4.8 Article

Quantifying through-space charge transfer dynamics in π-coupled molecular systems

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NATURE COMMUNICATIONS
卷 3, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms2083

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资金

  1. NSF Career Award [CHE-07-44185]
  2. Packard Foundation
  3. Alfred P. Sloan Foundation
  4. National Science Foundation Graduate Research Fellowship [DGE-07-07425]
  5. DOE Office of Basic Energy Sciences [DE-AC02-98CH10886]
  6. NSEC at Columbia University
  7. Italian Academy at Columbia University
  8. [PRIN2008-prot.20087NX9Y7 002]
  9. Direct For Mathematical & Physical Scien
  10. Division Of Chemistry [0744185] Funding Source: National Science Foundation

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Understanding the role of intermolecular interaction on through-space charge transfer characteristics in pi-stacked molecular systems is central to the rational design of electronic materials. However, a quantitative study of charge transfer in such systems is often difficult because of poor control over molecular morphology. Here we use the core-hole clock implementation of resonant photoemission spectroscopy to study the femtosecond charge-transfer dynamics in cyclophanes, which consist of two precisely stacked p pi-systems held together by aliphatic chains. We study two systems, [2,2] paracyclophane (22PCP) and [4,4] paracyclophane (44PCP), with inter-ring separations of 3.0 and 4.0 angstrom, respectively. We find that charge transfer across the pi-coupled system of 44PCP is 20 times slower than in 22PCP. We attribute this difference to the decreased inter-ring electronic coupling in 44PCP. These measurements illustrate the use of core-hole clock spectroscopy as a general tool for quantifying through-space coupling in pi-stacked systems.

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