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Ultrafast Charge Separation in Bioinspired BODIPY Arrays
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DOI：10.1021/acs.jpcc.6c01298.png)
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Abstract
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Photoinitiated charge separation is the key initial step for solar-energy conversion in both natural and synthetic molecular systems. In the bacterial photosynthetic reaction center, the primary electron donor is a strongly electronically coupled bacteriochlorin dimer (a special pair). The strong electronic coupling broadens the spectral range of optical absorption and has been hypothesized to contribute to the ultrafast initial charge separation. To investigate electron transfer in synthetic arrays that include strong electronic coupling within the donors, we synthesized and characterized a series of arrays containing either strongly coupled BODIPY dimers or BODIPY monomers as electron donors, and maleimide or naphthoquinone as electron acceptors. Ultrafast charge separation (CS) is observed for arrays with naphthoquinone acceptors; in these arrays, BODIPY dimers provide broader absorption than monomers but also result in slower CS. Ultrafast CS is also observed for arrays containing maleimide connected to two BODIPY subunits via a phenylacetylene linker at the meso position; by contrast, no CS is observed for arrays containing maleimide connected to a BODIPY at the β position. The meso-linked BODIPY-dimer/maleimide arrays feature an unusually long charge recombination time of approximately 7 ns, which would help enable subsequent charge extraction.
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