Abstract

We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.

Highlights

  • When an excited atom or molecule is embedded in an environment such as a cluster, novel decay channels can emerge that are absent for isolated particles

  • This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster

  • The electron emission is attributed to a correlated electronic decay, where energy is transferred from a localized electron in an atomic Rydberg state to a second nearby electron

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Summary

Introduction

When an excited atom or molecule is embedded in an environment such as a cluster, novel decay channels can emerge that are absent for isolated particles. Relaxation of the excited species can take place via a transfer of its excess energy to an atom or molecule in the environment that gets ionized, a process known as interatomic or intermolecular Coulombic decay (ICD) [1]. An electron is emitted that has a distinct kinetic energy [7]. This process could be experimentally confirmed in Ne clusters [8, 9] and in He nanodroplets [10, 11] following resonant excitation using intense XUV radiation from free-electron lasers

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