Role of Spin–Orbit Coupling in Long Range Energy Transfer in Metal–Organic Frameworks,Journal of the American Chemical Society

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Role of Spin–Orbit Coupling in Long Range Energy Transfer in Metal–Organic Frameworks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-20 , DOI: 10.1021/jacs.0c09503
Arnab Chakraborty ₁ , Stefan Ilic ₁ , Meng Cai ₁ , Bradley J Gibbons ₁ , Xiaozhou Yang ₁ , Connor C Slamowitz ₁ , Amanda J Morris ₁

Affiliation

Metal-organic frameworks (MOFs) are emerging as a promising platform for solar energy conversion applications. Their potential utilization as efficient chromophores in artificial photosynthesis is closely related to the understanding of light-harvesting and energy transfer processes that occur within these molecular scaffolds. Herein, we present the photophysical investigation of Ru(II), Ir(III), and Os(II) polypyridyl complexes incorporated into the backbone of UiO-67. In this work, we systematically study the effect of spin-orbit coupling on dipole-dipole energy transfer in MOFs using steady-state and time-resolved spectroscopic techniques. The results of our work indicate successful triplet-to-singlet energy transfer and a sizable increase in the transfer kinetics and critical distance, as direct consequences of strong spin-orbit couplings. Remarkably, the reported R0 value for OsDCBPY (R0 = 88 ± 10 Å) represents one of the largest Förster distances observed in an MOF. Collectively, this work contributes to the general knowledge of energy transfer in materials and provides groundwork for efficient utilization in artificial photosynthetic assemblies.

中文翻译：

自旋轨道耦合在金属有机框架中长距离能量转移中的作用

金属有机框架（MOF）正在成为太阳能转换应用的一个有前景的平台。它们在人工光合作用中作为有效发色团的潜在利用与对这些分子支架内发生的光捕获和能量转移过程的理解密切相关。在此，我们提出了掺入 UiO-67 主链的 Ru(II)、Ir(III) 和 Os(II) 聚吡啶配合物的光物理研究。在这项工作中，我们利用稳态和时间分辨光谱技术系统地研究了自旋轨道耦合对 MOF 中偶极子-偶极子能量转移的影响。我们的工作结果表明，三线态到单线态的能量转移成功，并且转移动力学和临界距离大幅增加，这是强自旋轨道耦合的直接后果。值得注意的是，报告的 OsDCBPY 的 R0 值 (R0 = 88 ± 10 Å) 代表了 MOF 中观察到的最大福斯特距离之一。总的来说，这项工作有助于增进材料中能量转移的常识，并为人工光合组件的有效利用提供基础。

更新日期：2020-11-20

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