Martin Corey R, Leith Gabrielle A, Kittikhunnatham Preecha, Park Kyoung Chul, Ejegbavwo Otega A, Mathur Abhijai, Callahan Cameron R, Desmond Shelby L, Keener Myles R, Ahmed Fiaz, Pandey Shubham, Smith Mark D, Phillpot Simon R, Greytak Andrew B, Shustova Natalia B
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC, 29208, USA.
Department of Metallurgical and Materials Engineering, Colorado School of Mines, Golden, CO, 80401, USA.
Angew Chem Int Ed Engl. 2021 Apr 6;60(15):8072-8080. doi: 10.1002/anie.202016826. Epub 2021 Feb 24.
Acquiring fundamental knowledge of properties of actinide-based materials is a necessary step to create new possibilities for addressing the current challenges in the nuclear energy and nuclear waste sectors. In this report, we established a photophysics-electronics correlation for actinide-containing metal-organic frameworks (An-MOFs) as a function of excitation wavelength, for the first time. A stepwise approach for dynamically modulating electronic properties was applied for the first time towards actinide-based heterometallic MOFs through integration of photochromic linkers. Optical cycling, modeling of density of states near the Fermi edge, conductivity measurements, and photoisomerization kinetics were employed to shed light on the process of tailoring optoelectronic properties of An-MOFs. Furthermore, the first photochromic MOF-based field-effect transistor, in which the field-effect response could be changed through light exposure, was constructed. As a demonstration, the change in current upon light exposure was sufficient to operate a two-LED fail-safe indicator circuit.
获取锕系元素基材料性质的基础知识是为应对核能和核废料领域当前挑战创造新可能性的必要步骤。在本报告中，我们首次建立了含锕系元素的金属有机框架（An-MOFs）的光物理-电子学相关性与激发波长的函数关系。通过整合光致变色连接体，首次对基于锕系元素的异金属MOFs应用了一种动态调制电子性质的逐步方法。利用光学循环、费米边缘附近态密度建模、电导率测量和光异构化动力学来阐明调整An-MOFs光电性质的过程。此外，构建了首个基于光致变色MOF的场效应晶体管，其中场效应响应可通过光照改变。作为演示，光照时电流的变化足以操作一个双LED故障安全指示电路。
