Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 29, Pages 11565-11571Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b03956
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Funding
- Engineering and Physical Sciences Research Council (EPSRC)
- Winton Programme for the Physics of Sustainability
- German Science Foundation (DFG
- Research Cluster NIM)
- Free State of Bavaria (Research Network SolTech)
- European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013)/ERC Grant [321339, 670405]
- University of Cambridge
- EPSRC [EP/M006360/1] Funding Source: UKRI
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Covalent organic frameworks (COFs) are a highly versatile group of porous materials constructed from molecular building blocks, enabling deliberate tuning of their final bulk properties for a broad range of applications. Understanding their excited-state dynamics is essential for identifying suitable COF materials for applications in electronic devices such as transistors, photovoltaic cells, and water splitting electrodes. Here, we report on the ultrafast excited state dynamics of a series of fully conjugated two-dimensional (2D) COFs in which different molecular subunits are connected through imine bonds, using transient absorption spectroscopy. Although these COFs feature different topologies and chromophores, we find that excited states behave similarly across the series. We therefore present a unified model in which charges are generated through rapid singlet singlet annihilation and show lifetimes of several tens of microseconds. These long-lived charges are of particular interest for optoelectronic devices, and our results point toward the importance of controlling the singlet singlet annihilation step in order to increase the yield of separated charges.
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