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.
N1 - Funding Information:
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 .
Publisher Copyright:
© 2021 Elsevier B.V.
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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U2 - 10.1016/j.jlumin.2021.118661
DO - 10.1016/j.jlumin.2021.118661
M3 - Article
AN - SCOPUS:85120934170
SN - 0022-2313
VL - 243
JO - Journal of Luminescence
JF - Journal of Luminescence
M1 - 118661
ER -