On the local relaxation of solid neon upon Rydberg excitation of a NO impurity: the role of the NO(A)-Ne interaction potential and zero-point quantum delocalization

J Phys Chem A. 2009 Dec 31;113(52):14399-406. doi: 10.1021/jp903538f.


The local relaxation of solid neon subsequent to the impulsive excitation of the NO chromophore to its A(3s sigma) Ryberg state is investigated using molecular dynamics simulations. This study makes use of empirical NO(X,A)-Ne isotropic pair potentials as well as a recently developed ab initio triatomic potential energy surface for the excited state. The role of these interaction potentials is analyzed, including many-body effects. In particular, empirical potentials, designed to reproduce correctly both the NO X-A steady-state absorption and emission bands, are shown to lead to a good description of the subpicosecond relaxation dynamics. The 600 fs expansion of the electronic bubble fairly agrees with experimental data. This relatively long time scale with respect to solid Argon, which was previously attributed to the range of the NO(A)-Ne interaction, is presumably related to the quantum nature of the medium. The time-resolved local relaxation of the Ne solid is understandably intermediate between that of classical solids (e.g., Ar) and that of quantum solids (e.g., H(2)).

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Kinetics
  • Molecular Dynamics Simulation
  • Neon / chemistry*
  • Nitric Oxide / chemistry*
  • Quantum Theory*


  • Nitric Oxide
  • Neon