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

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

doi:10.1021/acsenergylett.9b00991

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[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.

Authors:

Zhou, Chenkun ^[1]; Lin, Haoran ^[2]; Neu, Jennifer ^[2];

^[2]; Chaaban, Maya ^[2]; Lee, Sujin ^[2]; Worku, Michael ^[2]; Chen, Banghao ^[2]; Clark, Ronald ^[2]; Cheng, Wenhao ^[1]; Guan, Jingjiao ^[1];

^[3];

^[4]; Lü, Xujie ^[5]; Bullock, James ^[6]; Pak, Chongin ^[2];

^[2];

^[7]; Siegrist, Theo ^[8];

^[8]

FAMU-FSU College of Engineering, Tallahassee, FL (United States)
Florida State Univ., Tallahassee, FL (United States)
Univ. of Southern California, Los Angeles, CA (United States)
Univ. of Hawaii at Manoa, Honolulu, HI (United States)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
Univ. of Florida, Gainesville, FL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
FAMU-FSU College of Engineering, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (United States)

Publication Date:: Tue Jun 11 00:00:00 EDT 2019

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

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.

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                    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.  https://doi.org/10.1021/acsenergylett.9b00991

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                    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.  https://doi.org/10.1021/acsenergylett.9b00991.  https://www.osti.gov/servlets/purl/1531243.

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@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         = {Tue Jun 11 00:00:00 EDT 2019},

  month        = {Tue Jun 11 00:00:00 EDT 2019}

}

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

Abstract

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