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V R Smith1, E Samoylova, H-H Ritze

  • 1Max-Born Institut fur Nichtlineare Optik und Kurzzeitspektroskopie im FVB E.V., 2A Max-Born Str., 12489 Berlin, Germany.

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We studied how adenine (A) and its water clusters relax after photoexcitation. Hydration and dimerization significantly alter relaxation pathways and timescales, revealing new insights into excited-state dynamics.

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Area of Science:

  • Physical Chemistry
  • Photochemistry
  • Molecular Spectroscopy

Background:

  • Adenine is a fundamental component of nucleic acids.
  • Understanding its excited-state dynamics is crucial for photobiology and photochemistry.
  • The influence of hydration and dimerization on adenine's electronic relaxation is not fully understood.

Purpose of the Study:

  • To investigate the ultrafast excited-state relaxation dynamics of adenine (A) and its microhydrated clusters (A(m)(H2O)n).
  • To elucidate the role of water molecules and dimerization in altering relaxation pathways.
  • To determine the lifetimes of different electronic states and estimate adiabatic ionization potentials.

Main Methods:

  • Femtosecond pump-probe mass spectrometry.
  • Femtosecond photoelectron spectroscopy.
  • Study of isolated adenine, microhydrated adenine clusters, adenine dimer, and water-clustered adenine dimer.

Main Results:

  • Unhydrated adenine exhibits distinct relaxation via pi-pi* and n-pi* states (<0.1 ps and 1.3 ps lifetimes).
  • Microhydration quenches n-pi* relaxation, introducing faster pathways likely involving pi-sigma* states.
  • Adenine dimers show monomer-like relaxation, while pi-stacked dimers with water exhibit nanosecond lifetimes from excimer states.
  • Adiabatic ionization potentials were determined for various adenine clusters.

Conclusions:

  • Water molecules and dimerization significantly modify adenine's excited-state relaxation dynamics.
  • Hydration introduces new, faster relaxation channels, while dimerization can lead to excimer formation.
  • These findings provide critical insights into the photophysical behavior of adenine in different environments.