Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.169
Publication date: 23rd September 2021
Photo-induced charge transfer is at the heart of many solar harvesting technologies including ones that involve semiconductor nanocrystals. To increase the efficacy of these technologies, it is imperative that the energetic barriers to charge separation and transfer are reduced. We have examined the unexplored role of the redox acceptor’s internal reorganization energy in effecting the charge transfer rates from quantum dots. The charge transfer rate to cobalt complexes having an electrochemical reduction potential difference of only 350 mV, but having nearly 2 eV difference in the reorganization energy, was experimentally studied and modelled with Marcus Theory. While driving force is important to the electron transfer rates, the difference in reorganization energy proved to have a more profound effect altering charge transfer rates by several orders of magnitude. The design of redox mediators to minimize reorganization energy rather than focusing solely on driving force would seem to be a previously ignored method to increase the efficiency of charge transfer from quantum dot applications.
MJF thanks the Vanderbilt Institute of Nanoscale Science and Engineering graduate fellowship. JEM and MJF are thankful for funding provided by the U.S. National Science Foundation TNSCORE NSF EPS 1004083 and the Vanderbilt Institute for Nanoscale Science and Engineering. SMC and SJR thank U.S. National Science Foundation CHE 1506587. MJF and SMC thank the Vanderbilt Institute of Nanoscale Science and Engineering Graduate Fellowship. PVB thanks the Australian Research Council Discovery Project DP190103158.
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