Photoluminescence Enhancement by Light Harvesting of Metal-Organic Frameworks Surrounding Semiconductor Quantum Dots
Photoluminescence Enhancement by Light Harvesting of Metal-Organic Frameworks Surrounding Semiconductor Quantum Dots
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DOI：
10.1021/acs.chemmater.0c03367
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发表时间：
2021-03-09
影响因子：
8.6
通讯作者：
Kuwabata, Susumu
中科院分区：
文献类型：
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作者：
Kumagai, Kohei;Uematsu, Taro;Kuwabata, Susumu
基于金属有机框架（MOF）的光捕获作为光化学和光物理应用的人造天线已经引起了广泛的关注。在此，我们报告了半导体量子点（QD）的光致发光增强，通过从每个 QD 周围作为表面改性剂的光捕获框架（IRMOF-3）进行有效的能量转移。 IRMOF-3晶体直接生长在量子点表面，没有任何中间层，例如聚合物。通过稳态激发光谱测量和荧光寿命测量证实了由于 IRMOF-3 的光捕获而观察到的光致发光增强。在IRMOF-3具有高吸光度的波长区域观察到该现象。根据供体和受体之间的福斯特距离 (R-0)，估计了激发能转移到量子点的 IRMOF-3 的体积因子。我们通过实验证明，当 QD 完全被 IRMOF-3 涂覆时，能量传输效率比 QD 附着在 IRMOF-3 表面时高 11 倍。在最佳条件下，QD 的 PL 强度几乎翻倍，这表明使用光捕获 MOF 作为发光 QD 表面改性剂的优势。
Metal-organic framework (MOF) based light harvesting has been attracting considerable attention as an artificial antenna for photochemical and photophysical applications. Herein, we report the photoluminescence enhancement of semiconductor quantum dots (QDs) via efficient energy transfer from a light-harvesting framework (IRMOF-3) surrounding each QD as a surface modifier. IRMOF-3 crystals were directly grown on the surface of QDs without any intermediate layer such as polymers. The observed photoluminescence enhancement owing to the light harvesting of IRMOF-3 was confirmed by both steady-state excitation spectra measurement and fluorescence lifetime measurement. The phenomenon was observed at the wavelength region where IRMOF-3 had high absorbance. On the basis of the Forster distance (R-0) between the donor and acceptor, the volumetric factor of IRMOF-3 from which the excitation energy was transferred to QDs was estimated. We experimentally demonstrated that the energy transfer efficiency was 11 times higher when QDs were fully coated by IRMOF-3 than when QDs were attached to the surface of IRMOF-3. The PL intensity from QDs was almost doubled under optimal conditions, which indicates the advantage of using light-harvesting MOFs as a surface modifier for luminescent QDs.