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<p>Photochemistry involves elementary steps in which single electrons are transferred, but artificial photosynthesis requires multi-electron reactions. This discrepancy necessitates light-driven charge accumulation, which has so far proved very difficult to achieve without sacrificial redox reagents. Here we report a molecular donor–photosensitizer–acceptor compound in which light absorption leads to the reversible accumulation of two positive and two negative charges. The resulting photoproduct forms with an overall quantum yield of 37%, has a lifetime of more than 100 ns and stores 3.0 eV of energy. The use of a structurally well-defined molecular compound provides fundamental insights into how light-driven multi-electron transfer can generally be performed efficiently and sustainably, at irradiance levels orders of magnitude below those required in comparable systems. This represents a step towards more application-oriented research on solar fuels from fundamental studies of photoinduced (single) electron transfer.</p><p></p>

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Photoinduced double charge accumulation in a molecular compound

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月25日

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  • Mathis Brändlin,
  • Björn Pfund,
  • Oliver S. Wenger

摘要

Photochemistry involves elementary steps in which single electrons are transferred, but artificial photosynthesis requires multi-electron reactions. This discrepancy necessitates light-driven charge accumulation, which has so far proved very difficult to achieve without sacrificial redox reagents. Here we report a molecular donor–photosensitizer–acceptor compound in which light absorption leads to the reversible accumulation of two positive and two negative charges. The resulting photoproduct forms with an overall quantum yield of 37%, has a lifetime of more than 100 ns and stores 3.0 eV of energy. The use of a structurally well-defined molecular compound provides fundamental insights into how light-driven multi-electron transfer can generally be performed efficiently and sustainably, at irradiance levels orders of magnitude below those required in comparable systems. This represents a step towards more application-oriented research on solar fuels from fundamental studies of photoinduced (single) electron transfer.