Abstract

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. A well-known example is interatomic Coulombic decay, where an excited atom relaxes by transferring its excess energy to another atom in the environment, leading to its ionization. Such processes have been observed in clusters ionized by extreme-ultraviolet and X-ray lasers. Here, we report on a correlated electronic decay process that occurs following nanoplasma formation and Rydberg atom generation in the ionization of clusters by intense, non-resonant infrared laser fields. Relaxation of the Rydberg states and transfer of the available electronic energy to adjacent electrons in Rydberg states or quasifree electrons in the expanding nanoplasma leaves a distinct signature in the electron kinetic energy spectrum. These so far unobserved electron-correlation-driven energy transfer processes may play a significant role in the response of any nano-scale system to intense laser light.

Highlights

  • When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms

  • In clusters exposed to intense laser fields, excited atoms can be formed via direct laser excitation[19,22], electron–ion recombination[4,5,8,9,10] or electron impact excitation[23,24] (Fig. 1a–c)

  • Recent experiments have demonstrated that electron–ion recombination is the dominant mechanism for Rydberg atom formation in clusters exposed to intense laser pulses[8,9,10]

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Summary

Introduction

When an excited atom is embedded into an environment, novel relaxation pathways can emerge that are absent for isolated atoms. The observed decay channel emerges when these excited atoms relax to their ground state and donate the available energy to a second nearby electron (either quasifree, or itself weakly bound to an atomic core) that can escape the cluster potential. In this respect our mechanism includes the process of interatomic Coulombic decay (ICD)[11,12,13] and one of its variants involving excited states as discussed in refs 14–19. It is expected to be important in nano-scale systems interacting with laser pulses in different spectral regions

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