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Caged Nitric Oxide-Thiyl Radical Pairs.

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Researchers identified elusive caged radical pairs from S-Nitrosothiols (RSNO) decomposition. Red light irradiation reformed RSNO from these radical pairs, revealing insights into nitric oxide release mechanisms.

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Area of Science:

  • Chemical Physics
  • Photochemistry
  • Biophysical Chemistry

Background:

  • S-Nitrosothiols (RSNO) are crucial biological molecules that serve as sources of nitric oxide (NO).
  • The facile homolytic cleavage of the S-N bond in RSNO facilitates NO release.
  • Understanding the intermediate species in RSNO decomposition is vital for elucidating NO signaling pathways.

Purpose of the Study:

  • To investigate the photolytic decomposition of S-Nitrosothiols (RSNO) at low temperatures.
  • To identify and characterize the elusive caged radical pairs formed during RSNO photolysis.
  • To explore the reversible formation and dissociation of these radical pairs.

Main Methods:

  • Matrix isolation spectroscopy (IR and UV/vis) at cryogenic temperatures (<10 K) using Ne, Ar, and N2 matrices.
  • Photolysis of prototypical RSNO (R = Me and Et) with UV and visible light.
  • Computational chemistry calculations (CASPT2) to determine dissociation energies.

Main Results:

  • Identification of caged radical pairs comprising nitric oxide (NO•) and thiyl radicals (RS•), stabilized by O···S and H···N interactions.
  • Observation of the disappearance of caged radical pairs upon red-light irradiation.
  • Reformation of the original RSNO from the caged radical pairs upon red-light exposure.
  • Calculated dissociation energy for the methyl radical pair (MeS•···•ON) at 4.7 kcal mol⁻¹.

Conclusions:

  • The study successfully identified transient caged radical pairs in RSNO photolysis.
  • Red-light irradiation provides a pathway to reform RSNO from radical pairs, indicating a reversible photochemical process.
  • These findings offer critical insights into the mechanism of nitric oxide release from S-Nitrosothiols.