Structural relaxation dynamics of electronically excited XeArN clusters

In this article we explore the structural, dynamic, and spectroscopic implications of large local configurational changes in electronically excited Xe*ArN (N=12,54,146,199) heteroclusters, where the Xe* [≡Xe(3P1)] atom is excited to the lowest dipole-allowed extravalence Rydberg excitation. The ultrafast femtosecond and picosecond dynamics driven by the short-range repulsive interaction between the vertically excited Xe* Rydberg and the cluster Ar atoms was studied by molecular dynamics simulations. From the analysis of the time dependence of the structural parameters for site-specific Xe excitations in medium-sized (N=54) and large (N=146,199) clusters, two general configurational relaxation phenomena were established: a “bubble” formation (i.e., a large configurational dilation around Xe*) for Xe interior sites and a “spring” formation (i.e., the stretching of Xe* outside the cluster) for Xe surface sites. General Xe site-specific features of both bubble and spring formation involve ultrashort (Gaussian...

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