombination mechanism of photogenerated charge carriers by means of time-resolved PL (TR-PL) spectroscopy at low temperatures and various excitation powers and observed competing mono- and bimolecular recombination processes. A dynamic model is proposed to describe the TR-PL. We observed both long-lived and short-lived recombination where the short-lived time decay is attributed to free exciton recombination, whereas the long-lived decay to bound exciton recombination involving traps due to intrinsic disorder.

AB - We analyzed low-temperature photoluminescence (PL) and the band edge excitonic emission in bulk halide perovskite CsPbCl3 single crystals. Strong near band edge excitonic emission is observed at 420 nm and a series of excitonic states was observed. Temperature-dependent PL measurements on cesium lead chloride over a wide temperature range from 13 K to 295 K revealed significant electron phonon coupling with a Huang-Rhys parameter ranging from 1.34 to 3.38. A primary experimental finding is that the near band edge PL emission shows existence of multiple sharp features at low temperatures that are attributable to free excitons, bound excitons, and their phonon replicas. The PL also shows evidence of band tailing effects due to disorder. We investigated the recombination mechanism of photogenerated charge carriers by means of time-resolved PL (TR-PL) spectroscopy at low temperatures and various excitation powers and observed competing mono- and bimolecular recombination processes. A dynamic model is proposed to describe the TR-PL. We observed both long-lived and short-lived recombination where the short-lived time decay is attributed to free exciton recombination, whereas the long-lived decay to bound exciton recombination involving traps due to intrinsic disorder.

KW - CsPbCl single crystal

KW - Electron-phonon interaction

KW - Photoluminescence

KW - Thermal expansion

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