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- W4380763478 abstract "Many aspects of the correlation between the physical structure, light harvesting, and excitonic properties of covalent organic frameworks (COFs) remain unclear despite being key properties determining their photocatalytic function. One area of COF research that could bring clarity is using both electronic structure theory and time-resolved spectroscopic analysis over a series of systematically varied COFs. Here, we show structure–property relationships between four imine COFs built from a combination of ditopic and tritopic monomers using transient absorption spectroscopy together with time-dependent density functional theory. We find that monomer selection only moderately affects the charge transfer (CT) behavior of the COFs. Instead, we infer that imine chemistry profoundly impacts CT by acting as a CT mediator. Moreover, we discover two distinct valence bands arising from varying degrees of locally excited/CT mixing, which is responsible for energy-dependent exciton dynamics. Finally, we use theory to hypothesize that interlayer interactions can modify excitonic properties that we correlate with tail states commonly observed but rarely investigated in COFs. These results reveal that imine chemistry should be recognized as a very important factor to consider in the development of COF photocatalysts and the correlation of their structural environment with light-harvesting and CT properties that should ultimately determine their photocatalytic function." @default.
- W4380763478 created "2023-06-16" @default.
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- W4380763478 date "2023-06-15" @default.
- W4380763478 modified "2023-09-26" @default.
- W4380763478 title "Wavelength-Dependent Excitonic Properties of Covalent Organic Frameworks Explored by Theory and Experiments" @default.
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- W4380763478 doi "https://doi.org/10.1021/acs.jpcc.3c02296" @default.
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