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Electron Transfer around a Molecular Corner.

Hauke C Schmidt1, Christopher B Larsen1, Oliver S Wenger1

  • 1Department of Chemistry, University of Basel, St. Johanns-Ring 19, 4056, Basel, Switzerland.

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Summary
This summary is machine-generated.

Electron transfer (ET) in angled molecular wires is dominated by through-bond hopping, not direct transfer. A spirobifluorene corner limits the rate, crucial for designing multidimensional ET systems.

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charge transferdonor-acceptor systemselectron transfermolecular electronicstime-resolved spectroscopy

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Area of Science:

  • Chemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Electron transfer (ET) distance dependence is well-studied in linear molecular wires.
  • Studies on angled molecular wires, particularly those with 90° bends, are scarce.
  • Understanding ET in complex geometries is vital for advanced molecular electronics.

Purpose of the Study:

  • To investigate electron transfer in molecular wires with integrated 90° angles using spirobifluorene as a bridging unit.
  • To compare ET efficiency in linear versus angled donor-bridge-acceptor compounds.
  • To elucidate the mechanisms governing ET across spirobifluorene-based molecular architectures.

Main Methods:

  • Synthesis of two isomeric series of donor-bridge-acceptor compounds with linear and angled geometries.
  • Utilizing spirobifluorene as a central bridging element.
  • Photoinduced electron transfer studies to measure rate constants and analyze distance dependence.

Main Results:

  • Photoinduced ET in both linear and angled series is primarily through-bond hole hopping across oligofluorene bridges.
  • Direct through-space or through-solvent ET is negligible, even in angled configurations.
  • ET rate constants in angled series are independent of bridge length, suggesting a rate-limiting step at the spirobifluorene corner.

Conclusions:

  • Spirobifluorene effectively directs electron transfer through-bond, minimizing direct transfer pathways.
  • The spirobifluorene unit acts as a bottleneck for ET in angled molecular wires.
  • Findings are crucial for the development of multidimensional electron transfer systems and molecular grids.