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Probing charge transfer dynamics in a single iron tetraphenylporphyrin dyad adsorbed on an insulating surface

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Abstract

Although the dynamics of charge transfer (CT) processes can be probed with ultimate lifetime resolution, the inability to control CT at the nanoscale is one of the most important roadblocks to revealing some of its deep fundamental aspects. In this work, we present an investigation of CT dynamics in a single iron tetraphenylporphyrin (Fe-TPP) donor/acceptor dyad adsorbed on a CaF2/Si(100) insulating surface. The tip of a scanning tunneling microscope (STM) is used to create local ionic states in one fragment of the dyad. The CT process is monitored by imaging subsequent changes in the neighbor acceptor molecule and its efficiency is mapped, revealing the influence of the initial excited state in the donor molecule. In the validation of the experiments, simulations based on density functional theory show that holes have a higher donor–acceptor CT rate compared to electrons and highlight a noticeable initial state dependence on the CT process. We leverage the unprecedented spatial resolution achieved in our experiments to show that the CT process in the dyad is governed via molecule–molecule coherent tunneling with negligible surface-mediated character.

Graphical abstract: Probing charge transfer dynamics in a single iron tetraphenylporphyrin dyad adsorbed on an insulating surface

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Publication details

The article was received on 05 Jul 2018, accepted on 19 Aug 2018 and first published on 20 Aug 2018


Article type: Paper
DOI: 10.1039/C8NR05424J
Citation: Nanoscale, 2018, Advance Article
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    Probing charge transfer dynamics in a single iron tetraphenylporphyrin dyad adsorbed on an insulating surface

    P. Ramos, M. Mankarious, M. Pavanello and D. Riedel, Nanoscale, 2018, Advance Article , DOI: 10.1039/C8NR05424J

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