中国物理B ›› 2025, Vol. 34 ›› Issue (3): 36101-036101.doi: 10.1088/1674-1056/ada755

所属专题: SPECIAL TOPIC — Structures and properties of materials under high pressure

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Pressure-promoted ligand to metal energy transfer for emission enhancement of [Tb2(BDC)3(DMF)2(H2O)2]n metal-organic framework

Yunfeng Yang(杨云峰), Kaiyan Yuan(袁开岩), Binhao Yang(杨斌豪), Qing Yang(杨青)†, Yixuan Wang(王艺璇)‡, and Xinyi Yang(杨新一)§   

  1. Synergetic Extreme Condition High-Pressure Science Center, State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012, China
  • 收稿日期:2024-11-26 修回日期:2025-01-04 接受日期:2025-01-08 发布日期:2025-03-15
  • 通讯作者: Qing Yang, Yixuan Wang, Xinyi Yang E-mail:yangqing21@mails.jlu.edu.cn;wangyixuan19@jlu.edu.cn;yangxinyi@jlu.edu.cn
  • 基金资助:
    Project supported by the National Natural Science Foundation of China (Grant Nos. 12304261 and 12274177) and the China Postdoctoral Science Foundation (Grant No. 2024M751076).

Pressure-promoted ligand to metal energy transfer for emission enhancement of [Tb2(BDC)3(DMF)2(H2O)2]n metal-organic framework

Yunfeng Yang(杨云峰), Kaiyan Yuan(袁开岩), Binhao Yang(杨斌豪), Qing Yang(杨青)†, Yixuan Wang(王艺璇)‡, and Xinyi Yang(杨新一)§   

  1. Synergetic Extreme Condition High-Pressure Science Center, State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012, China
  • Received:2024-11-26 Revised:2025-01-04 Accepted:2025-01-08 Published:2025-03-15
  • Contact: Qing Yang, Yixuan Wang, Xinyi Yang E-mail:yangqing21@mails.jlu.edu.cn;wangyixuan19@jlu.edu.cn;yangxinyi@jlu.edu.cn
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Grant Nos. 12304261 and 12274177) and the China Postdoctoral Science Foundation (Grant No. 2024M751076).

摘要: Lanthanide metal-organic frameworks (Ln-MOFs) have received extensive attention in the development of photoluminescent (PL) materials due to their stable structures and unique line-like emission spectroscopic properties. However, in order to prepare Ln-MOFs with high PL quantum yield (PLQY), further improving the sensitization efficiency of the "antenna effect" is essential. Herein, remarkably enhanced PL in [Tb$_{2}$(BDC)$_{3}$(DMF)$_{2}$(H$_{2}$O)$_{2}$]$_{n}$ MOF is successfully achieved via high-pressure engineering at room temperature. Notably, the PL intensity continues to increase as the pressure increases, reaching its peak at 12.0 GPa, which is 4.4 times that of the initial state. Detailed experimental and theoretical calculations have demonstrated that pressure engineering significantly narrows the bandgap of [Tb$_{2}$(BDC)$_{3}$(DMF)$_{2}$(H$_{2}$O)$_{2}$]$_{n}$, optimizing both singlet and triplet energy levels. Ultimately, higher antenna effect sensitization efficiency is achieved by promoting intersystem crossing and energy transfer processes. Our work provides a promising strategy for the development of high PLQY Ln-MOFs.

关键词: lanthanide metal-organic frameworks, high pressure, green light photoluminescence enhancement, energy transfer

Abstract: Lanthanide metal-organic frameworks (Ln-MOFs) have received extensive attention in the development of photoluminescent (PL) materials due to their stable structures and unique line-like emission spectroscopic properties. However, in order to prepare Ln-MOFs with high PL quantum yield (PLQY), further improving the sensitization efficiency of the "antenna effect" is essential. Herein, remarkably enhanced PL in [Tb$_{2}$(BDC)$_{3}$(DMF)$_{2}$(H$_{2}$O)$_{2}$]$_{n}$ MOF is successfully achieved via high-pressure engineering at room temperature. Notably, the PL intensity continues to increase as the pressure increases, reaching its peak at 12.0 GPa, which is 4.4 times that of the initial state. Detailed experimental and theoretical calculations have demonstrated that pressure engineering significantly narrows the bandgap of [Tb$_{2}$(BDC)$_{3}$(DMF)$_{2}$(H$_{2}$O)$_{2}$]$_{n}$, optimizing both singlet and triplet energy levels. Ultimately, higher antenna effect sensitization efficiency is achieved by promoting intersystem crossing and energy transfer processes. Our work provides a promising strategy for the development of high PLQY Ln-MOFs.

Key words: lanthanide metal-organic frameworks, high pressure, green light photoluminescence enhancement, energy transfer

中图分类号:  (X-ray diffraction)

  • 61.05.cp
71.20.-b (Electron density of states and band structure of crystalline solids) 78.55.-m (Photoluminescence, properties and materials) 81.40.Vw (Pressure treatment)