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Researchers studied photoinduced proton-coupled electron transfer (PCET) in a biomimetic system. They revealed complex dynamics involving electron density changes and molecular twists on a 120 fs timescale, advancing our understanding of this crucial process.

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Area of Science:

  • Biophysical Chemistry
  • Photochemistry
  • Spectroscopy

Background:

  • Photoinduced proton-coupled electron transfer (PCET) is vital for photosynthesis.
  • Understanding PCET mechanisms is challenging due to complex nonequilibrium dynamics and coupled electronic-nuclear motion.

Purpose of the Study:

  • To investigate the photoinduced PCET dynamics in a biomimetic model system.
  • To elucidate the complex dynamics and synergistic motions involved in photoinduced PCET.

Main Methods:

  • Transient infrared (IR) spectroscopy
  • Two-dimensional electronic-vibrational (2DEV) spectroscopy
  • IR spectroelectrochemistry (IRSEC)
  • Long-range-corrected hybrid density functional calculations

Main Results:

  • The study provides a detailed picture of photoinduced PCET dynamics.
  • Evolution of the 2DEV line shape indicates mixing of vibronic states.
  • Computational modeling reveals a gradual change in electron density distribution linked to a dihedral twist within 120 fs.

Conclusions:

  • The combined experimental and theoretical approach offers nuanced insights into photoinduced PCET.
  • The findings highlight the interplay between electronic and nuclear degrees of freedom in PCET.
  • A specific molecular motion (dihedral twist) is identified as key to electron density redistribution during PCET.