Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

Chenkun Zhou, Michael Worku, Jennifer Neu, Haoran Lin, Yu Tian, Sujin Lee, Yan Zhou, Dan Han, Shiyou Chen, Ayou Hao, Peter I. Djurovich, Theo Siegrist, Mao Hua Du, Biwu Ma

Research output: Contribution to journalArticlepeer-review

200 Scopus citations

Abstract

We report the synthesis and characterization of (Ph4P)2SbCl5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph4P+) and antimony (Sb3+) chloride salts, (Ph4P)2SbCl5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl52- with strong excited-state structural distortion. Interestingly, (Ph4P)2SbCl5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.

Original languageEnglish
Pages (from-to)2374-2378
Number of pages5
JournalChemistry of Materials
Volume30
Issue number7
DOIs
StatePublished - Apr 10 2018
Externally publishedYes

Funding

The authors acknowledge the support from the National Science Foundation (DMR-1709116 and CHE-1664661). The work at the Oak Ridge National Laboratory was supported by the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. D.H. and S.C. were supported by the State Scholarship Fund in China and CC of ECNU. The authors thank Dr. Kenneth Hanson at the Florida State University for the access to a spectrophotometer and Dr. Hanwei Gao for the access to the instrument for the photostability test. The authors acknowledge the support from the National Science Foundation (DMR-1709116 and CHE-1664661).

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