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Direct Imaging of Laser-driven Ultrafast Molecular Rotation
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Quantum coherence in ultrafast photo-driven charge separation.

Brian T Phelan1, Jonathan D Schultz1, Jinyuan Zhang1

  • 1Department of Chemistry, Institute for Sustainability and Energy at Northwestern, Northwestern University, Evanston, IL 60208-3113, USA. m-wasielewski@northwestern.edu ryan.young@northwestern.edu.

Faraday Discussions
|May 9, 2019
PubMed
Summary

Coherent electron transfer was studied in molecular systems. Cryogenic temperatures preserve quantum coherence, enhancing electron transfer rates and delocalizing electrons, unlike room temperature conditions.

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Area of Science:

  • Photochemistry
  • Quantum Dynamics
  • Molecular Biophysics

Background:

  • Coherent interactions are crucial in photodriven processes like photosynthesis and electron transfer.
  • Quantum interference from coherently traversing multiple pathways leads to non-statistical scaling laws.

Purpose of the Study:

  • To investigate electron transfer dynamics in donor-acceptor molecular systems.
  • To understand the role of temperature and molecular architecture on quantum coherence and electron transfer rates.

Main Methods:

  • Ultrafast transient absorption spectroscopy was used to measure electron transfer.
  • Experiments were conducted on molecular systems with one or two electron acceptors at ambient and cryogenic temperatures.

Main Results:

  • A two-acceptor system exhibited a statistical rate enhancement of 2.1 ± 0.2 at room temperature.
  • At cryogenic temperatures, a non-statistical rate enhancement of 2.6 ± 0.2 was observed, indicating correlated acceptor interactions.
  • Charge recombination rates revealed electron delocalization over both acceptors at low temperatures and localization at room temperature.

Conclusions:

  • Cryogenic temperatures help preserve quantum coherence by minimizing bath fluctuations.
  • Correlated interactions between acceptors and with the environment play a significant role in electron transfer.
  • Shielding systems from bath fluctuations is essential for exploiting coherent interactions in molecular processes.