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Modelling proton tunnelling in the adenine-thymine base pair.

A D Godbeer1, J S Al-Khalili, P D Stevenson

  • 1University of Surrey, Guildford, Surrey GU2 7XH, UK. j.al-khalili@surrey.ac.uk.

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Quantum tunneling is unlikely to create adenine-thymine tautomers in DNA. Even with environmental interactions, the probability remains extremely low, suggesting other mechanisms are at play for base pair changes.

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Area of Science:

  • Computational chemistry
  • Quantum mechanics
  • Molecular dynamics

Background:

  • Adenine-thymine base pairs are fundamental to DNA structure and function.
  • Tautomerization of DNA bases can lead to mutations.
  • Understanding the mechanisms of tautomerization is crucial for molecular biology.

Purpose of the Study:

  • To investigate the role of quantum tunneling in adenine-thymine (A-T) base pair tautomerization.
  • To calculate the potential energy surface and barrier heights for A-T tautomerization.
  • To assess the influence of environmental factors, like water molecules, on proton transfer.

Main Methods:

  • Density functional theory (DFT) was used to calculate the energies of canonical and tautomeric A-T forms.
  • Transition state searches determined the reaction pathway and potential energy surface.
  • The time-dependent master equation, including a dissipative Lindblad term, modeled quantum tunneling and environmental effects.

Main Results:

  • Quantum tunneling is improbable as a significant mechanism for A-T tautomer formation.
  • The calculated tunneling probability, even with environmental coupling, reached a maximum of 2 × 10⁻⁹.
  • Variations in wave function or potential energy surface geometry minimally impacted tunneling probability.

Conclusions:

  • Proton transfer via quantum tunneling is not a likely driver for adenine-thymine tautomerization in DNA.
  • The study provides quantitative insights into the limitations of quantum tunneling in this biological context.
  • Further research may explore alternative mechanisms for DNA base pair alterations.