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Title: Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency

Abstract

Organic metal halide hybrids with zero-dimensional (0D) structure at the molecular level, or single-crystalline bulk assemblies of metal halides, are an emerging class of light-emitting materials with high photoluminescence quantum efficiencies (PLQEs) and color tunability. Here we report the synthesis and characterization of a new single-crystalline bulk assembly of metal halide clusters, (bmpy) 9[ZnCl 4] 2[Pb 3Cl 11] (bmpy: 1-butyl-1-methylpyrrolidinium), which exhibits green emission peaked at 512 nm with a remarkable near-unity PLQE at room temperature. Detailed structural and photophysical studies suggest that there are two emitting states in [Pb 3Cl 11] 5– clusters, whose populations are strongly dependent on the surrounding molecular environment that controls the excited-state structural distortion of [Pb 3Cl 11] 5– clusters. Furthermore, high chemical- and photostability have also been demonstrated in this new material.

Authors:
 [1];  [2];  [2]; ORCiD logo [2];  [2];  [2];  [2];  [2];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [4];  [5];  [6];  [2]; ORCiD logo [2]; ORCiD logo [7];  [8]; ORCiD logo [8]
  1. FAMU-FSU College of Engineering, Tallahassee, FL (United States)
  2. Florida State Univ., Tallahassee, FL (United States)
  3. Univ. of Southern California, Los Angeles, CA (United States)
  4. Univ. of Hawaii at Manoa, Honolulu, HI (United States)
  5. Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
  6. Univ. of Florida, Gainesville, FL (United States)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  8. FAMU-FSU College of Engineering, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1531243
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 4; Journal Issue: N/A; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhou, Chenkun, Lin, Haoran, Neu, Jennifer, Zhou, Yan, Chaaban, Maya, Lee, Sujin, Worku, Michael, Chen, Banghao, Clark, Ronald, Cheng, Wenhao, Guan, Jingjiao, Djurovich, Peter, Zhang, Dongzhou, Lü, Xujie, Bullock, James, Pak, Chongin, Shatruk, Michael, Du, Mao -Hua, Siegrist, Theo, and Ma, Biwu. Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.9b00991.
Zhou, Chenkun, Lin, Haoran, Neu, Jennifer, Zhou, Yan, Chaaban, Maya, Lee, Sujin, Worku, Michael, Chen, Banghao, Clark, Ronald, Cheng, Wenhao, Guan, Jingjiao, Djurovich, Peter, Zhang, Dongzhou, Lü, Xujie, Bullock, James, Pak, Chongin, Shatruk, Michael, Du, Mao -Hua, Siegrist, Theo, & Ma, Biwu. Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency. United States. doi:10.1021/acsenergylett.9b00991.
Zhou, Chenkun, Lin, Haoran, Neu, Jennifer, Zhou, Yan, Chaaban, Maya, Lee, Sujin, Worku, Michael, Chen, Banghao, Clark, Ronald, Cheng, Wenhao, Guan, Jingjiao, Djurovich, Peter, Zhang, Dongzhou, Lü, Xujie, Bullock, James, Pak, Chongin, Shatruk, Michael, Du, Mao -Hua, Siegrist, Theo, and Ma, Biwu. Tue . "Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency". United States. doi:10.1021/acsenergylett.9b00991.
@article{osti_1531243,
title = {Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency},
author = {Zhou, Chenkun and Lin, Haoran and Neu, Jennifer and Zhou, Yan and Chaaban, Maya and Lee, Sujin and Worku, Michael and Chen, Banghao and Clark, Ronald and Cheng, Wenhao and Guan, Jingjiao and Djurovich, Peter and Zhang, Dongzhou and Lü, Xujie and Bullock, James and Pak, Chongin and Shatruk, Michael and Du, Mao -Hua and Siegrist, Theo and Ma, Biwu},
abstractNote = {Organic metal halide hybrids with zero-dimensional (0D) structure at the molecular level, or single-crystalline bulk assemblies of metal halides, are an emerging class of light-emitting materials with high photoluminescence quantum efficiencies (PLQEs) and color tunability. Here we report the synthesis and characterization of a new single-crystalline bulk assembly of metal halide clusters, (bmpy)9[ZnCl4]2[Pb3Cl11] (bmpy: 1-butyl-1-methylpyrrolidinium), which exhibits green emission peaked at 512 nm with a remarkable near-unity PLQE at room temperature. Detailed structural and photophysical studies suggest that there are two emitting states in [Pb3Cl11]5– clusters, whose populations are strongly dependent on the surrounding molecular environment that controls the excited-state structural distortion of [Pb3Cl11]5– clusters. Furthermore, high chemical- and photostability have also been demonstrated in this new material.},
doi = {10.1021/acsenergylett.9b00991},
journal = {ACS Energy Letters},
number = N/A,
volume = 4,
place = {United States},
year = {2019},
month = {6}
}

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This content will become publicly available on June 11, 2020
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