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UV-Induced Proton Transfer between DNA Strands.

Yuyuan Zhang1, Kimberly de La Harpe2, Ashley A Beckstead1

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UV radiation excites DNA, forming damaging photoproducts. This study reveals excited states in DNA double helices involve electron transfer and proton transfer, forming radical ions that quickly recombine, preventing mutations.

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Area of Science:

  • Photochemistry
  • Molecular Biology
  • Quantum Chemistry

Background:

  • Ultraviolet (UV) radiation induces excited states in DNA, potentially leading to mutagenic photoproducts.
  • Excited state dynamics in single-stranded DNA involve base-to-base electron transfer.
  • The behavior of excited states within the DNA double helix remains a significant area of investigation.

Purpose of the Study:

  • To investigate the fate of excited states in DNA double helices upon UV irradiation.
  • To elucidate the mechanisms of photoinduced electron and proton transfer in DNA.
  • To determine if these processes lead to the accumulation of damaging species.

Main Methods:

  • Time-resolved vibrational spectroscopy was employed to detect transient species.
  • Quantum mechanical calculations were utilized to model excited state pathways.
  • Studies were performed on various DNA duplexes.

Main Results:

  • Photoinduced interstrand proton transfer (PT) triggered by intrastrand electron transfer (ET) was observed for the first time.
  • Long-lived excited states were identified as oppositely charged base pair radical ions.
  • In certain duplexes, radical anions formed via interstrand PT were observed as tautomers.
  • Charge recombination occurred on the picosecond timescale.

Conclusions:

  • The study demonstrates a novel mechanism for excited state decay in DNA involving coupled electron and proton transfer.
  • The rapid charge recombination prevents the accumulation of potentially mutagenic radicals and tautomers.
  • These findings offer new insights into DNA photoprotection mechanisms.